Improved kinetics of OER on Ru-Pb binary electrocatalyst by decoupling proton-electron transfer

doi:10.1016/S1872-2067(21)63856-1

Abstract

Abstract:

The acidic oxygen evolution reaction (OER) is central to water electrolysis using proton-exchange membranes. However, even as benchmark catalysts in the acidic OER, Ru-based catalysts still suffer from sluggish kinetics owing to the scaling relationship that arises from the traditional concerted proton-electron transfer (CPET) process. Motivated by the knowledge that a charged surface may be favorable for accelerating the OER kinetics, we posited the incorporation of elements with pseudocapacitive properties into Ru-based catalysts. Herein, we report a RuPbO_x electrocatalyst for efficient and stable water oxidation in acid with a low overpotential of 191 mV to reach 10 mA cm^-2 and a low Tafel slope of 39 mV dec^-1. The combination of electrochemical analysis, X-ray photoelectron spectroscopy, and in situ Raman spectroscopy demonstrated that the improved OER kinetics was associated with the formation of superoxide precursors on the strongly charged surface after Pb incorporation, indicating a non-concerted proton-electron transfer mechanism for the OER on RuPbO_x.

Key words: Electrocatalysis, Acidic oxygen evolution reaction, Ruthenium oxide, In situ Raman, Proton-coupled electron transfer

Rui Huang, Yunzhou Wen, Huisheng Peng, Bo Zhang. Improved kinetics of OER on Ru-Pb binary electrocatalyst by decoupling proton-electron transfer[J]. Chinese Journal of Catalysis, 2022, 43(1): 130-138.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63856-1

https://www.cjcatal.com/EN/Y2022/V43/I1/130

Figures/Tables 4

Fig. 1. Characterization of RuPbOx catalyst. (a) TEM image. Scale bar: 50 nm. (b) HR-TEM image. Inset: FFT pattern from the nanoparticle can be indexed to (110), (101), and (211) planes of rutile structure. Scale bar: 10 nm. (c) XRD patterns. (d-g) HADDF-STEM image and EDX element mappings. Scale bar: 50 nm. (h) Normalized Ru K-edge XANES spectra of RuPbOx, Ru powder, RuCl3, and commercial RuO2. (i) Fourier-transform EXAFS profile of Ru K-edge for RuPbOx, Ru powder, RuCl3, and commercial RuO2.

Fig. 2. Electrochemical performance. (a) OER polarization curves of different catalysts. The curves were 95% iR-compensated; (b) η10 and mass activities of different catalysts; (c) Steady-state Tafel plots for different catalysts; (d) Steady-state polarization curve of RuPbOx in PEM electrolyzer. Inset: schematic of PEM electrolyzer; (e) Chronopotentiometry stability test of RuPbOx at 10 mA cm-2.

Fig. 3. Surface chemical state of RuPbOx. (a) Cyclic voltammogram of RuPbOx in the range of 0-1.5 V vs. RHE at 200 mV s-1 scan rate; (b) Relationship between total charge and applied potential of different catalysts, measured by pulse voltammetry; (c,d) Fitted O 1s spectra for RuPbOx and RuO2 after OER. The fits are described in the text; (e,f) In situ EC-Raman spectra of RuPbOx and RuO2. * Peaks of H2SO4 electrolyte and substrate. The yellow region in (e) represents the superoxide species.

Fig. 4. Non-concerted proton-electron transfer steps on RuPbOx. (a) pH-dependent OER activity of RuPbOx and RuO2 at η = 300 mV; (b) pH-Dependence of Tafel slope of RuPbOx; (c) Schematic of the non-concerted proton-electron transfer mechanism. Brown balls: Ru, black balls: Pb, white balls: O, red ball: H. The active oxygen species are marked with yellow.

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