journal article·2020-11-13

Tungsten Oxide/Carbide Surface Heterojunction Catalyst with High Hydrogen Evolution Activity

Yanglansen Cui, Xin Tan, Kefeng Xiao, Shenlong Zhao, Nicholas M. Bedford, Yuefeng Liu, Zichun Wang, Kuang-Hsu Wu, Jian Pan, Wibawa Hendra Saputera, Soshan Cheong, Richard D. Tilley, Sean C. Smith, Jimmy Yun, Liming Dai, Rose Amal, Da-Wei Wang

ACS Energy Letters· Volume 5· Issue 11
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Abstract

Tungsten carbide (WC) with imperfect structures determined by phase engineering and heteroatom doping has attracted a great deal of attention with respect to hydrogen evolution reaction (HER). However, less is known about its surface in HER. Herein, we report a tungsten oxide/carbide surface heterojunction catalyst (SHC) and reveal that the surface heterojunction that oscillates at HER potentials is responsible for high HER activity. This tungsten oxide/carbide SHC is active in both acidic (0.5 M H2SO4) and neutral [0.1 M phosphate buffer (pH 7.02)] electrolytes with a current density of 20 mA cm-2 at 0.32 mg cm-2 at overpotentials of-233 and-292 mV, respectively. From electron paramagnetic resonance spectroscopy and density functional theory calculations, we find that the surface heterojunction relaxed the adsorption of HER intermediates on WC. With in situ X-ray absorption spectroscopy, we are able to relate the HER activity to the bias-stimulated oscillation of the surface oxide/carbide heterojunction, which reflects the strong interfacial electronic coupling. This bias-oscillating surface heterojunction is thus suggested as a unique structural descriptor for WC-based HER catalysts, and the finding could be useful to other SHCs.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Catalytic Processes in Materials Science

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Particles and Catalysis Research Laboratory, School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia

Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics and Engineering, The Australian National University, Canberra, ACT 2601, Australia

The UNSW-BUCT-CWRU International Joint Laboratory, School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia

Dalian National Laboratory for Clean Energy (DNL), Dalian Institute of Chemical Physics, Chinese Academy of Science, 457 Zhongshan Road, Dalian 116023, China

Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia

Department of Engineering, Macquarie University, Sydney, NSW 2109, Australia

Research Group on Energy and Chemical Engineering Processing System, Department of Chemical Engineering, Institut Teknologi Bandung, Bandung 40132, Indonesia

Electron Microscope Unit, Mark Wainwright Analytical Centre, The University of New South Wales, Sydney, NSW 2052, Australia

College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, 26th Yuxiang Road, Shijiazhuang, Hebei 050018, P. R. China

Qingdao International Academician Park Research Institute, Qingdao, Shandong 266000, China

UNSW Digital Grid Futures Institute, The University of New South Wales, Sydney, NSW 2052, Australia

Funding

Australian Research Council · Tsinghua University · University of New South Wales

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