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Tungsten Oxide/Carbide Surface Heterojunction Catalyst with High Hydrogen Evolution Activity
Cui Y.a, Tan X.b, Xiao K.a, Zhao S.a, Bedford N.M.a, Liu Y., Wang Z.d,e, Wu K.-H.a, Pan J.a, Saputera W.H.a,h, Cheong S.a, Tilley R.D.a, Smith S.C.b, Yun J.a,f,g, Dai L.a, Amal R.a, Wang D.-W.a
a Particles and Catalysis Research Laboratory, School of Chemical Engineering, University of New South Wales, Sydney, 2052, Australia
b Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics and Engineering, Australian National University, Canberra, 2601, Australia
c Dalian National Laboratory for Clean Energy (DNL), Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian, 116023, China
d Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, University of Sydney, Sydney, 2006, Australia
e Department of Engineering, Macquarie University, Sydney, 2109, Australia
f College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang, Hebei, 050018, China
g Qingdao International Academician Park Research Institute, Qingdao, Shandong, 266000, China
h Research Group on Energy and Chemical Engineering Processing System, Department of Chemical Engineering, Institut Teknologi Bandung, Bandung, 40132, Indonesia
[vc_row][vc_column][vc_row_inner][vc_column_inner][vc_separator css=”.vc_custom_1624529070653{padding-top: 30px !important;padding-bottom: 30px !important;}”][/vc_column_inner][/vc_row_inner][vc_row_inner layout=”boxed”][vc_column_inner width=”3/4″ css=”.vc_custom_1624695412187{border-right-width: 1px !important;border-right-color: #dddddd !important;border-right-style: solid !important;border-radius: 1px !important;}”][vc_empty_space][megatron_heading title=”Abstract” size=”size-sm” text_align=”text-left”][vc_column_text]© 2020 American Chemical Society. All rights reserved.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.[/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”Author keywords” size=”size-sm” text_align=”text-left”][vc_column_text]Electron paramagnetic resonance spectroscopy,Electronic coupling,Hydrogen evolution,Imperfect structures,In-situ X-ray absorption spectroscopy,Oscillating surfaces,Phosphate buffers,Structural descriptor[/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”Indexed keywords” size=”size-sm” text_align=”text-left”][vc_column_text][/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”Funding details” size=”size-sm” text_align=”text-left”][vc_column_text]D.-W.W. acknowledges the financial support from the Australian Research Council Discovery Project (DP190101008), a Future Fellowship (FT190100058), ARC ITRP (IH180100020), and a UNSW-Tsinghua Joint Grant. This research was partially supported by funding from the UNSW Digital Grid Futures Institute, UNSW Sydney, under a cross-disciplinary fund scheme; the views expressed herein are those of the authors and are not necessarily those of the institute. In situ XAS experiments were performed at beamline 10-ID-B of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. Beamline 10-ID-B is managed by the Materials Research Collaborative Access Team (MRCAT) and additionally supported by the DOE and MRCAT member institutions. The authors thank Dr. Joshua Wright for assistance with experiments at beamline 10-ID-B. The authors also thank the UNSW Mark Wainwright Analytical Centre for their facilities and technical support and facilities supported by Microscopy Australia at the Electron Unit at UNSW.[/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”DOI” size=”size-sm” text_align=”text-left”][vc_column_text]https://doi.org/10.1021/acsenergylett.0c01858[/vc_column_text][/vc_column_inner][vc_column_inner width=”1/4″][vc_column_text]Widget Plumx[/vc_column_text][/vc_column_inner][/vc_row_inner][/vc_column][/vc_row][vc_row][vc_column][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][/vc_column][/vc_row]