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      Multiscale structural and electronic control of molybdenum disulfide foam for highly efficient hydrogen production

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          Abstract

          Hydrogen production through water splitting has been considered as a green, pure and high-efficient technique. As an important half-reaction involved, hydrogen evolution reaction is a complex electrochemical process involving liquid-solid-gas three-phase interface behaviour. Therefore, new concepts and strategies of material design are needed to smooth each pivotal step. Here we report a multiscale structural and electronic control of molybdenum disulfide foam to synergistically promote the hydrogen evolution process. The optimized three-dimensional molybdenum disulfide foam with uniform mesopores, vertically aligned two-dimensional layers and cobalt atoms doping demonstrated a high hydrogen evolution activity and stability. In addition, density functional theory calculations indicate that molybdenum disulfide with moderate cobalt doping content possesses the optimal activity. This study demonstrates the validity of multiscale control in molybdenum disulfide via overall consideration of the mass transport, and the accessibility, quantity and capability of active sites towards electrocatalytic hydrogen evolution, which may also be extended to other energy-related processes.

          Abstract

          The hydrogen evolution reaction is a complicated process involving liquid-solid-gas three-phase interface behaviour. Here, the authors report the multiscale structural and electronic control of molybdenum disulfide foam and demonstrate its high activity and stability for hydrogen evolution.

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          Most cited references30

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          Generalized Gradient Approximation Made Simple.

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            Synergetic effect of MoS2 and graphene as cocatalysts for enhanced photocatalytic H2 production activity of TiO2 nanoparticles.

            The production of H(2) by photocatalytic water splitting has attracted a lot attention as a clean and renewable solar H(2) generation system. Despite tremendous efforts, the present great challenge in materials science is to develop highly active photocatalysts for splitting of water at low cost. Here we report a new composite material consisting of TiO(2) nanocrystals grown in the presence of a layered MoS(2)/graphene hybrid as a high-performance photocatalyst for H(2) evolution. This composite material was prepared by a two-step simple hydrothermal process using sodium molybdate, thiourea, and graphene oxide as precursors of the MoS(2)/graphene hybrid and tetrabutylorthotitanate as the titanium precursor. Even without a noble-metal cocatalyst, the TiO(2)/MoS(2)/graphene composite reaches a high H(2) production rate of 165.3 μmol h(-1) when the content of the MoS(2)/graphene cocatalyst is 0.5 wt % and the content of graphene in this cocatalyst is 5.0 wt %, and the apparent quantum efficiency reaches 9.7% at 365 nm. This unusual photocatalytic activity arises from the positive synergetic effect between the MoS(2) and graphene components in this hybrid cocatalyst, which serve as an electron collector and a source of active adsorption sites, respectively. This study presents an inexpensive photocatalyst for energy conversion to achieve highly efficient H(2) evolution without noble metals. © 2012 American Chemical Society
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              Nitrogen-doped mesoporous carbon of extraordinary capacitance for electrochemical energy storage.

              Carbon-based supercapacitors can provide high electrical power, but they do not have sufficient energy density to directly compete with batteries. We found that a nitrogen-doped ordered mesoporous few-layer carbon has a capacitance of 855 farads per gram in aqueous electrolytes and can be bipolarly charged or discharged at a fast, carbon-like speed. The improvement mostly stems from robust redox reactions at nitrogen-associated defects that transform inert graphene-like layered carbon into an electrochemically active substance without affecting its electric conductivity. These bipolar aqueous-electrolyte electrochemical cells offer power densities and lifetimes similar to those of carbon-based supercapacitors and can store a specific energy of 41 watt-hours per kilogram (19.5 watt-hours per liter).
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                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group
                2041-1723
                12 April 2017
                2017
                : 8
                : 14430
                Affiliations
                [1 ]State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University , Xiamen 361005, China
                [2 ]State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Chinese Academy of Science , Dalian 116023, China
                [3 ]School of Physics and Astronomy, University of Manchester , Oxford Road , M13 9PL Manchester, UK
                [4 ]Center for High Resolution Electron Microscopy, College of Materials Science and Engineering, Hunan University , Changsha 410082, China
                Author notes
                Article
                ncomms14430
                10.1038/ncomms14430
                5394285
                28401882
                543d2d7d-2468-4080-9dfb-85e65610fb84
                Copyright © 2017, The Author(s)

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 12 September 2016
                : 28 December 2016
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