Changzheng Wu

Metallic Few-Layered VS2 Ultrathin Nanosheets: High Two-Dimensional Conductivity for In-Plane Supercapacitors

With the rapid development of portable electronics, such as e-paper and other flexible devices, practical power sources with ultrathin geometries become an important prerequisite, in which supercapacitors with in-plane configurations are recently emerging as a favorable and competitive candidate. As is known, electrode materials with two-dimensional (2D) permeable channels, high-conductivity structural scaffolds, and high specific surface areas are the indispensible requirements for the development of in-plane supercapacitors with superior performance, while it is difficult for the presently available inorganic materials to make the best in all aspects. In this sense, vanadium disulfide (VS(2)) presents an ideal material platform due to its synergic properties of metallic nature and exfoliative characteristic brought by the conducting S-V-S layers stacked up by weak van der Waals interlayer interactions, offering great potential as high-performance in-plane supercapacitor electrodes. Herein, we developed a unique ammonia-assisted strategy to exfoliate bulk VS(2) flakes into ultrathin VS(2) nanosheets stacked with less than five S-V-S single layers, representing a brand new two-dimensional material having metallic behavior aside from graphene. Moreover, highly conductive VS(2) thin films were successfully assembled for constructing the electrodes of in-plane supercapacitors. As is expected, a specific capacitance of 4760 μF/cm(2) was realized here in a 150 nm in-plane configuration, of which no obvious degradation was observed even after 1000 charge/discharge cycles, offering as a new in-plane supercapacitor with high performance based on quasi-two-dimensional materials.

Ultrathin Two-Dimensional MnO2/Graphene Hybrid Nanostructures for High-Performance, Flexible Planar Supercapacitors

Planar supercapacitors have recently attracted much attention owing to their unique and advantageous design for 2D nanomaterials based energy storage devices. However, improving the electrochemical performance of planar supercapacitors still remains a great challenge. Here we report for the first time a novel, high-performance in-plane supercapacitor based on hybrid nanostructures of quasi-2D ultrathin MnO2/graphene nanosheets. Specifically, the planar structures based on the δ-MnO2 nanosheets integrated on graphene sheets not only introduce more electrochemically active surfaces for absorption/desorption of electrolyte ions, but also bring additional interfaces at the hybridized interlayer areas to facilitate charge transport during charging/discharging processes. The unique structural design for planar supercapacitors enables great performance enhancements compared to graphene-only devices, exhibiting high specific capacitances of 267 F/g at current density of 0.2 A/g and 208 F/g at 10 A/g and excellent rate capability and cycling stability with capacitance retention of 92% after 7000 charge/discharge cycles. Moreover, the high planar malleability of planar supercapacitors makes possible superior flexibility and robust cyclability, yielding capacitance retention over 90% after 1000 times of folding/unfolding. Ultrathin 2D nanomaterials represent a promising material platform to realize highly flexible planar energy storage devices as the power back-ups for stretchable/flexible electronic devices.

Two dimensional nanomaterials for flexible supercapacitors

Flexible supercapacitors, as one of most promising emerging energy storage devices, are of great interest owing to their high power density with great mechanical compliance, making them very suitable as power back-ups for future stretchable electronics. Two-dimensional (2D) nanomaterials, including the quasi-2D graphene and inorganic graphene-like materials (IGMs), have been greatly explored to providing huge potential for the development of flexible supercapacitors with higher electrochemical performance. This review article is devoted to recent progresses in engineering 2D nanomaterials for flexible supercapacitors, which survey the evolution of electrode materials, recent developments in 2D nanomaterials and their hybrid nanostructures with regulated electrical properties, and the new planar configurations of flexible supercapacitors. Furthermore, a brief discussion on future directions, challenges and opportunities in this fascinating area is also provided.

Metallic Nickel Nitride Nanosheets Realizing Enhanced Electrochemical Water Oxidation

Exploring efficient and inexpensive oxygen evolution reaction (OER) electrocatalysts is of great importance for various electrochemical energy storage and conversion technologies. Ni-based electrocatalysts have been actively pursued because of their promising activity and earth abundance. However, the OER efficiency for most of the developed Ni-based electrocatalysts has been intrinsically limited due to their low electrical conductivity and poor active site exposure yield. Herein, we report metallic Ni3N nanosheets as an efficient OER electrocatalyst for the first time. The first-principles calculations and electrical transport property measurements unravel that the Ni3N is intrinsically metallic, and the carrier concentration can be remarkably improved with dimensional confinement. The EXAFS spectra provide solid evidence that the Ni3N nanosheets have disordered structure resultant of dimensional reduction, which then could provide more active sites for OER. Benefiting from enhanced electrical conductivity with metallic behavior and atomically disordered structure, the Ni3N nanosheets realize intrinsically improved OER activity compared with bulk Ni3N and NiO nanosheets. Our finding suggests that metallic nitride nanosheets could serve as a new group of OER electrocatalysts with excellent property.

Fabrication of flexible and freestanding zinc chalcogenide single layers

Inorganic graphene analogues (IGAs) are a conceptually new class of materials with attractive applications in next-generation flexible and transparent nanodevices. However, their species are only limited to layered compounds, and the difficulty in extension to non-layered compounds hampers their widespread applicability. Here we report the fabrication of large-area freestanding single layers of non-layered ZnSe with four-atomic thickness, using a strategy involving a lamellar hybrid intermediate. Their surface distortion, revealed by means of synchrotron radiation X-ray absorption fine structure spectroscopy, is shown to give rise to a unique electronic structure and an excellent structural stability, thus determining an enhanced solar water splitting efficiency and photostability. The ZnSe single layers exhibit a photocurrent density of 2.14 mA cm(-2) at 0.72 V versus Ag/AgCl under 300 W Xe lamp irradiation, 195 times higher than that of bulk counterpart. This work opens the door for extending atomically thick IGAs to non-layered compounds and holds promise for a wealth of innovative applications.

Metallic Co4N Porous Nanowire Arrays Activated by Surface Oxidation as Electrocatalysts for the Oxygen Evolution Reaction

Designing highly efficient electrocatalysts for oxygen evolution reaction (OER) plays a key role in the development of various renewable energy storage and conversion devices. In this work, we developed metallic Co4N porous nanowire arrays directly grown on flexible substrates as highly active OER electrocatalysts for the first time. Benefiting from the collaborative advantages of metallic character, 1D porous nanowire arrays, and unique 3D electrode configuration, surface oxidation activated Co4N porous nanowire arrays/carbon cloth achieved an extremely small overpotential of 257 mV at a current density of 10 mA cm(-2), and a low Tafel slope of 44 mV dec(-1) in an alkaline medium, which is the best OER performance among reported Co-based electrocatalysts to date. Moreover, in-depth mechanistic investigations demonstrate the active phases are the metallic Co4N core inside with a thin cobalt oxides/hydroxides shell during the OER process. Our finding introduces a new concept to explore the design of high-efficiency OER electrocatalysts.

Giant Moisture Responsiveness of VS2 Ultrathin Nanosheets for Novel Touchless Positioning Interface

Utilizing a thin film of VS(2) ultrathin nanosheets with giant and fast moisture responsiveness, a brand-new model of moisture-based positioning interface is put forward here, by which not only the 2D position information of finger tips can be acquired, but also the relative height can be detected as the third dimensionality, representing a promising platform for advanced man-machine interactive systems.

Two-dimensional vanadyl phosphate ultrathin nanosheets for high energy density and flexible pseudocapacitors

Two-dimensional materials have been an ideal material platform for constructing flexible ultrathin-film supercapacitors, offering great advantages of flexibility, ultra-thinness and even transparency. Exploring new two-dimensional pseudocapacitive materials with high electrochemical activity is needed to achieve flexible ultrathin-film supercapacitors with higher energy densities. Here we report an inorganic graphene analogue, α1-vanadyl phosphate ultrathin nanosheets with less than six atomic layers, as a promising material to construct a flexible ultrathin-film pseudocapacitor in all-solid-state. The material exhibits a high potential plateau of ~ 1.0 V in aqueous solutions, approaching the electrochemical potential window of water (1.23 V). The as-established flexible supercapacitor achieves a high redox potential (1.0 V) and a high areal capacitance of 8,360.5 μF cm(-2), leading to a high energy density of 1.7 mWh cm(-2) and a power density of 5.2 mW cm(-2).

Single-Atom Pt as Co-Catalyst for Enhanced Photocatalytic H2 Evolution

Isolated single-atom platinum (Pt) embedded in the sub-nanoporosity of 2D g-C3 N4 as a new form of co-catalyst is reported. The highly stable single-atom co-catalyst maximizes the atom efficiency and alters the surface trap states of g-C3 N4 , leading to significantly enhanced photocatalytic H2 evolution activity, 8.6 times higher than that of Pt nanoparticles and up to 50 times that for bare g-C3 N4 .

Atomically Thick Bismuth Selenide Freestanding Single Layers Achieving Enhanced Thermoelectric Energy Harvesting

Thermoelectric materials can realize significant energy savings by generating electricity from untapped waste heat. However, the coupling of the thermoelectric parameters unfortunately limits their efficiency and practical applications. Here, a single-layer-based (SLB) composite fabricated from atomically thick single layers was proposed to optimize the thermoelectric parameters fully. Freestanding five-atom-thick Bi(2)Se(3) single layers were first synthesized via a scalable interaction/exfoliation strategy. As revealed by X-ray absorption fine structure spectroscopy and first-principles calculations, surface distortion gives them excellent structural stability and a much increased density of states, resulting in a 2-fold higher electrical conductivity relative to the bulk material. Also, the surface disorder and numerous interfaces in the Bi(2)Se(3) SLB composite allow for effective phonon scattering and decreased thermal conductivity, while the 2D electron gas and energy filtering effect increase the Seebeck coefficient, resulting in an 8-fold higher figure of merit (ZT) relative to the bulk material. This work develops a facile strategy for synthesizing atomically thick single layers and demonstrates their superior ability to optimize the thermoelectric energy harvesting.