Tungsten Oxide/Carbide Surface Heterojunction Catalyst with High Hydrogen Evolution Activity,ACS Energy Letters

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Tungsten Oxide/Carbide Surface Heterojunction Catalyst with High Hydrogen Evolution Activity
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-10-23 , DOI: 10.1021/acsenergylett.0c01858
Yanglansen Cui ₁ , Xin Tan ₂ , Kefeng Xiao ₁ , Shenlong Zhao ₃ , Nicholas M. Bedford ₁ , Yuefeng Liu ₄ , Zichun Wang _{5,

6} , Kuang-Hsu Wu ₁ , Jian Pan ₁ , Wibawa Hendra Saputera _{1,

7} , Soshan Cheong ₈ , Richard D. Tilley ₈ , Sean C. Smith ₂ , Jimmy Yun _{1,

9,

10} , Liming Dai ₃ , Rose Amal ₁ , Da-Wei Wang _{1,

11}

Affiliation

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

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.

中文翻译：

高放氢活性的氧化钨/碳化物表面异质结催化剂

由相工程和杂原子掺杂确定的具有不完美结构的碳化钨（WC）在制氢反应（HER）方面引起了极大的关注。但是，在HER中对其表面的了解却很少。本文中，我们报告了氧化钨/碳化物表面异质结催化剂（SHC），并揭示了在HER电位振荡的表面异质结是高HER活性的原因。此氧化钨/碳化物SHC是在酸性（0.5 MH活性₂ SO ₄）和中性[0.1M磷酸盐缓冲液（pH 7.02）]电解质用的20毫安cm 2的电流密度^-2 0.32毫克厘米^-2分别处于-233和-292 mV的过电势。通过电子顺磁共振光谱和密度泛函理论计算，我们发现表面异质结使HER中间体在WC上的吸附放宽了。借助原位X射线吸收光谱，我们能够将HER活性与表面氧化物/碳化物异质结的偏压激发振荡相关联，这反映了强界面电子耦合。因此，该偏压振荡的表面异质结被认为是基于WC的HER催化剂的独特结构描述，这一发现对其他SHC可能有用。

更新日期：2020-11-13

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