Atomic Ru coordinated by channel ammonia in V-doped tungsten bronze for highly efficient hydrogen-evolution reaction

doi:10.1016/S1872-2067(23)64489-4

Abstract

Abstract:

Regulation of the atomic distribution is crucial for the development of atomically dispersed electrocatalysts. In this study, atomic Ru coordinated by channel ammonia in V-doped tungsten bronze (Ru/V-NHWO, Ru 0.44 wt%, V 0.45 wt%) was used as a high-performance catalyst for the hydrogen evolution reaction (HER), demonstrating remarkable mass activity in a wide pH range. Atomic Ru with a regulated spatial distribution and electronic structure was achieved owing to its unique coordination with the ammonia species in the hexagonal channels of V-NHWO. V doping in NHWO led to enhanced intrinsic activity and conductivity. Theoretical calculations revealed that the multichannel, vertically integrated Ru sites in the V-doped channels, as well as the coexisting Ru sites without multichannels or V-doping, improved the free energy of water dissociation and hydrogen sorption, which boosted the HER activity. Our study paves a new way for constructing atomically dispersed materials with a regulated spatial distribution for diverse applications.

Key words: Atomic Ru, Channel ammonia, Hexagonal crystal channel, Tungsten bronze, Hydrogen evolution reaction

Ce Han, Bingbao Mei, Qinghua Zhang, Huimin Zhang, Pengfei Yao, Ping Song, Xue Gong, Peixin Cui, Zheng Jiang, Lin Gu, Weilin Xu. Atomic Ru coordinated by channel ammonia in V-doped tungsten bronze for highly efficient hydrogen-evolution reaction[J]. Chinese Journal of Catalysis, 2023, 51: 80-89.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64489-4

https://www.cjcatal.com/EN/Y2023/V51/I8/80

Figures/Tables 4

Fig. 1. (a) Schematic illustration for the fabrication of Ru/V-NHWO nanorod arrays supported by CC substrate. (b-e) SEM, TEM, atomic HAADF-STEM, and elemental mapping images of Ru/V-NHWO/CC.

Fig. 2. (a) XPS results of W 4f for V-NHWO/CC, Ru/NHWO/CC, and Ru/V-NHWO/CC. (b) XPS results of Ru 3d for Ru/NHWO/CC and Ru/V-NHWO/CC. (c) XPS results of N 1s for V-NHWO/CC, Ru/NHWO/CC, and Ru/V-NHWO/CC. Normalized Ru K-edge XANES curves (d), and FT (e) and WT (f) of k3-weighted EXAFS signals for Ru foil, RuO2, Ru/NHWO/CC, and Ru/V-NHWO/CC. Normalized W L3-edge XANES curves (g), and FT (h) and WT (i) of k3-weighted EXAFS signals for W foil, WO3, Ru/NHWO/CC, and Ru/V-NHWO/CC.

Fig. 3. iR-corrected LSV curves (a), Tafel plots (b), Nyquist plots (c), and electrochemical double-layer capacitances (d) of bare CC, V-NHWO/CC, Ru/NHWO/CC, and Ru/V-NHWO/CC in 1 mol L?1 KOH electrolyte. (e-g) iR-corrected LSV curves of Ru/V-NHWO/CC, Pt/C/CC, and Ru/C/CC. (h) Chronopotentiometric tests of Ru/V-NHWO/CC at 10?mA cm?2 for 20?h in 1 mol L?1 KOH, 1 mol L?1 PBS, and 0.5 mol L?1 H2SO4 electrolytes.

Fig. 4. (a) Structural models of SA Ru/V-NHWO, Ver-Ru/V-NHWO, and Ru/V-NHWO. DFT-calculated reaction energy diagrams of water dissociation (b) and H intermediate sorption (c) for V-NHWO, Ru NP/V-NHWO, SA Ru/V-NHWO, Ver-Ru/V-NHWO, Ru2 site, and Ru/V-NHWO. Charge-density difference analysis for Ru/V-NHWO before (d) and after (e) H-intermediate sorption. Yellow represents electron agglomeration, and blue represents electron dissipation.

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