催化作用
反应性(心理学)
活动站点
化学
吸附
氢原子
氢
分子
Atom(片上系统)
键裂
氢键
光化学
结晶学
立体化学
物理化学
有机化学
群(周期表)
计算机科学
嵌入式系统
病理
替代医学
医学
作者
Yuanyuan Yang,Cejun Hu,Jieqiong Shan,Chuanqi Cheng,Lili Han,Xinzhe Li,Ruguang Wang,Wei Xie,Yao Zheng,Tao Ling
标识
DOI:10.1002/anie.202300989
摘要
Decarbonizing N2 conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N2 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 N2 adsorbed on the Fe site. More importantly, we reveal that the reactivity of X/Fe-N-C catalysts for N2 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 N2 hydrogenation. With the most active H*, the Pd/Fe dual-atom site promotes the turnover frequency of N2 reduction by up to 10 times compared with the pristine Fe site.
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