Electrocatalytically Activating and Reducing N<sub>2</sub> Molecule by Tuning Activity of Local Hydrogen Radical
Yuanyuan Yang, Cejun Hu, Jieqiong Shan, Chuanqi Cheng, Lili Han, Xinzhe Li, Ruguang Wang, Wei Xie, Yao Zheng, Tao Ling
Abstract
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.