Introducing Brønsted acid sites to accelerate the bridging-oxygen-assisted deprotonation in acidic water oxidation

Yunzhou Wen, Cheng Liu, Rui Huang, Hui Zhang, Xiaobao Li, F. Pelayo García de Arquer, Zhi Liu, Youyong Li () and Bo Zhang ()
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Yunzhou Wen: Fudan University
Cheng Liu: Soochow University
Rui Huang: Fudan University
Hui Zhang: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
Xiaobao Li: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
F. Pelayo García de Arquer: ICFO - Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology
Zhi Liu: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
Youyong Li: Soochow University
Bo Zhang: Fudan University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Oxygen evolution reaction (OER) consists of four sequential proton-coupled electron transfer steps, which suffer from sluggish kinetics even on state-of-the-art ruthenium dioxide (RuO2) catalysts. Understanding and controlling the proton transfer process could be an effective strategy to improve OER performances. Herein, we present a strategy to accelerate the deprotonation of OER intermediates by introducing strong Brønsted acid sites (e.g. tungsten oxides, WOx) into the RuO2. The Ru-W binary oxide is reported as a stable and active iridium-free acidic OER catalyst that exhibits a low overpotential (235 mV at 10 mA cm−2) and low degradation rate (0.014 mV h−1) over a 550-hour stability test. Electrochemical studies, in-situ near-ambient pressure X-ray photoelectron spectroscopy and density functional theory show that the W-O-Ru Brønsted acid sites are instrumental to facilitate proton transfer from the oxo-intermediate to the neighboring bridging oxygen sites, thus accelerating bridging-oxygen-assisted deprotonation OER steps in acidic electrolytes. The universality of the strategy is demonstrated for other Ru-M binary metal oxides (M = Cr, Mo, Nb, Ta, and Ti).

Date: 2022
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DOI: 10.1038/s41467-022-32581-w

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