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1. Deciphering the Influence of Electrolytes on the Energy Storage Mechanism of Vertically-Oriented Graphene Nanosheet Electrodes by Using Advanced Electrogravimetric Methods

Author: Tao Lé, Gérard Bidan, Florence Billon, Marc Delaunay, Jean-Michel Gérard, Hubert Perrot, Ozlem Sel, and David Aradilla
Subjects: graphene, supercapacitor, electrolyte, ionic liquids, energy storage mechanisms, EQCM, Chemistry, QD1-999
Abstract: Electrolyte composition is a crucial factor determining the capacitive properties of a supercapacitor device. However, its complex influence on the energy storage mechanisms has not yet been fully elucidated. For this purpose, in this study, the role of three different types of electrolytes based on a propylene carbonate (PC) solution containing tetrabutylammonium perchlorate (TBAClO4), lithium perchlorate (LiClO4) and butyltrimethylammonium bis(trifluoromethylsulfonyl)imide (N1114TFSI) ionic liquid on vertically-oriented graphene nanosheet electrodes has been investigated. Herein, in situ electrochemical quartz crystal microbalance (EQCM) and its coupling with electrochemical impedance spectroscopy (EIS), known as ac-electrogravimetry, have allowed the dynamic aspects of the (co)electroadsorption processes at the electrode-electrolyte interface to be examined. A major contribution of ClO4− anions (TBAClO4) was evidenced, whereas in the PC/N1114TFSI mixture (50:50 wt%) both anions (TFSI−) and cations (N1114+) were symmetrically exchanged during cycling. In the particular case of LiClO4, solvation of Li+ cations in PC was involved, affecting the kinetics of electroadsorption. These results demonstrate the suitability of dynamic electrogravimetric methods to unveil the interfacial exchange properties of mobile species for the conception of new high performance energy storage devices.
Published: 2020
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2. Charge Storage Properties of Nanostructured Poly (3,4–ethylenedioxythiophene) Electrodes Revealed by Advanced Electrogravimetry

Author: Tao Lé, David Aradilla, Gérard Bidan, Florence Billon, Catherine Debiemme-Chouvy, Hubert Perrot, and Ozlem Sel
Subjects: PEDOT, nanowires, (pseudo)-supercapacitors, charge storage mechanism, interfacial ion transfer, EQCM, AC–EG, Chemistry, QD1-999
Abstract: PEDOT nanowires (NWs) directly grown on the conducting electrode of quartz resonators enable an advanced electrogravimetric analysis of their charge storage behavior. Electrochemical quartz crystal microbalance (EQCM) and its coupling with electrochemical impedance spectroscopy (ac–electrogravimetry or AC–EG) were used complementarily and reveal that TBA+, BF4− and ACN participate in the charge compensation process with different kinetics and quantity. BF4− anions were dominant in terms of concentration over TBA+ cations and the anion transfer results in the exclusion of the solvent molecules. TBA+ concentration variation in the electrode was small compared to that of the BF4− counterpart. However, Mw of TBA+ is much higher than BF4− (242.3 vs. 86.6 g·mol−1). Thus, TBA+ cations’ gravimetric contribution to the EQCM response was more significant than that of BF4−. Additional contribution of ACN with an opposite flux direction compared with BF4−, led to a net mass gain/lost during a negative/positive potential scan, masking partially the anion response. Such subtleties of the interfacial ion transfer processes were disentangled due to the complementarity of the EQCM and AC–EG methodologies, which were applied here for the characterization of electrochemical processes at the PEDOT NW electrode/organic electrolyte interface.
Published: 2019
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3. Multiscale Multiphase Lithiation and Delithiation Mechanisms in a Composite Electrode Unraveled by Simultaneous Operando Small-Angle and Wide-Angle X-Ray Scattering

Author: Christopher L. Berhaut, Sandrine Lyonnard, Diana Zapata Dominguez, Stéphanie Pouget, David Aradilla, Samuel Tardif, Praveen Kumar, Pierre-Henri Jouneau, Willy Porcher, SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), European Synchrotron Radiation Facility (ESRF), Service Général des Rayons X (SGX ), Modélisation et Exploration des Matériaux (MEM), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Laboratoire d'Etude des Matériaux par Microscopie Avancée (LEMMA ), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Nanostructures et Rayonnement Synchrotron (NRS ), ANR-11-EQPX-0010,CRGF,Lignes synchrotron françaises à l'ESRF(2011), European Project: 685716,H2020,H2020-NMP-2015-two-stage,SINTBAT(2016), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG)
Subjects: Materials science, Silicon, Small-angle X-ray scattering, Scattering, General Engineering, General Physics and Astronomy, chemistry.chemical_element, 02 engineering and technology, lithiation/delithiation mechanisms Li-ion batteries silicon/iron silicide/graphite composite electrode operando synchrotron simultaneous SAXS/WAXS, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, chemistry, Chemical engineering, Electrode, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [CHIM.CRIS]Chemical Sciences/Cristallography, General Materials Science, Lithium, Graphite, 0210 nano-technology, Wide-angle X-ray scattering, Cell aging
Abstract: International audience; The (de)lithiation process and resulting atomic and nanoscale morphological changes of an a-Si/c-FeSi2/graphite composite negative electrode are investigated within a Li-ion full cell at several current rates (C-rates) and after prolonged cycling by simultaneous operando synchrotron wide-angle and small-angle X-ray scattering (WAXS and SAXS). WAXS allows the probing of the local crystalline structure. In particular, the observation of the graphite (de)lithiation process, revealed by the LixC6 Bragg reflections, enables access to the respective capacities of both graphite and active silicon. Simultaneously and independently, information on the silicon state of (de)lithiation and nanoscale morphology (1 to 60 nm) is obtained through SAXS. During lithiation, the SAXS intensity in the region corresponding to characteristic distances within the a-Si/c-FeSi2 domains increases. The combination of the SAXS/WAXS measurements over the course of several charge/discharge cycles, in pristine and aged electrodes, provides a complete picture of the C-rate-dependent sequential (de)lithiation mechanism of the a-Si/c-FeSi2/graphite anode. Our results indicate that, within the composite electrode, the active silicon volume does not increase linearly with lithium insertion and point toward the important role of the electrode morphology to accommodate the nanoscale silicon expansion, an effect that remains beneficial after cell aging and most probably explains the excellent performance of the composite material.
Published: 2019

4. Beyond conventional supercapacitors: Hierarchically conducting polymer-coated 3D nanostructures for integrated on-chip micro-supercapacitors employing ionic liquid electrolytes

Author: Gérard Bidan, Saïd Sadki, and David Aradilla
Subjects: Materials science, Nanowire, Nanotechnology, 02 engineering and technology, 010402 general chemistry, Polypyrrole, 01 natural sciences, Capacitance, law.invention, chemistry.chemical_compound, law, Polyaniline, Materials Chemistry, Supercapacitor, Conductive polymer, Graphene, Mechanical Engineering, Metals and Alloys, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, chemistry, Mechanics of Materials, Ionic liquid, 0210 nano-technology
Abstract: The potential of electroactive conducting polymers (ECPs), as innovative pseudocapacitive materials, has recently emerged as a promising strategy to design new and advanced concepts in the field of electrochemical energy storage devices. From this point of view, the synergistic effect produced between high electroactivity ECPs (faradaic behaviour) and large active surface 3D nanostructured materials (electrochemical double layer behaviour) in terms of their high specific capacitance, high energy and power density as well as long lifetime, has awakened an enormous interest in the domain of (micro)-supercapacitors. Accordingly, in this work, we have originally analyzed the conformal electrochemical deposition of three different π-conjugated heterocyclic polymers [poly(3,4-ethylenedioxythiophene, polypyrrole and polyaniline] onto various vertically-oriented 3D nanoarchitectures, as for example silicon nanowires (SiNWs), diamond nanowires (DiNWs) or graphene nanosheets (GNs) among others. Next, the resulting as-grown hybrid materials were evaluated as attractive electrodes in symmetric supercapacitors (sandwich configuration) in presence of organic, aqueous, aprotic and protic ionic liquid (IL) electrolytes respectively. An exhaustive characterization of their corresponding electrochemical performances was investigated according to our previously reported works, confirming the remarkable cycling stability of ECPs in ILs. In addition, a detailed state-of-the-art dealing with other types of (micro)-supercapacitors in the literature was reported to corroborate the great impact of such devices to pave the way towards the elaboration of next generation high performance supercapacitors in the coming years.
Published: 2019

5. Multi-scale quantification and modeling of aged nanostructured silicon-based composite anodes

Author: Widanalage Dhammika Widanage, Stéphanie Pouget, Christopher L. Berhaut, Lukas Helfen, David Aradilla, Sandrine Lyonnard, Samuel Tardif, Fereshteh Falah Chamasemani, Thomas Vorauer, Bernd Fuchsbichler, Selcuk Atalay, Pierre-Henri Jouneau, Roland Brunner, Stefan Koller, Praveen Kumar, Montanuniversität Leoben (MUL), Laboratoire d'Etude des Matériaux par Microscopie Avancée (LEMMA ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Leibniz Institute for New Materials (INM), Leibniz Association, Nanostructures et Rayonnement Synchrotron (NRS ), Service Général des Rayons X (SGX ), Varta Micro Innovation GmbH, Karlsruhe Institute of Technology (KIT), Warwick Manufacturing Group [Coventry] (WMG), University of Warwick [Coventry], European Project: 685716,H2020,H2020-NMP-2015-two-stage,SINTBAT(2016), and European Project: 875514,ECO2LIB
Subjects: Amorphous silicon, Technology, Materials science, MATERIALS RESEARCH, Alloy, Composite number, Li-ion batteries, chemistry.chemical_element, Nanotechnology, 02 engineering and technology, tomography, engineering.material, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Biochemistry, lcsh:Chemistry, chemistry.chemical_compound, BATTERY MATERIALS, Phase (matter), Materials Chemistry, Environmental Chemistry, SAXS-WAXS, Nanoscopic scale, PHASE CONTRAST MICROTOMOGRAPHY, advanced characterization, General Chemistry, simulation, 021001 nanoscience & nanotechnology, [INFO.INFO-MO]Computer Science [cs]/Modeling and Simulation, 0104 chemical sciences, Anode, Characterization (materials science), lcsh:QD1-999, chemistry, BATTERY ELECTRODE, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], engineering, Lithium, 0210 nano-technology, ddc:600, LI IONIC CONDUCTORS
Abstract: Advanced anode material designs utilizing dual phase alloy systems like Si/FeSi2 nano-composites show great potential to decrease the capacity degrading and improve the cycling capability for Lithium (Li)-ion batteries. Here, we present a multi-scale characterization approach to understand the (de-)lithiation and irreversible volumetric changes of the amorphous silicon (a-Si)/crystalline iron-silicide (c-FeSi2) nanoscale phase and its evolution due to cycling, as well as their impact on the proximate pore network. Scattering and 2D/3D imaging techniques are applied to probe the anode structural ageing from nm to μm length scales, after up to 300 charge-discharge cycles, and combined with modeling using the collected image data as an input. We obtain a quantified insight into the inhomogeneous lithiation of the active material induced by the morphology changes due to cycling. The electrochemical performance of Li-ion batteries does not only depend on the active material used, but also on the architecture of its proximity. Alloy systems like Si/FeSi2 nano composites have great potential as stable anode materials in Li-ion batteries, but their characterization at different scales and throughout their ageing remains challenging. Here the authors use scattering and 2D/3D imaging techniques combined with modeling to elucidate morphology changes upon cycling of the anode.
Published: 2020

6. Plasma Heavily Nitrogen-Doped Vertically Oriented Graphene Nanosheets (N-VOGNs) for High Volumetric Performance On-Chip Supercapacitors in Ionic Liquid

Author: Michael Buhagiar, Hanako Okuno, Dmitry Aldakov, David Aradilla, Jérôme Faure-Vincent, Jean-Michel Gérard, Marc Delaunay, Gérard Bidan, Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Nanophysique et Semiconducteurs (NPSC), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Laboratoire d'Etude des Matériaux par Microscopie Avancée (LEMMA ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Aldakov, Dmitry
Subjects: [CHIM.INOR] Chemical Sciences/Inorganic chemistry, Materials science, Nanotechnology, Nitrogen doped, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 7. Clean energy, 01 natural sciences, law.invention, chemistry.chemical_compound, law, ComputingMilieux_MISCELLANEOUS, Supercapacitor, [CHIM.MATE] Chemical Sciences/Material chemistry, Graphene, [CHIM.MATE]Chemical Sciences/Material chemistry, General Medicine, Plasma, 021001 nanoscience & nanotechnology, [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 0104 chemical sciences, chemistry, [CHIM.OTHE] Chemical Sciences/Other, Ionic liquid, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology
Abstract: International audience
Published: 2018

7. Understanding the energy storage mechanisms of poly(3,4-ethylenedioxythiophene)-coated silicon nanowires by electrochemical quartz crystal microbalance

Author: Catherine Debiemme-Chouvy, Ozlem Sel, Florence Billon, Gérard Bidan, Pascal Gentile, Tao Lé, Hubert Perrot, David Aradilla, SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interfaces et Systèmes Electrochimiques (LISE), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Georg-August-University [Göttingen], LABEX MATISSE (ANR-11-IDEX-0004-02), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Georg-August-University = Georg-August-Universität Göttingen
Subjects: Materials science, 02 engineering and technology, Chemical vapor deposition, 010402 general chemistry, Electrochemistry, 01 natural sciences, chemistry.chemical_compound, PEDOT:PSS, [CHIM]Chemical Sciences, General Materials Science, SiNWs, PEDOT, Supercapacitor, Mechanical Engineering, [CHIM.MATE]Chemical Sciences/Material chemistry, Quartz crystal microbalance, 021001 nanoscience & nanotechnology, Condensed Matter Physics, EQCM, 0104 chemical sciences, chemistry, Chemical engineering, Mechanics of Materials, (Pseudo)-supercapacitors, Electrode, Cyclic voltammetry, 0210 nano-technology, Poly(3,4-ethylenedioxythiophene)
Abstract: International audience; The capacitive properties of electrodes elaborated from the electrochemical deposition of poly(3,4-ethylenedioxythiophene) (PEDOT) coatings onto chemical vapor deposition (CVD)-grown silicon nanowires (SiNWs) were investigated for supercapacitor applications. A high areal capacitance value of 17 mF cm−2 (50 F g−1) was obtained at a scan rate of 100 mV s−1 in a 3-electrode cell configuration. Furthermore, this 3D hybrid nanostructure was analyzed by electrochemical quartz crystal microbalance (EQCM) to correlate the interfacial ionic exchange mechanisms to their electrochemical performance. It was demonstrated that both anions (BF4−) and cations (TBA+) were simultaneously involved in the charge compensation during the oxidation-reduction scans of cyclic voltammetry measurements.
Published: 2019

8. Powering electrodes for high performance aqueous micro-supercapacitors: Diamond-coated silicon nanowires operating at a wide cell voltage of 3 V

Author: Georgia Lewes-Malandrakis, Gérard Bidan, Christoph E. Nebel, Pascal Gentile, Fang Gao, Stéphanie Pouget, David Aradilla, and W. Müller-Sebert
Subjects: Supercapacitor, Materials science, Silicon, business.industry, General Chemical Engineering, Diamond, chemistry.chemical_element, 02 engineering and technology, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, 0104 chemical sciences, Coating, chemistry, Electrode, Electrochemistry, engineering, Optoelectronics, 0210 nano-technology, business, Current density, Electrochemical window, Power density
Abstract: In this study, we report originally the excellent electrochemical performance of a micro-supercapacitor based on diamond-coated silicon nanowire (SiNW) electrodes using an aqueous electrolyte (0.1 M LiClO4). The deposition of a nanometric boron-doped diamond coating on SiNWs allowed the enlargement of the electrochemical window up to 3 V maintaining an extraordinary capacitive electrochemical response due to its high overvoltage. Thereby, the device exhibited an areal capacitance of 0.4 mF cm-2, a high power density of 50 mW cm-2 as well as an outstanding cycling stability after 2·106 galvanostatic charge-discharge cycles at a high current density of 10 mA cm-2. In addition, an ultra-fast charge-discharge rate was determined to be 1.5 ms, demonstrating the supercapacitor's enormous ability to deliver high power values at very rapid pulse times (Pmax: 321 mW cm-2). These results also evidence the potential of diamond coating to overcome the main drawbacks of silicon (e.g. rapid silicon oxidation due to presence of water) to be employed in aqueous electrolyte supercapacitors. Consequently, the role of diamond paves the way to high performance SiNW-based micro-supercapacitor development at large electrochemical windows in aqueous electrolytes, which are at present limited to 1 V.
Published: 2017

9. Scalable chemical synthesis of doped silicon nanowires for energy applications

Author: David Aradilla, Mathieu Salaun, Julien Danet, Olga Burchak, Peter Reiss, Caroline Keller, Jérôme Faure-Vincent, Pascale Chenevier, Brigitte Pépin-Donat, Christian Lombard, Yani Chen, Nedjma Bendiab, Gérard Lapertot, Anthony Vignon, SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Optique et Matériaux (OPTIMA ), Institut Néel (NEEL), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Systèmes hybrides de basse dimensionnalité (HYBRID), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Optique et Matériaux (NEEL - OPTIMA), and Systèmes hybrides de basse dimensionnalité (NEEL - HYBRID)
Subjects: Supercapacitor, Materials science, business.industry, Doping, 02 engineering and technology, Electrolyte, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, Capacitance, Chemical synthesis, 0104 chemical sciences, Catalysis, Colloidal gold, Electrode, Optoelectronics, General Materials Science, 0210 nano-technology, business
Abstract: International audience; A versatile, low-cost and easily scalable synthesis method is presented for producing silicon nanowires (SiNWs) as a pure powder. It applies air-stable diphenylsilane as a Si source and gold nanoparticles as a catalyst and takes place in a sealed reactor at 420°C (pressure 0.4%. When used in symmetric super-capacitor devices, 1% P-doped SiNWs exhibit an areal capacity of 0.25 mF cm −2 and retention of 80% of the initial capacitance after one million cycles, demonstrating excellent cycling stability of the SiNW electrodes in the presence of organic electrolytes.
Published: 2019

10. Charge Storage Properties of Nanostructured Poly (3,4–ethylenedioxythiophene) Electrodes Revealed by Advanced Electrogravimetry

Author: Gérard Bidan, Tao Lé, David Aradilla, Ozlem Sel, Florence Billon, Catherine Debiemme-Chouvy, Hubert Perrot, SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interfaces et Systèmes Electrochimiques (LISE), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), University Medical Center Göttingen (UMG), Labex MATISSE ANR-11-IDEX-0004-02, Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Subjects: Materials science, General Chemical Engineering, Analytical chemistry, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, lcsh:Chemistry, chemistry.chemical_compound, PEDOT:PSS, Electrogravimetry, TheoryofComputation_ANALYSISOFALGORITHMSANDPROBLEMCOMPLEXITY, [CHIM]Chemical Sciences, General Materials Science, (pseudo)-supercapacitors, AC–EG, EQCM, PEDOT, charge storage mechanism, interfacial ion transfer, nanowires, Communication, AC-EG, Quartz crystal microbalance, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Dielectric spectroscopy, chemistry, lcsh:QD1-999, Electrode, 0210 nano-technology, Poly(3,4-ethylenedioxythiophene)
Abstract: PEDOT nanowires (NWs) directly grown on the conducting electrode of quartz resonators enable an advanced electrogravimetric analysis of their charge storage behavior. Electrochemical quartz crystal microbalance (EQCM) and its coupling with electrochemical impedance spectroscopy (ac–electrogravimetry or AC–EG) were used complementarily and reveal that TBA+, BF4− and ACN participate in the charge compensation process with different kinetics and quantity. BF4− anions were dominant in terms of concentration over TBA+ cations and the anion transfer results in the exclusion of the solvent molecules. TBA+ concentration variation in the electrode was small compared to that of the BF4− counterpart. However, Mw of TBA+ is much higher than BF4− (242.3 vs. 86.6 g·mol−1). Thus, TBA+ cations’ gravimetric contribution to the EQCM response was more significant than that of BF4−. Additional contribution of ACN with an opposite flux direction compared with BF4−, led to a net mass gain/lost during a negative/positive potential scan, masking partially the anion response. Such subtleties of the interfacial ion transfer processes were disentangled due to the complementarity of the EQCM and AC–EG methodologies, which were applied here for the characterization of electrochemical processes at the PEDOT NW electrode/organic electrolyte interface.
Published: 2019

11. A step forward into hierarchically nanostructured materials for high performance micro-supercapacitors: Diamond-coated SiNW electrodes in protic ionic liquid electrolyte

Author: Pascal Gentile, W. Müller-Sebert, Gérard Bidan, Christoph E. Nebel, Fang Gao, Dorian Gaboriau, David Aradilla, Georgia Lewes-Malandrakis, Thomas J. S. Schubert, Saïd Sadki, Boyan Iliev, Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Fraunhofer Institute for Applied Solid State Physics (Fraunhofer IAF), Fraunhofer (Fraunhofer-Gesellschaft), Laboratoire d'Electronique Moléculaire Organique et Hybride (LEMOH), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Ionic Liquids Technologies GmbH (IOLITECH), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), gentile, pascal, Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, [SPI.NANO] Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, Inorganic chemistry, Nanowire, 02 engineering and technology, Electrolyte, Chemical vapor deposition, engineering.material, [SPI.MAT] Engineering Sciences [physics]/Materials, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Capacitance, [SPI.MAT]Engineering Sciences [physics]/Materials, lcsh:Chemistry, chemistry.chemical_compound, Electrochemistry, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, ComputingMilieux_MISCELLANEOUS, Supercapacitor, [SPI.NRJ]Engineering Sciences [physics]/Electric power, Diamond, 021001 nanoscience & nanotechnology, [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 0104 chemical sciences, chemistry, Chemical engineering, lcsh:Industrial electrochemistry, lcsh:QD1-999, Electrode, Ionic liquid, engineering, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 0210 nano-technology, [SPI.NRJ] Engineering Sciences [physics]/Electric power, lcsh:TP250-261
Abstract: Silicon nanowires (SiNWs) were successfully coated by uniform, adherent and homogenous ultra-thin crystalline diamond films through microwave enhanced chemical vapor deposition (MWCVD). The as-grown functionalized nanowires were employed as electrodes in a symmetric micro-supercapacitor (MSC) using a protic ionic liquid electrolyte [triethylammonium bis(trifluoromethylsulfonyl)imide; Et3NH TFSI]. The electrochemical performance of the device delivered a specific capacitance of 1.5 mF cm−2 and a power density of 25 mW cm−2 using an enlarged cell voltage of 4 V. Furthermore, a remarkable cycling stability was evaluated after 1 · 106 galvanostatic cycles at a high current density of 10 mA cm−2 with an excellent capacitive behavior. These results confirm that diamond-coated SiNW micro-supercapacitors exhibit very promising performances dealing with MSCs based on CVD-grown SiNWs. Keywords: Supercapacitors, Ionic liquid, Diamond, Silicon nanowires
Published: 2016

12. Solvent effects on the properties of hyperbranched polythiophenes

Author: Juan Torras, David Aradilla, Carlos Alemán, David Zanuy, Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. IMEM - Innovació, Modelització i Enginyeria en (BIO) Materials
Subjects: Chemistry, Implicit solvation, General Physics and Astronomy, Thermodynamics, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Electroquímica, Solvent, Molecular dynamics, chemistry.chemical_compound, Enginyeria química [Àrees temàtiques de la UPC], Biomolècules, Computational chemistry, Dendrimer, Molecule, Dimethylformamide, Density functional theory, Thiophenes--Electric properties, Physical and Theoretical Chemistry, Solvent effects, 0210 nano-technology
Abstract: The structural and electronic properties of all-thiophene dendrimers and dendrons in solution have been evaluated using very different theoretical approaches based on quantum mechanical (QM) and hybrid QM/molecular mechanics (MM) methodologies: (i) calculations on minimum energy conformations using an implicit solvation model in combination with density functional theory (DFT) or time-dependent DFT (TD-DFT) methods; (ii) hybrid QM/MM calculations, in which the solute and solvent molecules are represented at the DFT level as point charges, respectively, on snapshots extracted from classical molecular dynamics (MD) simulations using explicit solvent molecules, and (iii) QM/MM-MD trajectories in which the solute is described at the DFT or TD-DFT level and the explicit solvent molecules are represented using classical force-fields. Calculations have been performed in dichloromethane, tetrahydrofuran and dimethylformamide. A comparison of the results obtained using the different approaches with the available experimental data indicates that the incorporation of effects associated with both the conformational dynamics of the dendrimer and the explicit solvent molecules is strictly necessary to satisfactorily reproduce the properties of the investigated systems. Accordingly, QM/MM-MD simulations are able to capture such effects providing a reliable description of electronic properties–conformational flexibility relationships in all-Th dendrimers.
Published: 2016

13. Ion Sieving Effects in Chemically Tuned Pillared Graphene Materials for Electrochemical Capacitors

Author: Harish Banda, Florence Duclairoir, Yves Chenavier, Barbara Daffos, Olivier Crosnier, Lionel Dubois, Stéphanie Pouget, Pierre-Louis Taberna, David Aradilla, Patrice Simon, Sandy Périé, SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées, Réseau sur le stockage électrochimique de l'énergie (RS2E), Centre National de la Recherche Scientifique (CNRS), Service Général des Rayons X (SGX), Modélisation et Exploration des Matériaux (MEM), Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Institut des Matériaux Jean Rouxel (IMN), Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS), Conception d’Architectures Moléculaires et Processus Electroniques (CAMPE), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Université de Nantes (UN)-Aix Marseille Université (AMU)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP), Service Général des Rayons X (SGX ), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Microbiologie Environnementale et Moléculaire (MEM), Institut de Biosciences et Biotechnologies d'Aix-Marseille (ex-IBEB) (BIAM), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR-15-CE05-0022,SUGGEST,Architectures structurées de graphène conçues pour le stockage électrochimique(2015), Commissariat à l'Energie Atomique et aux énergies alternatives - CEA (FRANCE), Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE), Institut polytechnique de Grenoble (FRANCE), Sorbonne Université (FRANCE), Université Grenoble Alpes - UGA (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), Université de Haute Alsace - UHA (FRANCE), Université de Montpellier (FRANCE), Institut National Polytechnique de Toulouse - INPT (FRANCE), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), and Université de Nantes (UN)-Université de Nantes (UN)
Subjects: Energie électrique, Materials science, General Chemical Engineering, Matériaux, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, Energy storage, law.invention, Ion, [SPI.MAT]Engineering Sciences [physics]/Materials, X-ray, Sieve, law, Materials Chemistry, Supercapacitors, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS, Supercapacitor, Graphene, [SPI.NRJ]Engineering Sciences [physics]/Electric power, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Characterization (materials science), Chemical engineering, 0210 nano-technology
Abstract: International audience; Supercapacitors offer high power densities but require further improvements in energy densities for widespread commercial applications. In addition to the conventional strategy of using large surface area materials to enhance energy storage, recently, matching electrolyte ion sizes to material pore sizes has been shown to be particularly effective. However, synthesis and characterization of materials with precise pore sizes remain challenging. Herein, we propose to evaluate the layered structures in graphene derivatives as being analogous to pores and study the possibility of ion sieving. A class of pillared graphene based materials with suitable interlayer separation were synthesized, readily characterized by X-ray diffraction, and tested in various electrolytes. Electrochemical results show that the interlayer galleries could indeed sieve electrolyte ions based on size constrictions: ions with naked sizes that are smaller than the interlayer separation access the galleries, whereas the larger ions are restricted. These first observations of ion sieving in pillared graphene-based materials enable efficient charge storage through optimization of the d-spacing/ion size couple.
Published: 2018

14. A new high performance ionic liquid mixture electrolyte for large temperature range supercapacitor applications (−70 °C to 80 °C) operating at 3.5V cell voltage

Author: Boyan Iliev, David Aradilla, Rodrigo Newell, Jérôme Faure-Vincent, Thomas J. S. Schubert, Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut Nanosciences et Cryogénie (INAC), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Ionic Liquids Technologies GmbH (IOLITECH), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])
Subjects: Materials science, General Chemical Engineering, 02 engineering and technology, Electrolyte, Ionic liquid, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, chemistry.chemical_compound, Mixture, Supercapacitors, [CHIM]Chemical Sciences, Eutectic system, Supercapacitor, Temperature, Atmospheric temperature range, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, chemistry, Electrode, 0210 nano-technology, Electrochemical window
Abstract: International audience; In this work, we propose a new eutectic ionic liquid mixture based on 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide and 1-propyl-3-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide to be employed as electrolyte in large temperature range supercapacitor applications. The electrolyte exhibited excellent thermal properties in terms of high temperature decomposition (440 °C), a very low melting temperature (no phase transition up to −70 °C) as well as a wide electrochemical window (4.4 V vs Pt). Accordingly, a symmetric coin cell supercapacitor device was performed using porous Ni-foam electrodes in presence of the corresponding mixture at an extended working temperature range from −70 °C to 80 °C. The electrochemical performance of the device was characterised by a wide electrochemical window of 3.5 V maintaining an excellent electrochemical double layer capacitive behavior in all the range. In addition, areal capacitance values between 5 μF cm−2 (−70 °C) and 100 μF cm−2 (80 °C) were obtained at a high scan rate of 20 V s−1, evidencing the rapid and extraordinary electrochemical response even at such extreme temperatures with an excellent cycling stability.
Published: 2018

15. Unveiling the ionic exchange mechanisms in vertically-oriented graphene nanosheet supercapacitor electrodes with electrochemical quartz crystal microbalance and ac -electrogravimetry

Author: Tao Lé, Marc Delaunay, Gérard Bidan, Jean-Michel Gérard, Florence Billon, Ozlem Sel, Hubert Perrot, David Aradilla, Laboratoire Interfaces et Systèmes Electrochimiques (LISE), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Nanophysique et Semiconducteurs (NPSC), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), ANR-11-IDEX-0004,SUPER,Sorbonne Universités à Paris pour l'Enseignement et la Recherche(2011), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG)
Subjects: Materials science, Ionic bonding, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, law.invention, lcsh:Chemistry, law, Electrogravimetry, Supercapacitors, Microbalance, Ac-electrogravimetry, Nanosheet, Supercapacitor, Graphene, Quartz crystal microbalance, 021001 nanoscience & nanotechnology, 0104 chemical sciences, lcsh:Industrial electrochemistry, lcsh:QD1-999, Chemical engineering, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other, lcsh:TP250-261
Abstract: This work presents the first electrochemical quartz crystal microbalance (EQCM) results for vertically-oriented graphene nanosheets (VOGNs) as supercapacitor electrodes. Conventional EQCM technique delivered primary insights on the ionic exchange mechanisms between VOGNs and organic electrolytes, showing a major contribution of anions. A more advanced electrogravimetric methodology, ac-electrogravimetry, was then used to access specific dynamic attributes for each species exchanged at the VOGN electrode surface. Accordingly, under the conditions of this study, anions were confirmed to be the major energy storage vector with high kinetic values and low transfer resistance while cations and free solvent molecules are given non-negligible supporting roles. Keywords: Supercapacitors, Microbalance, ac-electrogravimetry, Graphene
Published: 2018

16. Etude électrogravimétrique d'électrodes à base de nanofils de silicium pour le stockage électrochimique de l'énergie

Author: Tao Lé, Gentile, P., David Aradilla, Gérard Bidan, Hubert Perrot, Ozlem Sel, Laboratoire Interfaces et Systèmes Electrochimiques (LISE), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Nanosciences et Cryogénie (INAC), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])
Subjects: [CHIM]Chemical Sciences
Abstract: International audience; Les électrodes élaborées avec des architectures nanométriquessont de plus en plus étudiées pour améliorer les performances desbatteries et supercondensateurs. En particulier les nanofils desilicium dopés permettent d’obtenir de hautes valeurs depuissance et d’énergie grâce à de larges surfaces développées etune bonne conductivité jusqu’au collecteur de courant [1].Cependant les mécanismes d’échanges ioniques et lesphénomènes de décomposition de l’électrolyte ayant lieu àl’interface des nanofils varient en fonction de l’électrolyte utiliséet restent largement méconnus.Une meilleure compréhension de ces mécanismes peut êtreobtenue avec la microbalance à quartz électrochimique(EQCM) qui couple l’analyse électrochimique à la mesure desvariations de masse de l’électrode, ce qui permet de distinguerles espèces mises en jeu et la cinétique des échanges ioniques[2].Pour réaliser cette étude, la croissance de nanofils de silicium aété mise au point sur un substrat piézoélectrique en GaPO4compatible avec la température de croissance par CVD à600°C (Fig. 1.a).Des mesures électrogravimétriques effectuées dans diversmilieux organiques et des mélanges de liquides ioniques ontpermis de distinguer différents mécanismes de stockageélectrochimique et leurs cinétiques associées (Fig. 1.b)Références :[1] Aradilla, D.; Gentile, P.; Bidan, G.; Ruiz, V.; Gómez-Romero, P.; Schubert, T. J.; Sahin, H.;Frackowiak, E.; Sadki, S. Nano Energy 2014, 9, 273–281.[2] Escobar-Teran, F.; Arnau, A.; Garcia, J.; Jiménez, Y.; Perrot, H.; Sel, O. ElectrochemistryCommunications 2016, 70, 73–77.
Published: 2017

17. One-step synthesis of highly reduced graphene hydrogels for high power supercapacitor applications

Author: Barbara Daffos, Lionel Dubois, Anass Benayad, Florence Duclairoir, Yves Chenavier, David Aradilla, Harish Banda, Commissariat à l'Energie Atomique et aux énergies alternatives - CEA (FRANCE), Centre National de la Recherche Scientifique - CNRS (FRANCE), Collège de France (FRANCE), Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE), Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE), Institut National Polytechnique de Toulouse - INPT (FRANCE), Institut polytechnique de Grenoble (FRANCE), Sorbonne Université (FRANCE), Université Grenoble Alpes - UGA (FRANCE), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Université de Nantes (FRANCE), Université de Picardie Jules Verne (FRANCE), Université de Pau et des Pays de l'Adour - UPPA (FRANCE), Université de Montpellier (FRANCE), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Polymères Conducteurs Ioniques (PCI), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Reconnaissance Ionique et Chimie de Coordination (RICC), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Université de Nantes (UN)-Aix Marseille Université (AMU)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), and Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE)
Subjects: Energie électrique, Materials science, Matériaux, Oxide, Energy Engineering and Power Technology, One-Step, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Capacitance, Graphene hydrogels, law.invention, [SPI.MAT]Engineering Sciences [physics]/Materials, chemistry.chemical_compound, Aqueous electrolyte, law, Supercapacitors, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, Monolith, Supercapacitor, geography, geography.geographical_feature_category, Renewable Energy, Sustainability and the Environment, Graphene, [SPI.NRJ]Engineering Sciences [physics]/Electric power, 021001 nanoscience & nanotechnology, [SDE.ES]Environmental Sciences/Environmental and Society, 0104 chemical sciences, chemistry, Self-healing hydrogels, 0210 nano-technology, Current density
Abstract: International audience; Graphene hydrogels with high electrical conductivity were prepared by a one-step process using hydrazine hydrate as gel assembly agent (GH-HD). Conventional two-step process of gel formation and further reduction to prepare highly conducting gels was replaced by a single step involving equivalent amount of hydrazine. Optimized graphene oxide concentration was established to facilitate such monolith formation. Extensive characterization and control studies enabled understanding of the material properties and gel formation mechanism. The synthesized gel shows a high electrical conductivity of 1141 S/m. The supercapacitor based on GH-HD delivers a high specific capacitance of 190 F/g at a current density of 0.5 A/g and 123 F/g at very high current density of 100 A/g. Furthermore, excellent power capability and cyclic stability were also observed. 3D macroporous morphology of GH-HD makes it ideal for high rate supercapacitor applications.
Published: 2017

18. New electrolyte mixture of propylene carbonate and butyltrimethylammonium bis(trifluoromethylsulfonyl)imide (N 1114 TFSI) for high performance silicon nanowire (SiNW)-based supercapacitor applications

Author: Gérard Bidan, Pascal Gentile, David Aradilla, Tao Lé, SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG)
Subjects: Materials science, General Chemical Engineering, Inorganic chemistry, 02 engineering and technology, Electrolyte, electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, chemistry.chemical_compound, Silicon nanowires, Imide, Power density, ionic liquid, Supercapacitor, supercapacitors, temperature, 021001 nanoscience & nanotechnology, 0104 chemical sciences, mixture, chemistry, Chemical engineering, Ionic liquid, Propylene carbonate, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other
Abstract: International audience; The use of a mixture of propylene carbonate (PC) and N1114 TFSI ionic liquid (50:50% w.t) has been investigated as an optimal electrolyte for symmetric micro-supercapacitors based on SiNWs using a large and stable cell voltage of 3.5 V. The device showed an areal capacitance of 150 μF cm−2, an energy density of 1 mJ cm−2 and a power density of 16 mW cm−2 maintaining an outstanding cycling stability after 3·106 galvanostatic charge-discharge cycles at room temperature. Such properties were comparable to those obtained using the pure ionic liquid. Additionally, the excellent electrochemical performances reported in this study reflect the potential of such mixture to be employed as a promising electrolyte in wide operating temperatures ranging from 0 to 80 °C at large electrochemical windows.
Published: 2017

19. Pulse electropolymerization synthesis of PPy(DBS) nanoparticle layers

Author: Alexandra Apostoluk, Ahmad Ahmadi Daryakenari, David Aradilla, Jean-Jacques Delaunay, Saïd Sadki, The University of Tokyo, School of Engineering, INL - Spectroscopies et Nanomatériaux (INL - S&N), Institut des Nanotechnologies de Lyon (INL), Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-École Centrale de Lyon (ECL), Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE), Structures et propriétés d'architectures moléculaire (SPRAM - UMR 5819), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), École Centrale de Lyon (ECL), Université de Lyon-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École Supérieure de Chimie Physique Électronique de Lyon (CPE)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-École Centrale de Lyon (ECL), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Institut Nanosciences et Cryogénie (INAC), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Conductive polymer, Materials science, Working electrode, Nucleation, Nanoparticle, Pulse duration, Nanotechnology, Electrolyte, Condensed Matter Physics, Polypyrrole, [SPI.MAT]Engineering Sciences [physics]/Materials, [SPI]Engineering Sciences [physics], chemistry.chemical_compound, Chemical engineering, chemistry, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Electrochemistry, General Materials Science, Particle size, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, Electrical and Electronic Engineering
Abstract: International audience; A one-step process using a pulse electropolymerization technique is used to fabricate nanoparticles of polypyrrole (PPy) with dodecyl benzene sulfonate (DBS) anions from an aqueous solution without template and without using any chemical additives. The morphology of particles is controlled by changing the pulse duration (from 120 to 0.5 s), while keeping the relaxation time constant at 15 s. Short pulses resulted in the formation of PPy(DBS) nanoparticles with an average particle size of about 50 nm. The control of the size of the PPy(DBS) nanoparticles is ascribed to a pulse electropolymerization growth mechanism, whereby progressive nucleation associated with two-dimensional growth is initiated at each new pulse cycle from the equilibrium electrolyte solution. Short pulses are needed to avoid nonuniform growth of nanoparticles and control the particle size. Sufficiently long relaxation time is required to restore the equilibrium concentrations in the vicinity of the working electrode by suppressing the double layer. Combining short pulses with sufficiently long relaxation times enables the formation of PPy(DBS) nanoparticles. The proposed short-pulse technique is meant to be applied to the fabrication of a wide range of nanostructured conductive polymers.
Published: 2014

20. Properties of oligothiophene polycations

Author: Carlos Alemán and David Aradilla
Subjects: Bipolaron, Molecular geometry, Chemistry, Computational chemistry, Ionization, Excited state, Organic Chemistry, Density functional theory, Singlet state, Physical and Theoretical Chemistry, Polaron, Molecular physics, Spin contamination
Abstract: The different electronic states of trications and tetracations have been studied for oligomers made of n 3,4-ethylenedioxythiophene units, where n ranges from 2 to 30. Results have been compared with those obtained for neutral, monodications and dications of the same n-oligomers. For the longer oligomer (n ≥ 24) trications, the doublet and quartet states are isoenergetic, while the triplet and quintet states are isoenergetic for tetracations of the same length. Analysis of the geometry reveals three separated polarons for the doublet and quartet states of tricationic n-oligomers, even though that of the former state has been attributed to a heavy spin contamination. In contrast, the structure of tetracations shows double bipolaron character for the singlet state and two polaron pairs for both the triplet and quintet states. Analyses of both charge and spin density distributions support the polaronic or bipolaronic behavior predicted by molecular geometry for the different electronic states. Results have been also used to evaluate the ionization potentials and the π-π* lowest transition energy of infinite polymer chains. Copyright © 2014 John Wiley & Sons, Ltd.
Published: 2014

21. All-polythiophene rechargeable batteries

Author: Francesc Estrany, José I. Iribarren, Francisco Casellas, David Aradilla, and Carlos Alemán
Subjects: Nanocomposite, Fabrication, Materials science, Nanotechnology, Organic radical battery, General Chemistry, Condensed Matter Physics, Cathode, Electronic, Optical and Magnetic Materials, Anode, law.invention, Biomaterials, chemistry.chemical_compound, Capacitor, chemistry, PEDOT:PSS, law, Materials Chemistry, Polythiophene, Electrical and Electronic Engineering
Abstract: All-conducting polymer batteries, in which both the anode and cathode consist of films made of perchlorate-doped pure poly(3,4-ethylenedioxythiophene) (PEDOT), alternated layers of PEDOT and poly(N-methylpyrrole) or PEDOT/clay nanocomposites, have been fabricated. Batteries, which have been used as power source for a LED bulb, are rechargeable and exhibit excellent charge/discharge cyclability and stability. The organic devices prepared using PEDOT and multilayered films have been found to be promising platforms to achieve metal-free power sources. Thus, these materials, in particular the multilayered films, show a dual behavior being useful for the fabrication of both capacitors and batteries.
Published: 2014

22. Nanometric ultracapacitors fabricated using multilayer of conducting polymers on self-assembled octanethiol monolayers

Author: José I. Iribarren, Maria M. Pérez-Madrigal, Denise Schermann Azambuja, Carlos Alemán, David Aradilla, Francesc Estrany, Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. IMEM - Innovació, Modelització i Enginyeria en (BIO) Materials
Subjects: Materials science, Polymers, Scanning electron microscope, Conducting polymers, Nanotechnology, Polypyrrole, Capacitance, Biomaterials, chemistry.chemical_compound, Enginyeria química [Àrees temàtiques de la UPC], Ultracapacitors, Monolayer, Materials Chemistry, Electrical and Electronic Engineering, Composite material, Supercapacitor, Conductive polymer, Self-assembled monolayer, Nanotecnologia, General Chemistry, Condensed Matter Physics, Polímers, Electronic, Optical and Magnetic Materials, Multilayered films, chemistry, Electrode, Alkanethiols
Abstract: Symmetric ultracapacitors have been fabricated considering nanometric 3-layered films made of alternated layers of poly(3,4-ethylenedioxythiophene) (external and internal layers) and polypyrrole (intermediate layer) deposited on steel uncoated and coated with octanethiol self-assembled monolayer. The highest electrochemical and capacitance parameters (i.e. electroactivity, doping level, stored charge, specific capacitance, Coulomb efficiency, energy density and power density) correspond to the ultracapacitor derived from the assembly of 3-layered films deposited on pre-treated steel. Thus, the interface separating the octanethiol monolayer and the most internal layer of the 3-layered film produces a very favorable interaction, which promotes important electrochemical benefits similar to those found for the interfaces in conventional multilayered films. Moreover, the pre-treatment of the steel electrode enhances the roughness and porosity of the film deposited on it, transmitting this effect layer-by-layer. Structural and morphological characteristics, which have been characterized using scanning electron microscopy and atomic force microscopy, have been related with the electrochemical and capacitance properties of the ultracapacitors.
Published: 2013

23. Capacitive Composites Made of Conducting Polymer and Lysozyme: Toward the Biocondenser

Author: David Aradilla, Daniel E. López-Pérez, Carlos Alemán, and Luis J. del Valle
Subjects: Conductive polymer, Materials science, Composite number, Adhesion, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, chemistry.chemical_compound, General Energy, Monomer, PEDOT:PSS, chemistry, Polymerization, Physical and Theoretical Chemistry, Lysozyme, Composite material, Acetonitrile
Abstract: Conducting polymer/protein composites, P(EDOT-LZ), of poly(3,4-ethylenedioxythiophene) (PEDOT) and lysozyme, a protein with bactericidal activity, have been prepared by in situ anodic polymerization. The stability of the composite obtained from a polymerization medium consisting of an acetonitrile:water solution (1:4 v/v) with a 1:1 monomer:lysozyme mass ratio is better than that of the individual conducting polymer, while the electrical conductivity and capacitive behavior of the two systems are very similar. Incorporation of the enzyme produces drastic changes in the morphology of PEDOT, resulting in the formation of very homogeneous aggregates with cotton flake morphology that has been shown to be hollow. Multilayered systems formed by alternating layers of PEDOT and P(EDOT-LZ) have been examined, even though results indicated that they do not show any practical advantage with respect to the individual P(EDOT-LZ) films. Adhesion assay using four eukaryotic cellular lines have evidenced that the behavio...
Published: 2013

24. Synergy of the redox pair in the capacitive properties of nanometric poly(3,4-ethylenedioxythiophene)

Author: Francesc Estrany, Carlos Alemán, and David Aradilla
Subjects: Supercapacitor, Materials science, Capacitive sensing, Analytical chemistry, General Chemistry, Electrolyte, Condensed Matter Physics, Electrochemistry, Electronic, Optical and Magnetic Materials, Dielectric spectroscopy, Biomaterials, chemistry.chemical_compound, chemistry, Chemical engineering, PEDOT:PSS, Materials Chemistry, Electrical and Electronic Engineering, Cyclic voltammetry, Poly(3,4-ethylenedioxythiophene)
Abstract: The effect of the I-/I3- redox pair electrolyte in the structural, electrochemical and capacitive properties of micrometric and nanometric PEDOT films have been examined. The thickness of the films has been found to play a key role on the capacitive properties, outstanding electrochemical properties being achieved at the nanometric scale. Electrochemical and capacitive properties were extensively investigated using cyclic voltammetry, recurrent galvanostatic pulse, chronopotentiometry and electrochemical impedance spectroscopy techniques. Results evidenced that nanometric PEDOT films exhibit very high electrochemical stabilities and excellent specific capacitances (∼185 F g−1), the latter being preserved in ∼94% after 2000 cycles in a I-/I3- -containing solution. Morphological studies revealed that the electrochemical and capacitive properties of PEDOT films are significantly influenced by their porosity, this property being relatively unaffected by the I-/I3- redox pair. The overall results allowed us to conclude that nanometric PEDOT films in presence of I-/I3- are promising candidates to be employed as supercapacitors.
Published: 2013

25. Designing 3D Multihierarchical Heteronanostructures for High-Performance On-Chip Hybrid Supercapacitors: Poly(3,4-(ethylenedioxy)thiophene)-Coated Diamond/Silicon Nanowire Electrodes in an Aprotic Ionic Liquid

Author: Fang Gao, Georgia Lewes-Malandrakis, Maxime Boniface, Gérard Bidan, Thomas J. S. Schubert, Dmitry Aldakov, Boyan Iliev, David Aradilla, W. Müller-Sebert, Christoph E. Nebel, Pascal Gentile, Structures et propriétés d'architectures moléculaire (SPRAM - UMR 5819), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Nanostructures et Magnétisme (NM), Service de Physique des Matériaux et Microstructures (SP2M - UMR 9002), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Fraunhofer Institute for Applied Solid State Physics (Fraunhofer IAF), Fraunhofer (Fraunhofer-Gesellschaft), Ionic Liquids Technologies GmbH (IOLITECH), European Project: 0243492(2003), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut Nanosciences et Cryogénie (INAC), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Publica
Subjects: Materials science, Inorganic chemistry, Nanowire, Ionic Liquids, Micro-Supercapacitors, 02 engineering and technology, 010402 general chemistry, High-Energy Density, 01 natural sciences, 7. Clean energy, Capacitance, Conducting Polymers, chemistry.chemical_compound, PEDOT:PSS, Supercapacitors, High-Power, General Materials Science, supercapacitor, Porous Carbon Electrodes, Ethylenedioxy, Conductive polymer, Supercapacitor, [PHYS]Physics [physics], Silicon Nanowires, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, chemistry, Electrode, Ionic liquid, Doped Silicon Nanowires, Diamond, 0210 nano-technology, Carbide Nanowires
Abstract: International audience; A versatile and robust hierarchically multifunctionalized nanostructured material made of poly(3,4-(ethylenedioxy)thiophene) (PEDOT)-coated diamond@silicon nanowires has been demonstrated to be an excellent capacitive electrode for supercapacitor devices. Thus, the electrochemical deposition of nanometric PEDOT films on diamond-coated silicon nanowire (SiNW) electrodes using N-methyl-N-propylpyrrolidinium bis((trifluoromethyl)sulfonyl)imide ionic liquid displayed a specific capacitance value of 140 F g(-1) at a scan rate of 1 mV s(-1). The as-grown functionalized electrodes were evaluated in a symmetric planar microsupercapacitor using butyltrimethylammonium bis((trifluoromethyl)sulfonypimide aprotic ionic liquid as the electrolyte. The device exhibited extraordinary energy and power density values of 26 mJ cm(-2) and 1.3 mW cm(-2) within a large voltage cell of 2.5 V, respectively. In addition, the system was able to retain 80% of its initial capacitance after 15 000 galvanostatic charge-discharge cycles at a high current density of 1 mA cm(-2) while maintaining a Coulombic efficiency around 100%. Therefore, this multifunctionalized hybrid device represents one of the best electrochemical performances concerning coated SiNW electrodes for a high-energy advanced on-chip supercapacitor.
Published: 2016

26. Silicon nanowires and nanotrees: elaboration and optimization of new 3D architectures for high performance on-chip supercapacitors

Author: Dorian Gaboriau, Thierry Brousse, Gérard Bidan, J. Le Bideau, Pascal Gentile, David Aradilla, Mylène Brachet, Saïd Sadki, Laboratoire d'Electronique Moléculaire Organique et Hybride (LEMOH), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Institut des Matériaux Jean Rouxel (IMN), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), ANR-12-BS09-0032,ISICAP,Supercondensateurs à base de Nanostructures de Si(2012), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), and Université de Nantes (UN)-Université de Nantes (UN)
Subjects: Supercapacitor, Materials science, Nanostructure, Silicon, business.industry, General Chemical Engineering, Doping, chemistry.chemical_element, Nanotechnology, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Energy storage, 0104 chemical sciences, chemistry, Electrode, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Microelectronics, 0210 nano-technology, business, ComputingMilieux_MISCELLANEOUS, Electrochemical window
Abstract: Micro-supercapacitors are increasingly foreseen as future energy storage or power buffer solutions for small scale integration on-chip. However, widely used electrode materials or electrolytes often proved to be incompatible with microelectronics processes. Although being the material of choice for on-chip integration, nanostructured silicon electrodes only recently caught attention for potential applications, and they displayed promising results especially for bottom-up silicon nanostructures, where the design liberty and fine control of nanostructure morphologies allow considerable improvements. The present work deals with the optimization of highly doped silicon nanowires (Si-NWs) and nanotrees (Si-NTrs) pioneered in the laboratory using an innovative, fast and efficient electroless gold deposition method in order to explore a wide variety of 3D architectures and their physicochemical properties. Through a systematic study of branches and trunks morphologies, the nature inspired nanotrees have been drastically improved compared to previously published works, resulting in excellent electrode properties, showing high energy and power densities, respectively, up to 2.8 mJ cm−2 and 235 mW cm−2. In addition, a cyclability of over a million charge–discharge galvanostatic cycles was determined using an enlarged electrochemical window of 4 V in an ionic liquid electrolyte.
Published: 2016

27. New insights into the characterization of poly(3-chlorothiophene) for electrochromic devices

Author: José I. Iribarren, Jordi Casanovas, David Aradilla, Francesc Estrany, and Carlos Alemán
Subjects: chemistry.chemical_classification, Materials science, Polymers and Plastics, Scanning electron microscope, Organic Chemistry, Doping, Bioengineering, Nanotechnology, Polymer, Electrochemistry, Electrochromic devices, Biochemistry, Dielectric spectroscopy, chemistry, Polymerization, Chemical engineering, Electrochromism
Abstract: Poly(3-chlorothiophene) has been prepared by anodic polymerization in boron trifluoride diethyl etherate with 0.1 M tetrabutylammonium tetrafluoroborate. The potential applied for the generation of the polymer has been found to affect considerably both physical (e.g. the thickness and roughness of the films, and the current efficiency) and electrochemical properties (e.g. the electroactivity, the doping level and the specific capacitance) whereas the density and the electrical conductivity remain practically unaltered in the interval ranging from 1.60 to 1.90 V. The dependence of the electrochemical behaviour with the generation potential has been explained by the morphological and topographical characteristics of the material, which have been investigated not only using scanning electron microscopy and atomic force microscopy but also electrochemical impedance spectroscopy. On the other hand, experimentally determined electronic properties have been reproduced by quantum mechanical calculations on model oligomers formed by up to 16 chemical repeating units that were arranged through a repetitive sequence of head-to-tail linkages. Oxidized and reduced poly(3-chlorothiophene) were found to be blue and Bordeaux red, respectively, the intensity of such two colors depending on the potential used for the generation of the film. Moreover, morphological changes induced by oxidation–reduction processes indicated that this polymer is a potential candidate for the fabrication of very stable electrochromic devices. Accordingly, an all-thiophene electrochromic device made of poly(3,4-ethylenedioxythiophene) and poly(3-chlorothiophene) has been successfully fabricated. This device has been proved to exhibit very remarkable redox stability: the loss of electroactivity is 65% of the initial value after 390 cycles and remains stable at such a value for more than 500 cycles.
Published: 2012

28. A Conducting Polymer/Protein Composite with Bactericidal and Electroactive Properties

Author: Carlos Alemán, Francesc Estrany, Bruno Teixeira-Dias, David Aradilla, and Luis J. del Valle
Subjects: Conductive polymer, chemistry.chemical_classification, Materials science, Polymers and Plastics, General Chemical Engineering, Organic Chemistry, Composite number, Polymer, Electrochemistry, chemistry.chemical_compound, Adsorption, Polymerization, Chemical engineering, chemistry, PEDOT:PSS, Polymer chemistry, Materials Chemistry, Lysozyme
Abstract: Lysozyme, an enzyme with bactericidal activity over Gram-positive bacteria cells, is incorporated into PEDOT to prepare films with high biological and electrochemical activity. Two different strategies are used: (1) PEDOT films are coated with a layer of enzyme, which was adsorbed on the surface; and (2) the lysozyme is added to the polymerization medium used for the preparation of the conducting polymer. The enzyme adsorbed at the surface of the polymer produces a biphasic system that retains the electrochemical properties of the conducting polymer but is not able to protect against bacterial growth. In contrast, the addition of lysozyme to the polymerization medium results in a homogeneous composite with high bactericidal and electrochemical activities.
Published: 2011

29. Water absorption in polyaniline emeraldine base

Author: Carlos Alemán, Manel Canales, and David Aradilla
Subjects: chemistry.chemical_classification, chemistry.chemical_compound, Absorption of water, Materials science, Polymers and Plastics, Base (chemistry), chemistry, Inorganic chemistry, Polyaniline, Polymer chemistry, Materials Chemistry, Physical and Theoretical Chemistry, Condensed Matter Physics
Published: 2011

30. Symmetric Supercapacitors Based on Multilayers of Conducting Polymers

Author: Carlos Alemán, Francesc Estrany, and David Aradilla
Subjects: Supercapacitor, Conductive polymer, General Energy, Materials science, Capacitive sensing, Nanotechnology, Physical and Theoretical Chemistry, Electrochemical degradation, Electrochemistry, Porosity, Capacitance, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials
Abstract: The electrochemical and structural properties, charge capacitance, and stability upon oxidation−reduction cycling of multilayered systems based on alternated layers of different conducting polymers have been analyzed. Parallel studies have been carried out on individual conducting polymers for comparison. In all cases, the capacitive properties of multilayered systems were better than those of individual conducting polymers, which have been attributed to both the synergistic effects at the interfaces between consecutive layers and the higher porosity of the multilayered materials. Moreover, after hundreds of consecutive oxidation−reduction processes, the porosity in multilayered systems remained relatively high, whereas it was moderate or even null in the individual materials, this difference being crucial to understanding the very different electrochemical degradation of the specific capacitance observed for these materials. Multilayered systems have been used to fabricate a supercapacitor in the type I ...
Published: 2011

31. Different properties for poly(3,4-ethylenedioxythiophene) films derived from single or multiple polymerization steps

Author: Carlos Alemán, Francesc Estrany, and David Aradilla
Subjects: Conductive polymer, chemistry.chemical_classification, Polymers and Plastics, General Chemistry, Polymer, Surfaces, Coatings and Films, chemistry.chemical_compound, chemistry, Polymerization, Phase (matter), Electron affinity, Polymer chemistry, Materials Chemistry, Molecule, Physical chemistry, Thermal stability, Poly(3,4-ethylenedioxythiophene)
Abstract: Films of poly(3,4-ethylenedioxythiophene) were prepared with single and multiple electropolymerization steps, where the numbers of polymerization steps (n's) were 3, 5, and 7, with identical experimental conditions and total polymerization times (τ's). The electroactivity of the films prepared with multiple steps remained almost unaltered when n increased, with the ability of the films to store charge with n > 3 being smaller than that of the films with similar thicknesses but derived from a single electrodeposition step. In contrast, the stability of the films produced with n polymerization steps was significantly higher than that of the films derived from a single step with the same τ, with the difference between the two systems increasing with n, that is, τ used to yield the films. On the other hand, although the morphological and topological characteristics of the surface and the electrical conductivity were affected by the procedure used to produce the films, the organization of the polymer molecules in the crystalline phase, the thermal stability, and the electronic properties (ionization potential, electron affinity, and lowest π–π* transition energy) were practically identical in both cases. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011
Published: 2011

32. Structural and Electronic Properties of Poly[N-(2-cyanoalkyl)pyrrole]s Bearing Small Alkyl Groups

Author: Juan Torras, David Aradilla, Carlos Alemán, Universitat Politècnica de Catalunya. Departament d'Enginyeria Química, and Universitat Politècnica de Catalunya. IMEM - Innovació, Modelització i Enginyeria en (BIO) Materials
Subjects: Models, Molecular, Física::Mecànica quàntica [Àrees temàtiques de la UPC], Molecular Conformation, Conducting polymers, Electrons, Ring (chemistry), Electrochemistry, law.invention, chemistry.chemical_compound, law, Polymer chemistry, Materials Chemistry, Pyrroles, Polímers conductors, Physical and Theoretical Chemistry, Alkyl, Pyrrole, Electronic properties, chemistry.chemical_classification, Bearing (mechanical), Enginyeria electrònica [Àrees temàtiques de la UPC], Polymer, Surfaces, Coatings and Films, chemistry, Polymerization, Quantum Theory, Spectrophotometry, Ultraviolet, Oxidation-Reduction
Abstract: The electronic and structural properties of poly[N-(2-cyanoalkyl) pyrrole]s bearing short alkyl groups have been investigated using different methodologies. Specifically, the electronic properties of poly[N-(2- cyanoethyl)pyrrole], which was prepared by anodic polymerization, have been determined using both electrochemical and spectroscopic techniques. On the other hand, quantum mechanical calculations on model oligomers of poly- [N-(2-cyanomethyl)pyrrole] have been used to propose the conformation of an idealized polymer chain and to examine the influence of the conformation on the predicted electronic properties. Results indicated that the electronic properties of poly[N-(2-cyanoalkyl)pyrrole]s are not only influenced by effect of the conformation in the conjugation of the π-system but also by the existence of secondary oxidative processes on the pyrrole ring of selected repeating units. In this case, the combination of experimental information and quantum mechanical calculations proved to be essential to propose a structural model. This consists of a cross-linked structure formed by small branches of around nine repeating units in each one, with a carbonyl group at the last repeating unit of each branch.
Published: 2011

33. Properties of nanometric and micrometric multilayered films made of three conducting polymers

Author: Francesc Estrany, David Aradilla, Carlos Alemán, and Ramon Oliver
Subjects: Conductive polymer, Materials science, Polymers and Plastics, Organic Chemistry, Layer by layer, General Physics and Astronomy, Polypyrrole, Electrochemistry, chemistry.chemical_compound, chemistry, Electrical resistivity and conductivity, Polymer chemistry, Materials Chemistry, Polythiophene, Thin film, Composite material, Deposition (law)
Abstract: The electrochemical, electrical and morphological properties of multilayered films formed by alternated layers of poly(3,4-ethylenedioxythiophene), polypyrrole, and poly[ N -(2-cyanoethyl)pyrrole], which were prepared by electrochemical layer-by-layer deposition, have been investigated and compared with those of multilayered films formed by two conducting polymers. Results indicate that the electrochemical behavior of the films formed by three conducting polymers depends on the micrometric or nanometric thickness of the layers. Thus, the electroactivity increases until the thickness of these films reaches a threshold value (∼2 μm), while the electrostability of the films is very remarkable when their thickness is close to ∼4 μm or higher. On the other hand, comparison between multilayered systems made of two and three conducting polymers indicates that the third component introduces heterogeneity in the interfaces between consecutive layers, reducing the ability to store charge. Among the latter, multilayered films formed by poly(3,4-ethylenedioxythiophene) and polypyrrole have been found to be particularly electroactive and electrostable. The surface morphology and topography of the layers have been used to rationalize the electrochemical properties of the different materials.
Published: 2010

34. Morphology and growing of nanometric multilayered films formed by alternated layers of poly(3,4-ethylenedioxythiophene) and poly(N-methylpyrrole)

Author: Elaine Armelin, Carlos Alemán, Francesc Estrany, and David Aradilla
Subjects: Conductive polymer, Materials science, Metals and Alloys, Surfaces and Interfaces, Conductivity, Chronoamperometry, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, chemistry.chemical_compound, chemistry, Chemical engineering, PEDOT:PSS, Polymerization, Polymer chemistry, Materials Chemistry, Copolymer, Polythiophene, Poly(3,4-ethylenedioxythiophene)
Abstract: Multilayered nanometric films formed by alternated layers of conducting poly(3,4-ethylenedioxythiophene) and poly(N-methylpyrrole) doped with perchlorate anions (ml-PEDOT/PNMPy) have been prepared using a layer-by-layer electrodeposition technique combined with a very small polymerization time. The mechanisms of formation and growth of the resulting multilayered systems have been investigated using Atomic Force Microscopy (AFM), and compared with those obtained for the corresponding homopolymers, which were prepared using identical experimental conditions. Furthermore, the local conductivity, electroactivity and electrostability have been also examined. Analyses of the morphology, topography and roughness of the surfaces indicate that the formation and growth of the multilayered films strongly depend on the number of layers as well as on the chemical nature of the conducting polymer. Interestingly, AFM reflects that the formation and growth of the ml-PEDOT/PNMPy films are significantly different from those of PEDOT and PNMPy homopolymers. The electrical and electrochemical properties of the systems under study are fully consistent with the proposed mechanisms. Results evidenced that multilayered systems formed by two conducting polymers are more advantageous from a technological point of view than the corresponding copolymers.
Published: 2010

35. Conducting poly(3,4-ethylenedioxythiophene)-montmorillonite exfoliated nanocomposites

Author: Carlos Alemán, Jordi Puiggalí, María Teresa Casas, Denise Schermann Azambuja, David Aradilla, Francesc Estrany, and Carlos A. Ferreira
Subjects: Conductive polymer, Aqueous solution, Nanocomposite, Materials science, Polymers and Plastics, Organic Chemistry, General Physics and Astronomy, Electrochemistry, chemistry.chemical_compound, Montmorillonite, Chemical engineering, chemistry, Transmission electron microscopy, Polymer chemistry, Bentonite, Materials Chemistry, Poly(3,4-ethylenedioxythiophene)
Abstract: Exfoliated nanocomposites formed by poly(3,4-ethylenedioxythiophene) and different concentrations of non-modified montmorillonite (bentonite), which range from 1% to 10% w/w, have been prepared by anodic electropolymerization in aqueous solution. Analyses of the electrochemical and electrical properties reveal that the electroactivity of the nanocomposites is higher than that of the individual homopolymer, while the electrical conductivity of the two systems is practically identical. On the other hand, the exfoliated distribution of the clay in the polymeric matrix and the morphology of the prepared materials have been characterized using transmission electron microscopy, X-ray diffraction and atomic force microscopy. The overall of the results represents a significant improvement with respect to other nanocomposites constituted by conducting polymers and clays, including those involving poly(3,4-ethylenedioxythiophene), and evidences the reliability of the preparation procedure employed in this work.
Published: 2010

36. Novel Cell Design for an Operando and in-Situ Study of Li-Ion Battery Electrode Aging Mechanisms through SAXS and SANS Measurements

Author: Christopher Logan Berhaut, Diana Zapata Dominguez, Samuel Tardif, Arnaud De Geyer, Stéphanie Pouget, David Aradilla, and Sandrine Lyonnard
Abstract: Due to an impressive and continuous improvement in performance, the use of lithium ion batteries (LiBs) has greatly increased since this technology was first commercialized by Sony in 1990 and is quickly spreading to more demanding applications. Today, LiBs are not only used to power portable electronic devices such as smartphones or laptops but also larger systems such as electric vehicles. One way of contributing to the continuing success of LiBs in the automotive field is to increase their energy density. Silicon has received considerable attention in recent years due to its high theoretical capacity. However, because of (i) the severe volume expansion/shrinkage of this material during cycling, which leads to the pulverization of the electrode and to a rapid capacity fading, and (ii) the first cycle high irreversible capacity, the implementation of silicon-based negative electrodes in commercial LiBs remains challenging. Two possible solutions have been approached to overcome these problems: (i) Reducing the size of the silicon particles, and (ii) using dual-phase (a dispersed active phase in an inactive host matrix) composite electrodes. Pulverization is alleviated by reducing silicon particles to nanosized particles or by using a homogenous inactive host matrix which acts as a buffer against volumetric changes. However, because of poor electrode structural stability during cycling, the use of nanoparticles only cannot reduce the capacity degradation and hence, be a practical solution. Even though the total capacity of silicon-based composite electrodes cannot be as high as that of pure silicon electrodes, composite electrodes allow a low first cycle irreversible capacity and good capacity retention. We have undertaken the study of the aging mechanisms in composite Si based electrodes, by means of small angle X-ray and neutron scattering (SAXS and SANS). These characterization techniques give access to the electrode nanostructure and its evolution upon cycling. Ex-situ measurements provided useful information on the evolution of the morphology of small domains. Indeed, initial results of SANS measurements performed at the Laue Langevin Institute (ILL, Grenoble), presented in Figures a and b, show the existence of two intensity regions at high and low Q values. Those respectively give information on small and large domains within the electrode. Interestingly, upon lithiating the electrode, the intensity in the intermediate and high-Q regions increases, while the low-Q region remains unchanged (Figure b). Moreover, after 100 cycles, the pristine electrode spectrum is recovered whereas it is not the case after 300 cycles (Figure a) thus showing signs of aging from the silicon-based composite electrode. In order to probe in real-time the effects of lithiation/delithiation on the composite anode nanostructure and, avoid any risk of altering the sample in between the opening of the cell and sample preparation, in-situ and operando measurements were conducted. For this purpose new electrochemical cells (Figure c) were designed using respectively beryllium or titanium windows. Particular care has been taken to ensure that the cycling conditions of the electrochemical system are as close as possible to those of a coin cell, with the use of a separator and applied pressure on the electrodes. In this talk we will present the first results on the evolution of the nanostructure of the composite electrodes. Figure 1
Published: 2018

37. From Poly(3,4-ethylenedioxythiophene) to Poly(3,4-phenylenedioxythiophene): Impact of the Substitution of the Ethylene Bridge by the Phenyl Ring on the Molecular Properties

Author: Sergio Carrión, Jordi Casanovas, Francisco Rodríguez-Ropero, Carlos Alemán, David Aradilla, and David Zanuy
Subjects: chemistry.chemical_classification, Conductive polymer, Acetonitriles, Materials science, Polymers, Doping, Benzene, Polymer, Ethylenes, Bridged Bicyclo Compounds, Heterocyclic, Surfaces, Coatings and Films, Solvent, chemistry.chemical_compound, chemistry, Atomic electron transition, Polymer chemistry, Materials Chemistry, Quantum Theory, Physical chemistry, Gases, Physical and Theoretical Chemistry, Acetonitrile, Poly(3,4-ethylenedioxythiophene)
Abstract: The structural and electronic properties of poly(3,4-phenylenedioxythiophene) and poly(3,4-ethylenedioxythiophene) have been studied using quantum mechanical methods. Calculations have been performed considering a series of oligomers up to 12 repeating units in the neutral and cation states, results being used to extrapolate the properties of the two polymers in the undoped and doped states. Moreover, the electronic properties were estimated in the gas phase and acetonitrile solution, the latter solvent being used in the electrogeneration of the two conducting polymers. A detailed analysis of the results indicates that, although the pi-pi* transition energy of poly(3,4-ethylenedioxythiophene) is lower than that of poly(3,4-phenylenedioxythiophene) in the neutral state, the latter behaves as excellent electronic conductor upon p-doping. Accordingly, the oxidized poly(3,4-phenylenedioxythiophene) shows the lowest pi-pi* electron transition energy.
Published: 2010

38. Properties of nanometric and submicrometric multilayered films of poly(3,4-ethylenedioxythiophene) and poly(N-methylpyrrole)

Author: Elaine Armelin, Carlos Alemán, David Aradilla, Francesc Estrany, and Ramon Oliver
Subjects: Conductive polymer, Morphology (linguistics), Materials science, Polymers and Plastics, Organic Chemistry, General Physics and Astronomy, Chronoamperometry, Electrochemistry, chemistry.chemical_compound, Chemical engineering, chemistry, Polymerization, Polymer chemistry, Materials Chemistry, Thin film, Layer (electronics), Poly(3,4-ethylenedioxythiophene)
Abstract: Multilayered films formed by 3, 5 and 7 alternated layers of poly(3,4-ethylenedioxythiophene) and poly(N-methylpyrrole) have been prepared by chronoamperometry under a constant potential of 1.4 V using a layer-by-layer electrodeposition technique. In order to examine influence of the interface:bulk dimensional ratio, the thickness of the yielded films was reduced from the submicrometric to the nanometric scale by decreasing the polymerization time of each layer from 100 s to 10 s. The electroactivity, electrochemical characteristics and morphologies of the resulting multilayered films have been compared with those obtained for both single-component poly(3,4-ethylenedioxythiophene) films prepared using identical experimental conditions and previously reported multilayered films with thickness within the micrometric scale [Estrany F, Aradilla D, Oliver R, Aleman C. Eur Polym J 2007;43:1876].
Published: 2008

39. Application of multilayered particles formed by poly(3,4-ethylenedioxythiophene) and poly(N-methylpyrrole) as anti-corrosive additives of conventional organic coatings

Author: Francesc Estrany, Carlos Alemán, Ramon Oliver, David Aradilla, Cintia Ocampo, and Elaine Armelin
Subjects: Conductive polymer, Materials science, N-methylpyrrole, Mechanical Engineering, Metals and Alloys, General Medicine, Epoxy, engineering.material, Surfaces, Coatings and Films, Corrosion, chemistry.chemical_compound, chemistry, Coating, Mechanics of Materials, visual_art, Materials Chemistry, visual_art.visual_art_medium, engineering, Environmental Chemistry, Composite material, Poly(3,4-ethylenedioxythiophene), Volume concentration
Abstract: Multilayered systems containing 3 or 5 layers of poly(3,4-ethylenedioxythiophene) and poly(N-methylpyrrole) have been prepared using a layer-by-layer electrodeposition technique. These multilayered systems have been found to present very high electro-activities suggesting that their performance as anti-corrosive additive of conventional organic coatings (paints) could be even better than that of single-component conducting polymers. The performance of the prepared multilayered systems as anti-corrosive additives of epoxy paints has been checked. For this purpose, accelerated corrosion tests were performed using an aggressive solution medium. Analysis of the corroded area indicates that the addition of a low concentration (0.2% w/w) of these multilayered systems to the paint formulation enhances significantly the corrosion protection imparted by the coating.
Published: 2007

40. Cellular adhesion and proliferation on poly(3,4-ethylenedioxythiophene): Benefits in the electroactivity of the conducting polymer

Author: Elaine Armelin, Francesc Estrany, David Aradilla, Carlos Alemán, A. Gamez, L. J. del Valle, Francesc Sepulcre, and Ramon Oliver
Subjects: Conductive polymer, Materials science, Polymers and Plastics, Biocompatibility, Organic Chemistry, General Physics and Astronomy, Adhesion, chemistry.chemical_compound, Chemical engineering, chemistry, Polymerization, Monolayer, Polymer chemistry, Materials Chemistry, Cyclic voltammetry, Cell adhesion, Poly(3,4-ethylenedioxythiophene)
Abstract: Cell adhesion and proliferation in poly(3,4-ethylenedioxythiophene), an electroactive polythiophene derivative generated by anodic polymerization, has been investigated. Results show that epithelial cells Hep-2 present significant activity on the surface of poly(3,4-ethylenedioxythiophene) electrodeposited on stainless steel electrodes, no sign of cytotoxicity being detected for this conducting polymer. Indeed, seeded and cultured cells bound better to poly(3,4-ethylenedioxythiophene) than to uncoated stainless steel, the latter substrate being used as a control. Furthermore, the electrochemical characteristics of poly(3,4-ethylenedioxythiophene) covered with cells was determined in different biological media using cyclic voltammetry experiments. Results reveal a significant increase in the electroactivity of this material when it is covered with a cellular monolayer. The overall of the results evidences not only the biocompatibility of poly(3,4-ethylenedioxythiophene) with Hep-2 cells but also their electrocompatibility.
Published: 2007

41. Electroactivity, electrochemical stability and electrical conductivity of multilayered films containing poly(3,4-ethylendioxythiophene) and poly(N-methylpyrrole)

Author: Ramon Oliver, Carlos Alemán, Francesc Estrany, and David Aradilla
Subjects: chemistry.chemical_classification, Conductive polymer, Materials science, N-methylpyrrole, Polymers and Plastics, Organic Chemistry, General Physics and Astronomy, Electrical stability, Polymer, Electrochemistry, chemistry, Chemical engineering, Electrical resistivity and conductivity, Polymer chemistry, Materials Chemistry, Electroactive polymers, Copolymer
Abstract: Multilayered systems of poly(3,4-ethylendioxythiophene) and poly(N-methylpyrrole) have been prepared using a layer-by-layer electrodeposition technique. The electrochemical and electrical properties of films formed by 3, 5, 7 and 9 layers have been characterized and compared with those of pure polymers and copolymers prepared from mixtures of 3,4-ethylendioxythiophene and N-methylpyrrole with various concentration ratios. Results indicate that the electroactivity and electrical stability of the multilayered systems are higher than those of both poly(3,4-ethylendioxythiophene) and copolymers. Furthermore, these electrochemical properties improve when the number of layers increases. On the other hand, the electrical conductivity of the multilayered systems is slightly lower than that of pure poly(3,4-ethylendioxythiophene), and significantly higher than those of poly(N-methylpyrrole) and copolymers.
Published: 2007

42. 3D hierarchical assembly of ultrathin MnO2 nanoflakes on silicon nanowires for high performance micro-supercapacitors in Li- doped ionic liquid

Author: Pascal Gentile, Pedro Gómez-Romero, David Aradilla, Jan Wimberg, Saïd Sadki, Gérard Bidan, Deepak P. Dubal, Thomas J. S. Schubert, ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Laboratoire d'Electronique Moléculaire Organique et Hybride (LEMOH), European Project: 309143,EC:FP7:ENERGY,FP7-ENERGY-2012-1-2STAGE,NEST(2012), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Silicon, Materials science, Nanowire, chemistry.chemical_element, Energy-Storage, Nanotechnology, Electrolyte, All-Solid-State, Electrochemical Capacitors, 7. Clean energy, Article, Wafer, Fiber, Electrodes, Films, [PHYS]Physics [physics], Supercapacitor, Multidisciplinary, Doping, Oxide, Conversion, Carbon, Porous, chemistry, Electrode, Mesoporous material
Abstract: Building of hierarchical core-shell hetero-structures is currently the subject of intensive research in the electrochemical field owing to its potential for making improved electrodes for high-performance micro-supercapacitors. Here we report a novel architecture design of hierarchical MnO2@silicon nanowires (MnO2@SiNWs) hetero-structures directly supported onto silicon wafer coupled with Li-ion doped 1-Methyl-1-propylpyrrolidinium bis(trifluromethylsulfonyl)imide (PMPyrrBTA) ionic liquids as electrolyte for micro-supercapacitors. A unique 3D mesoporous MnO2@SiNWs in Li-ion doped IL electrolyte can be cycled reversibly across a voltage of 2.2 V and exhibits a high areal capacitance of 13 mFcm−2. The high conductivity of the SiNWs arrays combined with the large surface area of ultrathin MnO2 nanoflakes are responsible for the remarkable performance of these MnO2@SiNWs hetero-structures which exhibit high energy density and excellent cycling stability. This combination of hybrid electrode and hybrid electrolyte opens up a novel avenue to design electrode materials for high-performance micro-supercapacitors.
Published: 2015

43. Diamond-coated silicon nanowires for enhanced micro-supercapacitor with ionic liquids

Author: Dorian Gaboriau, Pascal Gentile, Gérard Bidan, Jan Wimberg, W. Mueller-Sebert, Pedro Gómez-Romero, Thomas J. S. Schubert, Girish S. Gund, Deepak P. Dubal, David Aradilla, and Saïd Sadki
Subjects: Supercapacitor, Fabrication, business.industry, Diamond, Chemical vapor deposition, engineering.material, chemistry.chemical_compound, Coating, chemistry, Electrode, Ionic liquid, engineering, Optoelectronics, Wafer, business
Abstract: Silicon nanowires (SiNWs) and diamond-coated SiNWs (D@SiNWs) on highly n-doped silicon wafer substrates were prepared through standard chemical vapor deposition (CVD) method as electrodes for micro-supercapacitors. The surface of electrodes exhibited uniform distribution of SiNWs on silicon wafer and continuous diamond coating on SiNWs. Electrochemical measurements were carried out in order to test the combined effect of using Ionic Liquid electrolytes and diamond coating on SiNWs on energy storage performance. Optimal values of areal capacitance, energy density and power densities were 317 µF cm−2, 0.13 µWh cm−2 and 150 µW cm−2, respectively. So, the work reported here confirms the suitability and compatibility of D@SiNWs electrode materials and ionic liquid electrolytes for the fabrication of high-performing and robust micro-supercapacitors.
Published: 2015

44. Vertically aligned graphene nanosheets on silicon using an ionic liquid electrolyte: towards high performance on-chip micro-supercapacitors

Author: Gérard Bidan, Marc Delaunay, Saïd Sadki, Jean-Michel Gérard, David Aradilla, Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Nanophysique et Semiconducteurs (NPSC), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Laboratoire d'Electronique Moléculaire Organique et Hybride (LEMOH), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Silicon, chemistry.chemical_element, Double-Layer Capacitor, Density, Nanotechnology, Energy-Storage, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 7. Clean energy, 01 natural sciences, Capacitance, Electrochemical Capacitors, law.invention, chemistry.chemical_compound, Fabrication, law, High-Power, General Materials Science, Operation, Supercapacitor, [PHYS]Physics [physics], Renewable Energy, Sustainability and the Environment, business.industry, Graphene, Raman-Spectroscopy, General Chemistry, 021001 nanoscience & nanotechnology, Carbon, 0104 chemical sciences, chemistry, Ionic liquid, Optoelectronics, 0210 nano-technology, business, Current density, Carbide Nanowires
Abstract: International audience; Vertically oriented graphene nanosheets were synthesized by an alternative and simple approach based on electron cyclotron resonance-plasma enhanced chemical vapor deposition (ECR-CVD) onto highly doped silicon substrates. The as-grown graphene electrodes were employed in a symmetric micro-supercapacitor using an aprotic ionic liquid [N-methyl-N-propylpyrrolidinium bis(trifluoromethyl-sulfonylimide); PYR13TFSI] as electrolyte. The device was able to deliver an outstanding specific capacitance value of 2 mF cm(-2), a power density value of 4 mW cm(-2) and an energy density value of 4 mu W h cm(-2) operating at a large and stable cell voltage of 4 V with a quasi-ideal capacitive behaviour. Moreover, the lifetime of the device exhibited a remarkable electrochemical stability retaining 80% of the initial capacitance after 150 000 galvanostatic charge-discharge cycles at a high current density of 1 mA cm(-2). This excellent electrochemical performance results from the obtained channel-based 3-D graphene network promoting rapid electrolyte ion-transport and short diffusion paths.
Published: 2015

45. An innovative 3-D nanoforest heterostructure made of polypyrrole coated silicon nanotrees for new high performance hybrid micro-supercapacitors

Author: Pedro Gómez-Romero, Gérard Bidan, Pascal Gentile, Jan Wimberg, Saïd Sadki, Maxime Boniface, Deepak P. Dubal, Thomas J. S. Schubert, Dorian Gaboriau, David Aradilla, Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'Electronique Moléculaire Organique et Hybride (LEMOH), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Laboratoire d'Etude des Matériaux par Microscopie Avancée (LEMMA ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), European Project: 309143,EC:FP7:ENERGY,FP7-ENERGY-2012-1-2STAGE,NEST(2012), European Commission, Commissariat à l'Ènergie Atomique et aux Ènergies Alternatives (France), Ministère de la Défense (France), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG)
Subjects: Materials science, Silicon, Electrochemical Energy-Storage, chemistry.chemical_element, 02 engineering and technology, Chemical vapor deposition, Capacitors, 010402 general chemistry, Polypyrrole, Electrochemistry, 7. Clean energy, 01 natural sciences, Capacitance, chemistry.chemical_compound, Fabrication, Ultracapacitors, Devices, General Materials Science, Arrays, Electrodes, Films, Supercapacitor, Conductive polymer, [PHYS]Physics [physics], Renewable Energy, Sustainability and the Environment, Nanowires, General Chemistry, 021001 nanoscience & nanotechnology, Carbon, 0104 chemical sciences, chemistry, Chemical engineering, Electrode, 0210 nano-technology
Abstract: In this work, an innovative 3-D symmetric micro-supercapacitor based on polypyrrole (PPy) coated silicon nanotree (SiNTr) hybrid electrodes has been fabricated. First, SiNTrs were grown on silicon substrates by chemical vapor deposition (CVD) and then via an electrochemical method, the conducting polymer coating was deposited onto the surface of SiNTr electrodes. This study illustrates the excellent electrochemical performance of a hybrid micro-supercapacitor device using the synergistic combination of both PPy as the electroactive pseudo-capacitive material and branched SiNWs as the electric double layer capacitive material in the presence of an aprotic ionic liquid (N-methyl-N-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide; PYR13TFSI) as the electrolyte. The hybrid device exhibited a specific capacitance as high as ∼14 mF cm−2 and an energy density value of ∼15 mJ cm−2 at a wide cell voltage of 1.5 V using a high current density of 1 mA cm−2. Furthermore, a remarkable cycling stability after thousands of galvanostatic charge–discharge cycles with a loss of approximately 30% was obtained. The results reported in this investigation demonstrated that PPy coated SiNTr-based micro-supercapacitors exhibit the best performances among hybrid micro-supercapacitors made of silicon nanowire electrodes grown by CVD in terms of specific capacitance and energy density., This project has received funding from the European Union's Seventh Program for Research, Technological Development and Demonstration under Grant agreement no. 309143 (2012–2015). Dorian Gaboriau thanks the 'Délégation Générale pour l'Armament' (DGA) and the CEA for financial support.
Published: 2015

46. Diamond-coated silicon wires for supercapacitor applications in ionic liquids

Author: Georgia Lewes-Malandrakis, Christoph E. Nebel, W. Müller-Sebert, Marco Wolfer, Fang Gao, Thomas J. S. Schubert, Pascal Gentile, David Aradilla, Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), European Project: 309143,EC:FP7:ENERGY,FP7-ENERGY-2012-1-2STAGE,NEST(2012), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), and Publica
Subjects: Materials science, Silicon, Nanowire, chemistry.chemical_element, Nanotechnology, 02 engineering and technology, Chemical vapor deposition, engineering.material, 010402 general chemistry, 01 natural sciences, Capacitance, Electrochemical Capacitors, law.invention, chemistry.chemical_compound, Fabrication, law, Materials Chemistry, Core-shell nanowires, Electrical and Electronic Engineering, Electrodes, Film, Supercapacitor, [PHYS]Physics [physics], business.industry, Graphene, Mechanical Engineering, Temperature, Diamond, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Ionic liquids, Nanocrystalline diamond, chemistry, Surface enlargement, Doped Diamond, Ionic liquid, engineering, Optoelectronics, 0210 nano-technology, business
Abstract: International audience; For a long time sp(2) carbon has been the dominating material for supercapacitor applications. In this paper a new concept of using boron-doped diamond for supercapacitors is proposed. Diamond surface enlargement is realized via bottom-up template-growth. In this method, silicon nanowire electrodes are coated with a thin (similar to 100 nm) layer of nanocrystalline diamond (NCD) by microwave enhanced chemical vapor deposition (MWCVD). The quality of overgrowth is characterized by high resolution scanning electron microscopy which reveals a homogeneous coverage of diamond on Si nanowire surface. To enhance the potential window to 4 V, a room temperature ionic liquid is used as electrolyte. The dilution of the ionic liquid is investigated in terms of conductivity and specific capacitance. The capacitance as measured via cyclic voltammetry reaches 105 mu F/cm(2). An energy density of 84 mu J/cm(2) and a high power density of 0.94 mW/cm(2) are obtained in combination with good stability of over 10,000 charging/discharging cycles. (C) 2014 Elsevier B.V. All rights reserved.
Published: 2015

47. SiNWs-based electrochemical double layer micro-supercapacitors with wide voltage window (4V) and long cycling stability using a protic ionic liquid electrolyte

Author: Pedro Gómez-Romero, Thomas J. S. Schubert, Gérard Bidan, Saïd Sadki, Boyan Iliev, Pascal Gentile, David Aradilla, Vanesa Ruiz, Jan Wimberg, Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), Laboratoire d'Electronique Moléculaire Organique et Hybride (LEMOH), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), European Project: 309143,EC:FP7:ENERGY,FP7-ENERGY-2012-1-2STAGE,NEST(2012), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), and Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Subjects: Performance, Analytical chemistry, Ionic Liquids, Micro-Supercapacitors, Energy-Storage, Electrolyte, Capacitors, Electrochemistry, 7. Clean energy, Industrial and Manufacturing Engineering, chemistry.chemical_compound, Devices, General Materials Science, Electrical and Electronic Engineering, Deposition, Power density, Chemical Vapor, Supercapacitor, [PHYS]Physics [physics], Silicon Nanowires, Carbon, Dielectric spectroscopy, Surface, chemistry, Chemical engineering, Electrode, Ionic liquid, Doped Silicon Nanowires, Cyclic voltammetry
Abstract: International audience; The present work reports the use and application of a novel protic ionic liquid (triethylammonium bis(trifluoromethylsulfonyl)imide; NEt3H TFSI) as an electrolyte for symmetric planar micro-supercapacitors based on silicon nanowire electrodes. The excellent performance of the device has been successfully demonstrated using cyclic voltammetry, galvanostatic charge-discharge cycles and electrochemical impedance spectroscopy. The electrochemical characterization of this system exhibits a wide operative voltage of 4 V as well as an outstanding long cycling stability after millions of galvanostatic cycles at a high current density of 2 mA cm(-2). In addition, the electrochemical double layer micro-supercapacitor was able to deliver a high power density of 4 mW cm(-2) in a very short time pulses (a few ms). Our results could be of interest to develop prospective on-chip micro-supercapacitors using protic ionic liquids as electrolytes with high performance in terms of power and energy densities.
Published: 2015

48. Novel hybrid micro-supercapacitor based on conducting polymer coated silicon nanowires for electrochemical energy storage

Author: Gérard Bidan, Hülya Sahin, Pascal Gentile, Vanesa Ruiz, Patrick Weathers, Thomas J. S. Schubert, Pedro Gómez-Romero, Saïd Sadki, Fleur Thissandier, David Aradilla, Polymères Conducteurs Ioniques (PCI), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Service de Chimie Inorganique et Biologique (SCIB - UMR E3), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Centre National de la Recherche Scientifique (CNRS), Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Structures et propriétés d'architectures moléculaire (SPRAM - UMR 5819), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), Institut de Ciència de Materials de Barcelona (ICMAB), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Ionic Liquids Technologies GmbH (IOLITECH), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), European Commission, and Commissariat à l'Ènergie Atomique et aux Ènergies Alternatives (France)
Subjects: Materials science, General Chemical Engineering, Nanotechnology, 02 engineering and technology, Electrolyte, engineering.material, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Capacitance, [SPI]Engineering Sciences [physics], Coating, Specific energy, [CHIM]Chemical Sciences, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, ComputingMilieux_MISCELLANEOUS, Power density, Supercapacitor, Conductive polymer, [SPI.NRJ]Engineering Sciences [physics]/Electric power, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, engineering, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 0210 nano-technology
Abstract: The development of a novel hybrid symmetric micro-supercapacitor based on poly(3,4-ethylenedioxythiophene) coated silicon nanowires using an ionic liquid (N-methyl-N-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide) as an electrolyte has been demonstrated. The hybrid supercapacitor device was able to deliver a specific energy of 10 W h kg-1 and a maximal power density of 85 kW kg-1 at a cell voltage of 1.5 V. The hybrid device exhibited long lifetime and an outstanding electrochemical stability retaining 80% of the initial capacitance after thousands of galvanostatic charge-discharge cycles at a high current density of 1 mA cm-2. The improvement of the capacitive properties compared with the bare SiNWs was attributed to the pseudo-capacitive behavior induced by the conducting polymer coating., The authors acknowledge the CEA for financial support of this work. This project has received funding from the European Union's Seventh Programme for research, technological development and demonstration under grant agreement no. 309143 (2012–2015).
Published: 2014

49. High performance of symmetric micro-supercapacitors based on silicon nanowires using N-methyl-N-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide as electrolyte

Author: Gérard Bidan, Pascal Gentile, Elzbieta Frackowiak, Pedro Gómez-Romero, Vanesa Ruiz, Hülya Sahin, Saïd Sadki, Thomas J. S. Schubert, David Aradilla, Commissariat à l'Ènergie Atomique et aux Ènergies Alternatives (France), European Commission, Silicon Nanoelectronics Photonics and Structures (SiNaps), PHotonique, ELectronique et Ingénierie QuantiqueS (PHELIQS), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Structures et propriétés d'architectures moléculaire (SPRAM - UMR 5819), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Institut Nanosciences et Cryogénie (INAC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), Faculty of Chemical Technology, Poznan University of Technology (PUT), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Chemical vapour deposition, Materials science, Silicon, micro-supercapacitors, Micro-supercapacitors, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, Chemical vapor deposition, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Capacitance, chemical vapor deposition, ionic liquids, chemistry.chemical_compound, Silicon nanowires, General Materials Science, Electrical and Electronic Engineering, Supercapacitor, Renewable Energy, Sustainability and the Environment, electrochemical energy storage, [SPI.NRJ]Engineering Sciences [physics]/Electric power, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Ionic liquids, Chemical engineering, chemistry, Ionic liquid, Electrochemical energy storage, 0210 nano-technology, Faraday efficiency
Abstract: This work describes the development and performance of a symmetric micro-supercapacitor made of nanostructured electrodes based on silicon nanowires (SiNWs) deposited using chemical vapor deposition (CVD) on silicon substrates. The performance of the SiNWs micro-supercapacitor employing an aprotic ionic liquid (N-methyl-N-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide) (PYR13TFSI) as an electrolyte was able to deliver a maximal power density of 182mWcm-2 and a specific energy of 190μJcm-2 operating at a wide cell voltage of 4V with a quasi-ideal capacitive behavior. The lifetime of the device exhibited a remarkable electrochemical stability retaining 75% of the initial capacitance after several million galvanostatic charge-discharge cycles at a high current density of 1mAcm-2. Furthermore, a coulombic efficiency of approximately 99% was obtained after galvanostatic cycling test without structural degradation on the morphology of SiNWs., The authors acknowledge the CEA for financial support of this work. This project has received funding from the European Union׳s Seventh Program for Research, Technological Development and Demonstration under Grant agreement no. 309143 (2012–2015).
Published: 2014

50. (Invited) Bottom-up Silicon Nanostructures: A Toolbox for Integrated on-Chip Edlcs

Author: Dorian Gaboriau, Mylène Brachet, Maxime Boniface, David Aradilla, Dmitry Aldakov, Gerard Bidan, Jean Le Bideau, Thierry Brousse, Pascal Gentile, and Said Sadki
Abstract: The current trend towards miniaturized and autonomous electronic devices requires innovative energy storage solutions. For instance, autonomous micro-sensor networks or implantable medical devices would need a robust power source with an extended cyclability as well as a large power density, which might be out of the scope of conventional battery technologies. For such applications, Electrochemical Double Layer Capacitors (EDLCs) are promising alternatives, and their integration “on-chip” could allow tremendous innovations to emerge.1 However, finding a suitable “on-chip” EDLC technology implies addressing key challenges, such as temperature resistance, silicon industry compatibility and good electrochemical performances on a small footprint. Although often considered as an “unconventional” supercapacitive electrode material, bottom-up, highly-doped nanostructured silicon offers extremely promising characteristics, both as bare electrode material in EDLCs2, 3 or as current collector for pseudo-capacitive materials.4 The fine morphological tuning of the nanostructure allowed by the bottom-up approach permits a careful design of the electrodes’ architectures, with considerable freedom compared to other techniques. Such latitude allows the optimization of porosity as well as ionic and electronic pathways while keeping robust mechanical performances, depending on the target application and other requirements such as the electrolyte, functionalization by pseudo-capacitive materials or other surface modifications. Moreover, using silicon as EDLC electrode material instead of carbon allows developments towards “on-chip” integration and potential production scale-up considerably easier using standard silicon industry processes for small micro-sized energy storage devices. Nanostructures such as silicon nanowires (Si-NWs) or nanotrees (Si-NTrs) demonstrated excellent cyclability with more than 1 million cycles of galvanostatic charge/discharge under a 4 V wide electrochemical windows in EMI-TFSI ionic liquid, with large power densities and good capacitance values.2,3 The aim of the present study is to provide insight on the potentialities of bottom-up silicon nanostructures as a toolbox for designing “on-chip” energy storage devices, by addressing several key challenges. In particular, the accessible surface area of electrodes can be greatly improved through careful optimization of the nanostructure morphologies, resulting in larger capacitances. A systematic study was conducted over different growth parameters, leading to interestingly diverse morphologies ranging from hyper branched Si-NTrs to a 3D interpenetrated highly conductive silicon nanowires network. We demonstrated capacitance values as high as 1.7 mF.cm-2 in a 3 electrodes cell and excellent energy and maximum power densities for symmetric 2 electrodes devices (respectively 2.8 mJ.cm-2 and 235 mW.cm-2) while retaining 80 % of the capacitance after 106 galvanostatic charge/discharge cycles. Additionally, a quasi-ideal capacitive behavior was retained throughout long term cycling, with linear and symmetric galvanostatic profiles even after millions of cycles. Furthermore, surface modification of the silicon nanostructures by Atomic Layer Deposited thin Al2O3 films boosted electrochemical performances, allowing symmetric 2 electrode devices to reach an unprecedented cell voltage of 5.5 V, improving energy and maximum power densities compared to unmodified nanostructured silicon. The cyclability was also largely enhanced, with only 3% capacitance fade after 106 galvanostatic charge/discharge cycles at 4 V, and no further degradation even after several subsequent 105 cycles over 5 V. Finally, “on-chip” integrated devices were designed by growing optimized nanostructures on an interdigitated electrode pattern, demonstrating the compatibility of our material with standard micro-patterning processes. In combination with a solid-state ionogel electrolyte, the devices can also display remarkable electrochemical performances over a wide temperature range (between 15° C and 100° C), and a resistance to the “solder reflow” conditions, paving the way to fully integrated “on-chip” micro-supercapacitors which fulfill the key challenges for future applications. (1) Beidaghi, M.; Gogotsi, Y. Energy & Environ. Sci. 2014, 7 (3), 867-884 (2) Thissandier, F. ; Gentile, P. ; Pauc, N. ; Brousse, T. ; Bidan, G. ; Sadki, S. Nano Energy 2014, 5, 20-27 (3) Thissandier, F. ; Gentile, P. ; Brousse, T. ; Bidan, G. ; Sadki, S. J. Power Sources 2014, 269, 740-746 (4) Aradilla, D. ; Gaboriau, D. ; Bidan, G. ; Gentile, P. ; Boniface, M. ; Dubal, D. ; Gómez-Romero, P. ; Wimberg, J. ; Schubert, T.J.S. ; Sadki, S. J. Mater. Chem. A 2015, 3, 13978-13985 Figure 1
Published: 2016

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