Electrocatalytically Activating and Reducing N 2 Molecule by Tuning Activity of Local Hydrogen Radical

作者：Yuanyuan Yang, Cejun Hu, Jieqiong Shan, Chuanqi Cheng, Lili Han, Xinzhe Li, Ruguang Wang, Wei Li Xie, Yao Zheng, Tao Ling · 发表于：Angewandte Chemie International Edition · 年份：2023 · DOI：10.1002/anie.202300989 · 被引用次数：50 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Caching and Content Delivery、Advanced Photocatalysis Techniques

Abstract Decarbonizing N 2 conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N 2 on X/Fe−N−C (X=Pd, Ir and Pt) dual‐atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe−N−C catalysts can participate in the activation/reduction of N 2 adsorbed on the Fe site. More importantly, we reveal that the reactivity of X/Fe−N−C catalysts for N 2 activation/reduction can be well adjusted by the activity of H* generated on the X site, i.e., the interaction between the X−H bond. Specifically, X/Fe−N−C catalyst with the weakest X−H bonding exhibits the highest H* activity, which is beneficial to the subsequent cleavage of X−H bond for N 2 hydrogenation. With the most active H*, the Pd/Fe dual‐atom site promotes the turnover frequency of N 2 reduction by up to 10 times compared with the pristine Fe site.