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

作者：Yunzhou Wen, Cheng Liu, Rui Huang, Hui Zhang, Xiaobao Li, F. Pelayo Garcı́a de Arquer, Zhi Liu, Youyong Li, Bo Zhang · 发表于：Nature Communications · 年份：2022 · DOI：10.1038/s41467-022-32581-w · 被引用次数：228 · 研究领域：Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques、Catalytic Processes in Materials Science

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 (RuO 2 ) 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, WO x ) into the RuO 2 . 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).