Revealing the role of interfacial water and key intermediates at ruthenium surfaces in the alkaline hydrogen evolution reaction

作者：Xing Chen, Xiaoting Wang, Jiabo Le, Shumin Li, Xue Wang, Yujin Zhang, Petar M. Radjenovic, Yu Zhao, Yaohui Wang, Xiu‐Mei Lin, Jin‐Chao Dong, Jian‐Feng Li · 发表于：Nature Communications · 年份：2023 · DOI：10.1038/s41467-023-41030-1 · 被引用次数：563 · 研究领域：Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science、Ammonia Synthesis and Nitrogen Reduction

Abstract Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na + ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts.