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3. Na2.4Al0.4Mn2.6O7 anionic redox cathode material for sodium-ion batteries – a combined experimental and theoretical approach to elucidate its charge storage mechanism

Author

Cindy Soares, Begoña Silván, Yong-Seok Choi, Veronica Celorrio, Valerie R. Seymour, Giannantonio Cibin, John M. Griffin, David O. Scanlon, and Nuria Tapia-Ruiz

Subjects
Renewable Energy, Sustainability and the Environment, General Materials Science, General Chemistry
Abstract

Al substitution and subsequent Na excess in Na2Mn3O7 were achieved by a ceramic method, realizing the high-performance Na2.4Al0.4Mn2.6O7 oxygen-redox cathode for Na-ion batteries. A comparison between the two cathodes revealed the role of Al doping.

Published
2022

4. Importance of Composite Electrolyte Processing to Improve the Kinetics and Energy Density of Li Metal Solid-State Batteries

Author

Frederic Aguesse, Begoña Silván, Jakub Zagórski, Damien Saurel, and Anna Llordes

Subjects
Materials science, Kinetics, Solid-state, Energy Engineering and Power Technology, 02 engineering and technology, Metal anode, Electrolyte, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Metal, Chemical engineering, visual_art, Materials Chemistry, Electrochemistry, Energy density, visual_art.visual_art_medium, Chemical Engineering (miscellaneous), Electrical and Electronic Engineering, 0210 nano-technology, Electrical conductor, Composite electrolyte
Abstract

Solid-state batteries with a Li metal anode and polymer–ceramic electrolytes hold the promise to boost safety and energy density, provided that stable conductive interfaces are achieved. Here, by f...

Published
2020

5. 2021 roadmap for sodium-ion batteries

Author

John T. S. Irvine, Emma Kendrick, Valerie R. Seymour, Aamod V. Desai, Edmund J. Cussen, Peter Gross, Andrew J. Naylor, Maria-Magdalena Titirici, Jake M. Brittain, Rebecca Boston, Ruth Sayers, Stewart A. M. Dickson, Sudeshna Sen, Sara I. R. Costa, Zhuangnan Li, Ashish Rudola, Heather Au, Dominic S. Wright, Nuria Tapia-Ruiz, Yongseok Choi, Hande Alptekin, John M. Griffin, Martin O. Jones, Marco Amores, Shahin Nikman, Eun Jeong Kim, A. Robert Armstrong, Reza Younesi, Maria Crespo Ribadeneyra, Laure Monconduit, William I. F. David, Christopher I Thomas, Patrik Johansson, Serena A. Cussen, Grant S. Stone, Jincheng Tong, Russell E. Morris, Clare P. Grey, Alexandre Ponrouch, Oleg Kolosov, Emmanuel I. Eweka, Darren M. C. Ould, Robert G. Palgrave, Thomas J. Wood, Yue Chen, Jerry Barker, Ronnie Mogensen, Stijn F. L. Mertens, Philippe Poizot, Juan Forero-Saboya, David O. Scanlon, Manish Chhowalla, Lorenzo Stievano, Emily M. Reynolds, Xiao Hua, Moulay Tahar Sougrati, William R. Brant, Martin Karlsmo, Stéven Renault, Christopher A. O’Keefe, Begoña Silván, Lancaster University, Harwell Science and Innovation Campus, Imperial College London, University of Sheffield [Sheffield], Faradion Limited, University of Virginia [Charlottesville], University of Oxford [Oxford], University of Cambridge [UK] (CAM), University College of London [London] (UCL), University of St Andrews [Scotland], AUTRES, Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Chalmers University of Technology [Gothenburg, Sweden], Science and Technology Facilities Council (STFC), University of Birmingham [Birmingham], Uppsala University, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-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 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)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), Alistore, European Commission, Swedish Research Council, Swedish Energy Agency, Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning, Ministerio de Economía, Industria y Competitividad (España), Faraday Institution, Austrian Science Fund, Innovate UK, Tapia-Ruiz, Nuria [0000-0002-5005-7043], Armstrong, A Robert [0000-0003-1937-0936], Alptekin, Hande [0000-0001-6065-0513], Au, Heather [0000-0002-1652-2204], Barker, Jerry [0000-0002-8791-1119], Brant, William R [0000-0002-8658-8938], Choi, Yong-Seok [0000-0002-3737-2989], Costa, Sara I R [0000-0001-8105-207X], Crespo Ribadeneyra, Maria [0000-0001-6455-4430], Cussen, Serena A [0000-0002-9303-4220], Desai, Aamod V [0000-0001-7219-3428], Forero-Saboya, Juan D [0000-0002-3403-6066], Griffin, John M [0000-0002-8943-3835], Irvine, John T S [0000-0002-8394-3359], Johansson, Patrik [0000-0002-9907-117X], Karlsmo, Martin [0000-0002-0437-6860], Kendrick, Emma [0000-0002-4219-964X], Kolosov, Oleg V [0000-0003-3278-9643], Mertens, Stijn F L [0000-0002-5715-0486], Monconduit, Laure [0000-0003-3698-856X], Naylor, Andrew J [0000-0001-5641-7778], Poizot, Philippe [0000-0003-1865-4902], Renault, Stéven [0000-0002-6500-0015], Rudola, Ashish [0000-0001-9368-0698], Sayers, Ruth [0000-0003-1289-0998], Seymour, Valerie R [0000-0003-3333-5512], Silván, Begoña [0000-0002-1273-3098], Sougrati, Moulay Tahar [0000-0003-3740-2807], Stievano, Lorenzo [0000-0001-8548-0231], Thomas, Chris I [0000-0001-8090-4541], Titirici, Maria-Magdalena [0000-0003-0773-2100], Tong, Jincheng [0000-0001-7762-1460], Wood, Thomas J [0000-0002-5893-5664], Younesi, Reza [0000-0003-2538-8104], Apollo - University of Cambridge Repository, Kim, Eunjeong [0000-0002-2941-068], Kim, Eunjeong [0000-0002-2941-0682], University of Virginia, University of Oxford, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), 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), 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), Tapia-Ruiz, N [0000-0002-5005-7043], Armstrong, AR [0000-0003-1937-0936], Alptekin, H [0000-0001-6065-0513], Au, H [0000-0002-1652-2204], Barker, J [0000-0002-8791-1119], Brant, WR [0000-0002-8658-8938], Choi, YS [0000-0002-3737-2989], Costa, SIR [0000-0001-8105-207X], Ribadeneyra, MC [0000-0001-6455-4430], Cussen, SA [0000-0002-9303-4220], Desai, AV [0000-0001-7219-3428], Forero-Saboya, JD [0000-0002-3403-6066], Griffin, JM [0000-0002-8943-3835], Irvine, JTS [0000-0002-8394-3359], Johansson, P [0000-0002-9907-117X], Karlsmo, M [0000-0002-0437-6860], Kendrick, E [0000-0002-4219-964X], Kolosov, OV [0000-0003-3278-9643], Mertens, SFL [0000-0002-5715-0486], Monconduit, L [0000-0003-3698-856X], Naylor, AJ [0000-0001-5641-7778], Poizot, P [0000-0003-1865-4902], Renault, S [0000-0002-6500-0015], Rudola, A [0000-0001-9368-0698], Sayers, R [0000-0003-1289-0998], Seymour, VR [0000-0003-3333-5512], Silván, B [0000-0002-1273-3098], Sougrati, MT [0000-0003-3740-2807], Stievano, L [0000-0001-8548-0231], Thomas, CI [0000-0001-8090-4541], Titirici, MM [0000-0003-0773-2100], Tong, J [0000-0001-7762-1460], Wood, TJ [0000-0002-5893-5664], Younesi, R [0000-0003-2538-8104], The Faraday Institution, University of St Andrews. School of Chemistry, University of St Andrews. Centre for Energy Ethics, University of St Andrews. Centre for Designer Quantum Materials, and University of St Andrews. EaSTCHEM

Subjects
Chemical process, Technology, Computer science, PAIR DISTRIBUTION FUNCTION, HIGH-ENERGY DENSITY, ELECTROCHEMICAL PROPERTIES, Materialkemi, 02 engineering and technology, 01 natural sciences, 7. Clean energy, Materials Chemistry, QD, LITHIUM-ION, Energy demand, Scope (project management), anodes, NA2TI3O7 NANOSHEETS, [CHIM.MATE]Chemical Sciences/Material chemistry, sodium ion, 021001 nanoscience & nanotechnology, Variety (cybernetics), General Energy, Roadmap, T-DAS, Lithium, 0210 nano-technology, Battery (electricity), energy materials, Energy & Fuels, HIGH-CAPACITY ANODE, batteries, Materials Science (miscellaneous), Materials Science, chemistry.chemical_element, Materials Science, Multidisciplinary, electrolytes, 010402 general chemistry, Energy storage, MECHANISTIC INSIGHTS, SDG 7 - Affordable and Clean Energy, STRUCTURAL EVOLUTION, SOLID-ELECTROLYTE INTERPHASE, Science & Technology, QD Chemistry, 0104 chemical sciences, chemistry, 13. Climate action, Sustainability, HIGH-PERFORMANCE CATHODE, Biochemical engineering, cathodes
Abstract

Tapia-Ruiz, Nuria et al., Increasing concerns regarding the sustainability of lithium sources, due to their limited availability and consequent expected price increase, have raised awareness of the importance of developing alternative energy-storage candidates that can sustain the ever-growing energy demand. Furthermore, limitations on the availability of the transition metals used in the manufacturing of cathode materials, together with questionable mining practices, are driving development towards more sustainable elements. Given the uniformly high abundance and cost-effectiveness of sodium, as well as its very suitable redox potential (close to that of lithium), sodium-ion battery technology offers tremendous potential to be a counterpart to lithium-ion batteries (LIBs) in different application scenarios, such as stationary energy storage and low-cost vehicles. This potential is reflected by the major investments that are being made by industry in a wide variety of markets and in diverse material combinations. Despite the associated advantages of being a drop-in replacement for LIBs, there are remarkable differences in the physicochemical properties between sodium and lithium that give rise to different behaviours, for example, different coordination preferences in compounds, desolvation energies, or solubility of the solid–electrolyte interphase inorganic salt components. This demands a more detailed study of the underlying physical and chemical processes occurring in sodium-ion batteries and allows great scope for groundbreaking advances in the field, from lab-scale to scale-up. This roadmap provides an extensive review by experts in academia and industry of the current state of the art in 2021 and the different research directions and strategies currently underway to improve the performance of sodium-ion batteries. The aim is to provide an opinion with respect to the current challenges and opportunities, from the fundamental properties to the practical applications of this technology., The authors gratefully acknowledge RS2E and Alistore-ERI for funding their research into Na-ion batteries. The funding received from the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 646433 (NAIADES), the Swedish Research Council, the Swedish Energy Agency (#37671-1), and the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning (FORMAS), are all gratefully acknowledged. The many fruitful discussions within ALISTORE-ERI, and especially with M Rosa Palacín, have been most valuable. P J is also grateful for the continuous support from several of the Chalmers Areas of Advance: Materials Science and Energy. Funding from the European Union’s innovation program H2020 is acknowledged: H2020-MSCA-COFUND-2016 (DOC-FAM, Grant Agreement No. 754397). A Ponrouch is grateful to the Spanish Ministry for Economy, Industry and Competitiveness Severo Ochoa Programme for Centres of Excellence in R&D (SEV-2015-0496).

Published
2021

6. On the dynamics of transition metal migration and its impact on the performance of layered oxides for sodium-ion batteries: NaFeO2as a case study

Author

Begoña Silván, Elena Gonzalo, Neeraj Sharma, Damien Saurel, François Fauth, and Lisa Djuandhi

Subjects
Diffraction, Materials science, Renewable Energy, Sustainability and the Environment, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Thermal diffusivity, Electrochemistry, 7. Clean energy, 01 natural sciences, Cathode, 0104 chemical sciences, Dielectric spectroscopy, law.invention, Transition metal, Chemical physics, law, Structural stability, General Materials Science, Titration, 0210 nano-technology
Abstract

Transition metal (TM) layered oxides constitute one of the most promising families of compounds for the cathode of Na-ion batteries. However, their structural stability at the charged state is a critical performance limiting factor, which is believed to be closely related to irreversible TM migration into the Na layers. Nevertheless, experimental evidence of this TM migration and its influence on the electrochemical performance is still scarce, while the understanding of such a phenomenon constitutes a key step for developing better performing TM layered oxides. Here NaFeO2 has been studied as a model system, since it is expected to produce one of the most pronounced TM migrations and provide possibly one of the highest theoretical energy densities of TM layered oxides. By combining the Potential Intermittent Titration Technique (PITT), Electrochemical Impedance Spectroscopy (EIS) and operando X-ray diffraction, it has been possible to analyze the structural evolution of NaxFeO2, track the iron migration and observe its influence on the insertion capacity and Na diffusivity.

Published
2018

7. Mechanistic Insight into the High Voltage Stability of Fe-Rich Transition Metal Layered Oxides As the Positive Electrode of Na-Ion Batteries

Author

Javier Carrasco, Jian Xiang Lian, Begoña Silván, Damien Saurel, and Elena Gonzalo

Subjects
Materials science, Transition metal, Chemical engineering, Electrode, High voltage
Abstract

Transition metal layered oxides (TMLOs) of general formula LiTMO2 are the cornerstone of the present Li-ion technology as these cathode active materials allow the highest energy density thanks to the large capacity they offer. This is due to the high concentration of alkali metal their structure includes in the form of Li layers between TMO2 metal oxide layers, with Van der Walls bounds between the two type of layers. However, this structural particularity also consists in their main drawback: a full charge would require removal of 1/4 of the atoms of the structure, which consists in ½ of its structural layers. The layered structure cannot sustain such heavy change and tends to irreversibly transform into a more 3D structure, such as spinel or rock-salt. As a consequence, only 50 to 70% of the theoretical capacity is effectively used to ensure reversible electrochemical response with good cycle life. Na-TMLOs share the same advantages that Li-TMLOs, as the best compounds present the highest capacities of all known Na-ion cathodes, but also the same drawbacks as the structural instability under deep deintercalation is even more pronounced than in the case of Li. However, Na-TMLOs have an additional cost-related advantage. Stable compounds can be rich in abundant elements such as Fe, Mn and Ni, without the requirement of incorporating critical metals such as Co. Fe is especially interesting because it allows a fairly high working potential while being from far the most abundant. However, Fe-rich Na-TMLOs show the least structural stability under Na extraction due to the occurrence of TM migration to the Na-layers which is believed to be irreversible and thus responsible for the fast degradation of the electrochemical response of these compounds.[1] The mechanism of Fe migration is thus the focus of the intense research activity so as to understand its features as well as its correlation with the degradation of the electrochemical performance, see e.g. refs. [1-4]. New mechanistic insights on the high voltage structural evolution of Fe-rich Na-TMLOs will be presented based on the combination of various operando techniques, coupled PITT and impedance spectroscopy, and with the support of DFT calculations. The mechanism of Fe migration will be described in detail as well as its correlation with the electrochemical response. It will be showed how surprisingly reversible is the Fe migration phenomenon in certain compounds, as shown in Figure 1,[4] and that the degradation of the electrochemical performance actually occurs when oxygen redox is involved,[5] the two phenomena being closely intercorrelated. How the dilution of Fe and the nature of the initial structure, P2 or O3, influences the dynamics and reversibility of Fe migration will also be shown. Finally, it will be highlighted how the high voltage evolution of Fe-rich TMLOs can easily go unnoticed using operando synchrotron X-ray diffraction depending on the design of the electrochemical cell. References: [1] X. Li et al, Chem. Mater., 28, 6575 (2016). [2] D. Susanto et al., Chem. Mater. 31, 3644 (2019). [3] Y. Li et al., Nano Energy 47, 519 (2018). [4] B. Silván et al., J. Mater. Chem. A 6, 15132 (2018). [5] B. Silván et al, in preparation. Figure 1

Published
2020

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