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Small. 2019 Mar;15(11):e1900358. doi: 10.1002/smll.201900358. Epub 2019 Feb 8.

Big to Small: Ultrafine Mo2 C Particles Derived from Giant Polyoxomolybdate Clusters for Hydrogen Evolution Reaction.

Author information

1
School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales, 2006, Australia.
2
School of Chemical Engineering, Sichuan University, Chengdu, Sichuan, 610065, China.
3
Department of Chemistry and the Institute for Computational and Engineering Sciences, The University of Texas at Austin, 105 E. 24th Street, Stop A5300, Austin, TX, 78712, USA.
4
Faculty of Engineering, The University of Tokyo, Yayoi, Bunkyo-Ku, Tokyo, 113-00, Japan.
5
School of Aerospace, Mechanical and Mechatronic Engineering, The University of Sydney, Sydney, New South Wales, 2006, Australia.
6
School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, 637459, Singapore.

Abstract

Due to its electronic structure, similar to platinum, molybdenum carbides (Mo2 C) hold great promise as a cost-effective catalyst platform. However, the realization of high-performance Mo2 C catalysts is still limited because controlling their particle size and catalytic activity is challenging with current synthesis methods. Here, the synthesis of ultrafine β-Mo2 C nanoparticles with narrow size distribution (2.5 ± 0.7 nm) and high mass loading (up to 27.5 wt%) on graphene substrate using a giant Mo-based polyoxomolybdate cluster, Mo132 ((NH4 )42 [Mo132 O372 (CH3 COO)30 (H2 O)72 ]·10CH3 COONH4 ·300H2 O) is demonstrated. Moreover, a nitrogen-containing polymeric binder (polyethyleneimine) is used to create MoN bonds between Mo2 C nanoparticles and nitrogen-doped graphene layers, which significantly enhance the catalytic activity of Mo2 C for the hydrogen evolution reaction, as is revealed by X-ray photoelectron spectroscopy and density functional theory calculations. The optimal Mo2 C catalyst shows a large exchange current density of 1.19 mA cm-2 , a high turnover frequency of 0.70 s-1 as well as excellent durability. The demonstrated new strategy opens up the possibility of developing practical platinum substitutes based on Mo2 C for various catalytic applications.

KEYWORDS:

graphene; hydrogen evolution reaction; molybdenum carbide; polyoxomolybdate

PMID:
30735307
DOI:
10.1002/smll.201900358

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