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      Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production

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          Abstract

          Electrochemical water splitting has been considered as a promising approach to produce clean and sustainable hydrogen fuel. However, the lack of high-performance and low-cost electrocatalysts for hydrogen evolution reaction hinders the large-scale application. As a new class of porous materials with tunable structure and composition, metal-organic frameworks have been considered as promising candidates to synthesize various functional materials. Here we demonstrate a metal-organic frameworks-assisted strategy for synthesizing nanostructured transition metal carbides based on the confined carburization in metal-organic frameworks matrix. Starting from a compound consisting of copper-based metal-organic frameworks host and molybdenum-based polyoxometalates guest, mesoporous molybdenum carbide nano-octahedrons composed of ultrafine nanocrystallites are successfully prepared as a proof of concept, which exhibit remarkable electrocatalytic performance for hydrogen production from both acidic and basic solutions. The present study provides some guidelines for the design and synthesis of nanostructured electrocatalysts.

          Abstract

          There is extensive research into non-platinum electrocatalysts for hydrogen evolution. Here, the authors report a molybdenum carbide catalyst, prepared via the carburization of a copper metal-organic framework host/molybdenum-based polyoxometalates guest system, and demonstrate its catalytic activity.

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          Most cited references 16

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          Metal-organic frameworks.

           S. James (2003)
          Metal-organic frameworks are a recently-identified class of porous polymeric material, consisting of metal ions linked together by organic bridging ligands, and are a new development on the interface between molecular coordination chemistry and materials science. A range of novel structures has been prepared which feature amongst the largest pores known for crystalline compounds, very high sorption capacities and complex sorption behaviour not seen in aluminosilicate zeolites. The development of synthetic approaches to these materials and investigations of their properties are reviewed.
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            Enhanced Catalytic Activity in Strained Chemically Exfoliated WS2 Nanosheets for Hydrogen Evolution

            The ability to efficiently evolve hydrogen via electrocatalysis at low overpotentials holds tremendous promise for clean energy. Hydrogen evolution reaction (HER) can be easily achieved from water if a voltage above the thermodynamic potential of the HER is applied. Large overpotentials are energetically inefficient but can be lowered with expensive platinum based catalysts. Replacement of Pt with inexpensive, earth abundant electrocatalysts would be significantly beneficial for clean and efficient hydrogen evolution. Towards this end, promising HER characteristics have been reported using 2H (trigonal prismatic) XS2 (where X = Mo or W) nanoparticles with a high concentration of metallic edges as electrocatalysts. The key challenges for HER with XS2 are increasing the number and catalytic activity of active sites. Here we report atomically thin nanosheets of chemically exfoliated WS2 as efficient catalysts for hydrogen evolution with very low overpotentials. Atomic-resolution transmission electron microscopy and spectroscopy analyses indicate that enhanced electrocatalytic activity of WS2 is associated with high concentration of strained metallic 1T (octahedral) phase in the as-exfoliated nanosheets. Density functional theory calculations reveal that the presence of strain in the 1T phase leads to an enhancement of the density of states at the Fermi level and increases the catalytic activity of the WS2 nanosheet. Our results suggest that chemically exfoliated WS2 nanosheets could be interesting catalysts for hydrogen evolution.
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              Powering the planet with solar fuel.

               Harry B Gray (2009)
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                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Pub. Group
                2041-1723
                11 March 2015
                : 6
                Affiliations
                [1 ]School of Chemical and Biomedical Engineering, Nanyang Technological University , 62 Nanyang Drive, Singapore 637459, Singapore
                Author notes
                [*]

                These authors contributed equally to this work.

                Article
                ncomms7512
                10.1038/ncomms7512
                4382699
                25758159
                Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.

                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/

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