Unveiling the Spatially Dependent Cooperative Effect in Iridium Sites for Enhanced Acidic Water Oxidation

作者：Xiaoxia Chen, Hanwen Hu, Meihuan Liu, Xiaoyan Zhong, Donghai Wu, Hui Su · 发表于：Nano Letters · 年份：2025 · DOI：10.1021/acs.nanolett.5c04193 · 被引用次数：21 · 研究领域：Electrocatalysts for Energy Conversion、Ammonia Synthesis and Nitrogen Reduction、Catalytic Processes in Materials Science

The spatial distance between active sites is a critical factor governing hydroxyl (*OH)-group-mediated synergies in multiphase electrocatalysis. But direct experimental evidence correlating atomic-scale spatial arrangement with synergistic behavior, reaction kinetics, and catalytic mechanisms remains scarce. Using the acidic oxygen evolution reaction (OER) as a model, this study employs in situ synchrotron radiation infrared spectroscopy to demonstrate that adjacent active sites enable direct *OH coupling, forming the *O–O* intermediate. Complementary in situ X-ray absorption spectroscopy and theoretical calculations reveal that adjacent Ir sites induce electronic restructuring. This optimized electronic configuration facilitates unlocking a dual-site synergistic mechanism. Conversely, isolated sites (at a farther distance) exhibit spatial inaccessibility of *OH intermediates, forcing a higher-energy pathway via *OOH formation. These findings establish a universal paradigm for manipulating interfacial *OH dynamics through atomic-scale spatial engineering, applicable to diverse reactions including hydrogen evolution, oxygen reduction, and CO 2 reduction.