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Highlights Ultrathin and defect-free graphene ink is prepared through a high-throughput fluid dynamics process, resulting in a high exfoliation yield (53.5%) and a high concentration (47.5 mg mL−1). A screen-printed graphene conductor exhibits a high electrical conductivity of 1.49 × 104 S m−1 and good mechanical flexibility. An electrochemical sodium ion sensor based on graphene ink exhibits an excellent potentiometric sensing performance in a mechanically bent state. Real-time monitoring of sodium ion concentration in sweat is demonstrated. Abstract Conductive inks based on graphene materials have received significant attention for the fabrication of a wide range of printed and flexible devices. However, the application of graphene fillers is limited by their restricted mass production and the low concentration of their suspensions. In this study, a highly concentrated and conductive ink based on defect-free graphene was developed by a scalable fluid dynamics process. A high shear exfoliation and mixing process enabled the production of graphene at a high concentration of 47.5 mg mL−1 for graphene ink. The screen-printed graphene conductor exhibits a high electrical conductivity of 1.49 × 104 S m−1 and maintains high conductivity under mechanical bending, compressing, and fatigue tests. Based on the as-prepared graphene ink, a printed electrochemical sodium ion (Na+) sensor that shows high potentiometric sensing performance was fabricated. Further, by integrating a wireless electronic module, a prototype Na+-sensing watch is demonstrated for the real-time monitoring of the sodium ion concentration in human sweat during the indoor exercise of a volunteer. The scalable and efficient procedure for the preparation of graphene ink presented in this work is very promising for the low-cost, reproducible, and large-scale printing of flexible and wearable electronic devices.

Two-dimensional molybdenum disulfide (MoS2) nanosheets have attracted great attention for electrochemical storage and conversion, but the scalable preparation of highly conductive and stable MoS2 n...

Flexible, thin, and lightweight supercapacitors have been regarded as important power sources for portable and wearable electronics; however, these are usually limited by relatively low areal or vo...

In this study, ultrathin and defect-free graphene (Gr) sheets were prepared through a fluid dynamics–induced shear exfoliation method using graphite. The high hydrophobicity and surface area of Gr make it attractive as a solid-contact ion-to-electron transducer for potentiometric K+ sensors, in which the electrodes are fabricated through a screen-printing process. The electrochemical characterization demonstrates that Gr solid contact results in a high double-layer capacitance, potential stability, and strong resistance against water layer, gases, and light. The Gr-based K+ sensors showed a Nernstian slope of 53.53 mV/log[K+] within a linear concentration range of 10−1–10−4 M, a low detection limit of 10−4.28 M, a fast response time of ~8 s, good repeatability, and excellent long-term stability. Moreover, the Gr-based K+ sensors provided accurate ion concentrations in actual samples of human sweat and sports drinks.

We report potentiometric performances of ion-to-electron transducer based on reduced graphene oxide (RGO) for application of all-solid-state potassium ion sensors. A large surface area and pore structure of RGO are obtained by a hydrothermal self-assembly of graphene oxide. The extensive electrochemical characterization of RGO solid contact at the interface of ion-selective membrane and gold electrode shows that the potassium ion-selective electrode based on RGO had a high sensitivity (53.34 mV/log[K+]), a low detection of limit (− 4.24 log[K+], 0.06 mM) a good potential stability, and a high resistance to light and gas interferences. The potentiometric K+-sensor device was fabricated by combining of screen-printed electrodes and a printed circuit board. The K+-sensor device accurately measures the ion concentration of real samples of commercial sports drinks, coke and orange juice, and then transfers the collected data to a mobile application through a Bluetooth module. The screen-printed ion sensors based on RGO solid contact show a great potential for real-time monitoring and point-of-care devices in human health care, water-treatment process, and environmental and chemical industries.

The noninvasive early detection of biomarkers for Alzheimer’s disease (AD) is essential for the development of specific treatment strategies. This paper proposes an advanced method for fabricating highly ordered and flexible nanopillar-based electrochemical biosensors by the combination of soft/photolithography and metal evaporation. The nanopillar array (NPA) exhibits high surface area containing 1500 nm height and 500 nm diameter with 3:1 ratio. In regard with physical properties of polyurethane (PU) substrate, the developed NPA is sustainable and durable to external pressure such as bending and twisting. To manipulate the NPA surface to biocompatible, the gold was uniformly deposited on the PU substrate. The thiol chemistry which is stably modified on the gold surface as a form of self-assembled monolayer was employed for fabricating the NPA as a biocompatible chip by covalently immobilize the antibodies. The proposed nanopillar-based immunoelectrochemical biosensor exhibited good and stable electrochemical performance in β-amyloid (Aβ) detection. Moreover, we successfully confirmed the performance of the as-developed sensor using the artificial injection of Aβ in human tear, with sensitivity of 0.14 ng/mL and high reproducibility (as a standard deviation below 10%). Our findings show that the developed nanopillar-based sensor exhibits reliable electrochemical characteristics and prove its potential for application as a biosensor platform for testing at the point of care.

Current collectors and substrate materials are of pivotal importance for the design and preparation of electrodes and energy storage devices, because their surface areas, morphologies, ionic and electronic conductivities, and mechanical properties substantially influence electrochemical performances. Although carbon cloths (CCs) are widely considered the most promising current collectors for flexible energy storage devices, the majority of carbon-based textiles have poor capacitances due to their low surface areas and porosities, which reduce device performances. Here, we report a rapid and straightforward method for preparing CC-based electrode materials for high performance supercapacitors using microwaves. Microwave irradiation efficiently activates the surface pores of carbon fibers, and increases specific capacitance markedly as compared with pristine CC. In addition, surfaces of microwave-treated CCs (m-CCs) are coated with reduced graphene oxide (RGO) or MnO2, and the resulting electrode materials exhibit excellent electrochemical performances, such as, high specific capacitances, high rate capabilities, and long-term cycling stabilities. Flexible solid-state supercapacitor devices are fabricated using a RGO/m-CC as a negative electrode and a MnO2/m-CC as a positive electrode. The produced asymmetric supercapacitors show an excellent resilience to harsh electrochemical and mechanical conditions, and high energy and power densities.

Hierarchical 3D nanostructures based on waste biomass are being offered as promising materials for energy storage due to their processabilities, multifunctionalities, environmental benignities, and low cost. Here we report a facile, inexpensive, and scalable strategy for the fabrication of hierarchical porous 3D structure as electrode materials for supercapacitors based on MnO2 nanowires and hemp-derived activated carbon (HC). Vertical MnO2 wires are uniformly deposited onto the surface of HC using a one-step hydrothermal method to produce hierarchical porous structures with conductive interconnected 3D networks. HC acts as a near-ideal 3D current collector and anchors electroactive materials, and this confers a specific capacitance of 340 F g–1 at 1 A g–1 with a high rate capability (88% retention) of the 3D MnO2/HC composite because of its open-pore system, which facilitates ion and electron transports and synergistic contribution of two energy-storage materials. Moreover, asymmetric supercapacitors fab...

The integration of organic and inorganic building blocks into hierarchical porous architectures makes potentially desirable electrocatalytic materials in many electrochemical applications due to their combination of attractive qualities of dissimilar components and well-constructed charge transfer pathways. Herein, we demonstrate the preparation of the hierarchical porous Co3O4@graphene (Co3O4@G) microspheres by one-step hydrothermal method to achieve high electrocatalytic performance for enzyme-free biosensor applications. The obtained Co3O4@G microspheres are consisted of the interconnected networks of Co3O4 and graphene sheets, and thus provide large accessible active sites through porous structure, while graphene sheets offer continuous electron pathways for efficient electrocatalytic reaction of Co3O4. These structural merits with synergy effect of Co3O4 and graphene lead to a high performance of enzyme-free detection for glucose: high sensitivity, good selectivity, and remarkable stability.

Straightforward and scalable fabrications of energy storage electrode materials with high electrochemical performance are of great interest for applications in batteries and supercapacitors. Herein, we report a one-step process for producing high-performance NiO/reduced graphene oxide (RGO) nanocomposites using a ball mill based method, which is simple, environmentally friendly, and cost-effective. Graphite oxide (GO) and nickel power were pulverized in a ball mill, to produce NiO/RGO nanocomposites. GO played an important role in promoting a redox reaction between GO and metallic nickel, which produced a strong bond between the as-formed Ni oxide and RGO. The electrochemical performances of NiO/RGO were investigated by cyclic voltammetry (CV), galvanostatic charge/discharge measurement, and impedance spectroscopy. The NiO/RGO electrodes exhibited high specific capacitance (590 F g− 1 at 1 A g− 1), a high rate capability (88% retention at a high rate of 15 A g− 1), and an excellent cycling stability (100% retention after 1000 charge/discharge cycles).

Development of sensing technology with wearable chemical sensors is realizing non-invasive, real-time monitoring healthcare and disease diagnostics. The advanced sensor devices should be compact and portable for use in limited space, easy to wear on human body, and low-cost for personalized healthcare markets. Here, we report a highly sensitive, flexible, and autonomously self-healable pH sensor cable developed by weaving together two carbon fiber thread electrodes coated with mechanically robust self-healing polymers. The pH sensor cable showed excellent electrochemical performances of sensitivity, repeatability, and durability. Spontaneous and autonomous sensor healing efficiency of the pH sensor cable was demonstrated by measuring sensitivity during four cycles of cutting and healing process. The pH sensor cable could measure pH in small volumes of real human fluid samples, including urine, saliva, and sweat, and the results were similar to those of a commercial pH meter. Taken together, successful real-time pH monitoring for human sweat was demonstrated by fabricating a wearable sensing system in which the pH sensor cable was knitted into a headband integrated with wireless electronics.

Herein, we report a rapid and simultaneous synthesis of manganese oxide (MnO2) nanoparticles deposited on porous graphene foam by microwave-assisted method. The microwave irradiation enables simultaneously reduction and porous structure of graphene oxide and deposition of MnO2. As-synthesized MnO2/graphene nanocomposites are characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The resultant MnO2/graphene nanocomposite electrodes exhibit as high as specific capacitance of 372 F g− 1 at 0.5 A g− 1, high rate capability (82% retention at 5 A g− 1), and good long-term stability (98.5% retention during 3000 cycles). This synthetic method could be applicable to the mass production of porous nanocomposites as energy storage materials for supercapacitors and lithium-ion batteries.

A hierarchical porous structure of MnO2 nanosheet arrays is synthesized on three-dimensional surface of carbon fiber paper (CFP). As-synthesized MnO2/CFP is thoroughly characterized by transmission electron microscopy, scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The direct deposition of MnO2 enables a good electrical connection to the CFP, and thus eliminates the need for polymeric binders and carbon additives. Moreover, the unique structure with a large surface area enables efficient and rapid ion and electron transfer in electrochemical processes. When testing as an electrode for supercapacitors, the MnO2/CFP shows a specific capacitance (204 F/g), rate capability (75% retention), and good cycling life (~ 100% retention after 1000 cycles).

Flower-shaped Ni3S2/Ni structures were synthesized on the surface of three-dimensional (3D) carbon fiber webs (CFWs) using electroless plating of Ni and subsequent sulfuration. The as-obtained product of this treatment was characterized using various techniques including scanning electron microscopy and X-ray diffraction, and was confirmed to indeed be Ni3S2/Ni-coated CFWs. Moreover, these webs were observed to have a unique architecture, consisting of a hierarchical porous structure with the flower-shaped morphology. This structure apparently enabled efficient ion diffusion and rapid electron transfer through the 3D CFW supports, as the Ni3S2/Ni-coated CFWs showed excellent electrochemical performances: a high areal capacitance of 240 mF/cm2 at current density of 1 mA/cm2, a high rate capability of 85.4% retention at current density of 15 mA/cm2, and good long-term stability (98% over 2000 cycles).

Flexible and highly ordered nanopillar arrayed electrodes have brought great interest for many electrochemical applications, especially to the biosensors, because of its unique mechanical and topological properties. Herein, we report an advanced method to fabricate highly ordered nanopillar electrodes produced by soft-/photo-lithography and metal evaporation. The highly ordered nanopillar array exhibited the superior electrochemical and mechanical properties in regard with the wide space to response with electrolytes, enabling the sensitive analysis. As-prepared gold and silver electrodes on nanopillar arrays exhibit great and stable electrochemical performance to detect the amplified gene from foodborne pathogen of Escherichia coli O157:H7. Additionally, lightweight, flexible, and USB-connectable nanopillar-based electrochemical sensor platform improves the connectivity, portability, and sensitivity. Moreover, we successfully confirm the performance of genetic analysis using real food, specially designed intercalator, and amplified gene from foodborne pathogens with high reproducibility (6% standard deviation) and sensitivity (10 × 1.01 CFU) within 25 s based on the square wave voltammetry principle. This study confirmed excellent mechanical and chemical characteristics of nanopillar electrodes have a great and considerable electrochemical activity to apply as genetic biosensor platform in the fields of point-of-care testing (POCT).

Although exfoliated MoS2 sheets have recently demonstrated their great potential for use as electrodes for supercapacitors, they suffer from poor intrinsic electrical conductivity and strong tendency for intersheet aggregation. Here, we develop a synthetic method for preparation of N-doped carbon-coated MoS2 (NC-MoS2) nanosheets composed of coating of polydopamine and a post carbonization process. Construction of carbon layers on the MoS2 surface enables effective prevention of sheet aggregation and provide a rapid pathway for electron transfer. As-prepared NC-MoS2 materials are then characterized by electrochemical measurements to demonstrate the superior performance of the supercapacitor electrodes. The NC-MoS2 electrode exhibits improved electrochemical performance relative to the exfoliated MoS2 sheets, with a high specific capacitance (158 F g−1), high rate capability (83% retention), and good cycling life (89% retention) during 1000 cycles.

Two dimensional nanosheets, such as graphene and metal disulfides, have attracted a great deal of attention as anode materials for lithium-ion batteries, owing to their unique capability for lithium-ion storage. In this work, we integrate graphene and MoS 2 nanosheets into a free standing film form using a simple vacuum filtration method. As-prepared composite film could be readily employed as a binder- and carbon-free anode for lithium-ion batteries, removing the polymeric binders and conductive carbon additives that are required for the preparation of conventional electrodes. In addition, the interconnected structure of graphene and MoS 2 sheets provide a good electrical conductivity to the entire film electrode. When tested electrochemical performance as an anode for lithium-ion batteries, the composite film electrode exhibits superior performance compared to the exfoliated MoS 2 electrode, such as 65.8% capacity retention at a high current rate of 1000 mA g −1 and 91.1% capacity retention after 100 cycles.

Graphene and its derivatives have attracted much attention in application of electrochemical devices. Construction of three-dimensional (3D) heterostructured composites is promising for establishing high-performance devices, which enables large surface area, facilitated ion and electron transport, and synergistic effects between multicomponents. Here, we report a simple and general sonochemical-assisted synthesis to prepare various 3D porous graphene/nanoparticle (i.e., Pt, Au, Pd, Ru, and MnO2) foams using colloidal template. The 3D porous network structure of composite foams significantly improves a large surface area of around 550m(2)g(-1) compared to the bare graphene (215m(2)g(-1)). This unique structure of 3D graphene/MnO2 enables further improvement of electrochemical characteristics, compared with bare graphene/MnO2 composite, showing a high specific capacitance of 421Fg(-1) at 0.1Ag(-1), high rate capability (97% retention at 20Ag(-1)), and good cycling performance (97% retention over 1000 cycles). Moreover, electrochemical impedance analysis demonstrates that electron and ion transfer are triggered by 3D porous structure.

This study aimed to develop a more sensitive method for the detection of hepatitis B surface antigen (HBsAg) using heteroassembled gold nanoparticles (AuNPs). A single layered localized surface plasmon resonance (LSPR) chip format was developed with antigen-antibody reaction-based detection symmetry using AuNPs, which detected HBsAg at 10 pg/mL. To further improve the detection limit, a modified detection format was fabricated by fixing a secondary antibody (to form a heteroassembled sandwich format) to the AuNP monolayer, which enhanced the detection sensitivity by about 100 times. The developed heteroassembled AuNPs sandwich-immunoassay LSPR chip format was able to detect as little as 100 fg/mL of HBsAg within 10–15 min. In addition, the heteroassembled AuNPs sandwich-immunoassay LSPR chip format did not show any non-specific binding to other tested antigens, including alpha fetoprotein (AFP), C-reactive protein (CRP), and prostate-specific antigen (PSA). These findings confirm that the proposed detection strategy of heteroassembled AuNPs sandwich-immunoassay LSPR chip format may provide a new platform for early diagnosis of various human diseases.

Design and fabrication of electrodes is key in the development of electrochemical sensors with superior electrochemical performances. Herein, an enzymeless electrochemical sensor is developed for detection of hydrogen peroxide based on the use of highly ordered polyoxometalate (POM)-doped polyaniline (PANI) nanopillar films. The electrodeposition technique enables the entrapment of POMs into PANI during electropolymerization to produce thin coatings of POM-PANI. Electrochemical investigations of the POM-PANI/nanopillar electrode showed well-defined multiple pairs of redox peaks and rapid electron transfer. The nanopillar structure facilitated the diffusion of the electrolyte and thus, enhanced the redox reaction. In particular, the POM-PANI/nanopillar electrode was incorporated into a flow injection biosensor and it demonstrates its electrocatalytic activity to detect hydrogen peroxide with high sensitivity, rapid response time, and low detection limit.

In this report, we fabricate the porous graphene films through embossing process and vacuum filtration method and demonstrate their superior electrochemical properties as supercapacitor electrode materials. Insertion/ removal of polystyrene nanoparticles between the graphene sheets allows to provide pore structures, leading to the effec- tive prevention of restacking in graphene films. As-prepared porous graphene films have a large surface area, a bicontinuous porous structures, high electrical conductivity, and excellent mechanical integrity. The electrochemical properties of the porous graphene films as electrode materials of supercapacitor are investigated by using aqueous H2SO4 and ionic liq- uid solution under three-electrode system. The porous graphene films exhibit a high specific capacitance (284.5 F/g), which is two-fold higher than that of packing graphene films (138.9 F/g). In addition, the rate capability (98.7% reten- tion) and long-term cycling stability (97.2%) for the porous graphene films are significantly enhanced, due to the facili- tated ion mobility between the graphene layers.

The electrochemical performances of electrochemical biosensors largely depend on electrode characteristics, such as size, composition, surface area, and electron and ion conductivities. Herein, highly efficient electrocatalytic polyoxometalate (POM) was directly deposited on polymeric ionic liquid (PIL)-functionalized reduced graphene oxide (rGO) in a simple manner. The nano-sized POM with PIL functional groups was uniformly distributed on the surface of rGO sheets. The unique nanostructure of the resultant POM-g-rGO nanohybrids enabled well-defined multiple redox reaction of POMs and rapid electron transfer. In particular, as-prepared nanohybrids demonstrated high electrocatalytic activity for the electrochemical detection of H2O2 and glucose molecules in flow-injection biosensor device with high sensitivity, rapid response time, and low detection limit.

The effects of introducing gold (Au) nanoparticles (NP) on the electrochemical properties of graphene functionalized with ionic liquid were investigated by cyclic voltammetry, amperometry, and AC impedance analysis. The introduction of Au NPs onto graphene-ionic liquid sheets led to enhanced electron transfer rate, low charge transfer resistance, and large electrocatalytic area. An electrochemical biosensor device based on the hybrid of Au NPs and functionalized graphenes was fabricated and found to have superior electrochemical performance in the detection of glucose, with a sensitivity of 0.16 m Am M � 1 , a detection limit of 0.13 mM, and a response time of 5 s.

We report a simple and bio-friendly method to synthesize platinum (Pt) and nitrogen (N)-doped carbon@silica using polydopamine (PDA). This silica-based composite permits greater humidifying capacity to sufficiently hydrate membrane electrode assemblies (MEAs), thus improving electrochemical properties for polymer electrolyte membrane fuel cells (PEMFC).

We have demonstrated the fabrication of the biosensor platforms by means of the integration of the genetically engineered fusion proteins and the uniform gold nanoparticle-deposited multi-walled nanotube hybrid (Au-MWNT-HB) films for the detection of C-reactive protein (CRP). Au-MWNT-HB films were used as a good electrochemical transducer due to their excellent electrical properties and large surface areas for the signal transduction, while the genetically engineered fusion proteins, or 6His–GBP–SpA fusion proteins, specifically bind onto the surface of the Au-MWNT-HB films and efficiently immobilize bioreceptors for the detection of CRP. As-obtained biosensor platforms were characterized by electrochemical and optical analysis and revealed better performance compared to conventional Au-based biosensors. The concept delineated herein opens a new insight into nanobiotechnology through the integration of genetically engineered biomaterials with carbon nanotube (CNT)-based nanohybrids for emerging applications.

Nanohybrids of chemically modified graphene (CMG) and ionic liquid (IL) were prepared by sonication to modify the electrode. The modified CMG-IL electrodes showed a higher current and smaller peak-to-peak potential separation than a bare electrode due to the promoted electron transfer rate. Furthermore, the glucose oxidase (GOx) immobilized on the modified electrode displayed direct electron transfer rate and symmetrical redox potentials with a linear relationship at different scan rates. The fabricated GOx/CMG-IL electrodes were developed selective glucose biosensor with respect to a sensitivity of 0.64 μA mM−1, detection limit of 0.376 mM, and response time of

A versatile, facile, and rapid synthetic method of advanced carbon nanotube (CNT)-based nanohybrid fabrication, or the so-called ionic-liquid-assisted sonochemical method (ILASM), which combines the supramolecular chemistry between ionic liquids (ILs) and CNTs with sonochemistry for the control in the size and amount of uniformly decorated nanoparticles (NPs) and interfacial engineering, is reported. The excellence in electrocatalysis of hybrid materials with well-designed nanostructures and favorable interfaces is demonstrated by applying them to electrochemical catalysis. The synthetic method discussed in this report has an important and immediate impact not only on the design and synthesis of functional hybrid nanomaterials by supramolecular chemistry and sonochemistry but also on applications of the same into electrochemical devices such as sensors, fuel cells, solar cells, actuators, batteries, and capacitors.

Current collectors are essential features of batteries and many other electronic devices being responsible for efficient charge transport to active electrode materials. Three-dimensional (3D), high surface area current collectors considerably improve the performance of cathodes and anodes in batteries, but their technological implementation is impeded by the complexity of their preparation, which needs to be simple, fast, and energy efficient. Here we demonstrate that field-stimulated assembly of ∼3 nm copper nanoparticles (NPs) enables the preparation of porous Cu NP films. The use of NP dispersions enables 30× reduction of the deposition current for making functional 3D coatings. In addition to high surface area, lattice-to-lattice connectivity in the self-assembly of NPs in 3D structures enables fast charge transport. The mesoscale dimensions of out-of-plane features and the spacing between them in Cu films made by field-stimulated self-assembly of NPs provides promising morphology for current collection in lithium ion batteries (LIBs). Half-cell electrochemical models based on self-assembled films show improved specific capacity, total capacity, and cycling performance compared to traditional flat and other 3D current collectors. While integration of active electrode material into the 3D topography of the current collector needs to be improved, this study indicates that self-assembled NP films represent a viable manufacturing approach for 3D electrodes.

In this work, we report on a simple and scalable process to synthesize the core-shell nanostructure of MoS2@N-doped carbon nanosheets (MoS2@C), in which polydopamine is coated on the MoS2 surface and is then carbonized. An intensive investigation using transmission electron microscopy and Raman spectroscopy reveals that the as-synthesized MoS2@C possesses a nanoscopic and ultrathin layer of MoS2 sheets with a thin and conformal coating of carbon layers (∼ 3 nm). The MoS2@C demonstrates a superior electrochemical performances as an anode material for lithium ion batteries compared to exfoliated MoS2 and bulk MoS2 samples. This unique core-shell structure is capable of delivering an excellent Li(+) ion charging-discharging process as follows: a specific capacity as high as 1239 mA h g(-1), a high rate capability even at a high current rate of 10 A g(-1) while retaining 597 mA h g(-1), and a good cycle stability over 200 cycles at a high current rate of 2 A g(-1).

Development of nanostructured materials with enhanced redox reaction capabilities is important for achieving high energy and power densities in energy storage systems. Here, we demonstrate that the nanohybridization of ionic liquids (ILs, 1-butyl-3-methylimidazolium tetrafluoroborate) and cobalt hydroxide (Co(OH)2) through ionothermal synthesis leads to a rapid and reversible redox reaction. The as-synthesized IL-Co(OH)2 has a favorable, tailored morphology with a large surface area of 400.4 m(2)/g and a mesopore size of 4.8 nm. In particular, the IL-Co(OH)2-based electrode exhibits improvement in electrochemical characteristics compared with bare Co(OH)2, showing a high specific capacitance of 859 F/g at 1 A/g, high-rate capability (∼95% retention at 30 A/g), and excellent cycling performance (∼96% retention over 1000 cycles). AC impedance analysis demonstrates that the introduction of ILs on Co(OH)2 facilitates ion transport and charge transfer: IL-Co(OH)2 shows a higher ion diffusion coefficient (1.06 × 10(-11) cm(2)/s) and lower charge transfer resistance (1.53 Ω) than those of bare Co(OH)2 (2.55 × 10(-12) cm(2)/s and 2.59 Ω). Our density functional theory (DFT) calculations reveal that the IL molecules, consisting of anion and cation groups, enable easier hydrogen desorption/adsorption process, that is, a more favorable redox reaction on the Co(OH)2 surface.

In order to develop energy storage devices with high power and energy densities, electrodes should hold well-defined pathways for efficient ionic and electronic transport. Herein, we demonstrate high-performance supercapacitors by building a three-dimensional (3D) macroporous structure that consists of chemically modified graphene (CMG). These 3D macroporous electrodes, namely, embossed-CMG (e-CMG) films, were fabricated by using polystyrene colloidal particles as a sacrificial template. Furthermore, for further capacitance boost, a thin layer of MnO(2) was additionally deposited onto e-CMG. The porous graphene structure with a large surface area facilitates fast ionic transport within the electrode while preserving decent electronic conductivity and thus endows MnO(2)/e-CMG composite electrodes with excellent electrochemical properties such as a specific capacitance of 389 F/g at 1 A/g and 97.7% capacitance retention upon a current increase to 35 A/g. Moreover, when the MnO(2)/e-CMG composite electrode was asymmetrically assembled with an e-CMG electrode, the assembled full cell shows remarkable cell performance: energy density of 44 Wh/kg, power density of 25 kW/kg, and excellent cycle life.

A facilitated electrochemical reaction at the surface of electrodes is crucial for highly efficient energy conversion and storage. Herein, various nanoparticles (NPs) including Au, Pt, Pd, Ru, and RuO(2), were synthesized in situ and directly deposited on the ionic liquid (IL)-functionalized reduced graphene oxides (RGOs) in a controlled manner. The size, amount, and crystalline structures of discrete NPs were readily controlled, giving rise to enhanced methanol oxidation and pseudocapacitance. The well-defined nanostructure of decorated NPs and the favorable interaction between ILs and RGOs (or NPs) facilitated the electrochemical reaction, where NPs acted as electrocatalysts for energy conversion and played the role of redox-active electrodes for energy storage.

The chemistry and structure of ion channels within the polymer electrolytes are of prime importance for studying the transport properties of electrolytes as well as for developing high-performance electrochemical devices. Despite intensive efforts on the synthesis of polymer electrolytes, few studies have demonstrated enhanced target ion conduction while suppressing unfavorable ion or mass transport because the undesirable transport occurs through an identical pathway. Herein, we report an innovative, chemical strategy for the synthesis of polymer electrolytes whose ion-conducting channels are physically and chemically modulated by the ionic (not electronic) conductive, functionalized graphenes and for a fundamental understanding of ion and mass transport occurring in nanoscale ionic clusters. The functionalized graphenes controlled the state of water by means of nanoscale manipulation of the physical geometry and chemical functionality of ionic channels. Furthermore, the confinement of bound water within the reorganized nanochannels of composite membranes was confirmed by the enhanced proton conductivity at high temperature and the low activation energy for ionic conduction through a Grotthus-type mechanism. The selectively facilitated transport behavior of composite membranes such as high proton conductivity and low methanol crossover was attributed to the confined bound water, resulting in high-performance fuel cells.

Graphene sheets have the potential for practical applications in electrochemical devices, but their development has been impeded by critical problems with aggregation of graphene sheets. Here, we demonstrated a facile and bottom-up approach for fabrication of DNA sensor device using water-soluble sulfonated reduced graphene oxide (SRGO) sheets via microwave-assisted sulfonation (MAS), showing enhanced sensitivity, reliability, and low detection limit. Key to achieving these performances is the fabrication of the SRGOs, where the MAS method enabled SRGOs to be highly dispersed in water (10 mg mL(-1)) due to the acidic sulfonated groups generated within 3 min of the functionalization reaction. The water-soluble SRGO-DNA (SRGOD) hybrids prepared by electrostatic interactions between a flat single layer of graphene sheets and DNAs are suitable for fabrication of electrical DNA sensor devices because of the unique electrical characteristics of SRGODs. The high sensing performance of SRGOD sensors was demonstrated with detection of DNA hybridization using complementary DNAs, single base mismatched DNAs, and noncomplementary DNAs, with results showing higher sensitivity and lower detection limit than those of reduced graphene oxide-based DNA sensors. Simple and easy fabrication of DNA sensor devices using SRGODs is expected to provide an effective way for electrical detection of DNA hybridization using miniature sensors without the labor-intensive labeling of the sensor and complex measurement equipment.

In this research, ionic liquids are considered as multifunctional components by employing not only templates and co-solvents for fabricating nanostructured materials but also proton conductors for electrochemical devices. Two ionic liquid-aluminum hydroxide nanohybrids obtaining 1D and 3D shape were synthesized via a one-pot ionothermal process. The shape-controlled nanohybrids are expected to be a strong candidate for electrochemical device in terms of reasonable ionic conductivity and thermal stability as a result of the one-pot assembled nano-confinements.

A high surface area of electrodes along with rapid and efficient electron and ion transfer is essential for the development of high-performance electrochemical biosensors. Here, we present a simple and effective shadow evaporation method for the preparation of highly ordered gold (Au)-nanotube films for use as biosensor electrodes. This unique electrode structure results in a large surface area for enzyme immobilization, increased electrode electricity, and accelerated diffusion of electrolyte ions. When electrochemical reactions were tested, the Au-nanotube film electrode exhibits quasi-reversible and diffusion controlled behaviours. The flow-injection amperometric system for glucose biosensors is fabricated using the Au-nanotube films, and resulted in a fast response time of approximately 4 s, a sensitivity of 1.64 μA mM−1, a limit of detection of 0.07 mM, and a linear detection range of 2–20 mM. Moreover, the interference responses from oxidizable species such as ascorbic acid and uric acid are negligible at an operating potential of −0.1 V.

In this research, we report an innovative, chemical strategy for the in situ synthesis and direct two-dimensional (2D) arraying of various nanoparticles (NPs) on graphenes using both programmed-peptides as directing agents and graphenes as pre-formed 2D templates. The peptides were designed for manipulating the enthalpic (coupled interactions) constraint of the global system. Along with the functionalization of graphene for the stable dispersion, peptides directed the growth and array of NPs in a controllable manner. In particular, the sequences of peptides were encoded by the combination of glutamic acid (E), glycine (G), and phenylalanine (F) amino acids as follows: (E-G-F)(3)-G, with E for the interaction with NPs and F and G for the interaction with graphenes. For the entropic (restricted geometry) constraint, graphene was used as a 2D scaffold to tune the size, density, and position of NPs, while maintaining the intrinsic properties for electrochemical applications. The excellent quality of the resultant hybrids was demonstrated by their high electrocatalytic activity in the electrooxidation of methanol. This synergistic combination of peptides and graphenes allowed for a uniform 2D array and spontaneous organization of various NPs (i.e., Pt, Au, Pd, and Ru), which would greatly expand the utility and versatility of this approach for the synthesis and array of the advanced nanomaterials.