Journal
ACS ENERGY LETTERS
Volume 5, Issue 11, Pages 3560-3568Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c01858
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Funding
- Australian Research Council [DP190101008, FT190100058]
- ARC ITRP [IH180100020]
- UNSW-Tsinghua Joint Grant
- UNSW Digital Grid Futures Institute, UNSW Sydney
- DOE Office of Science [DE-AC02-06CH11357]
- DOE
- MRCAT member institutions
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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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