Electrocatalytically Activating and Reducing N2 Molecule by Tuning Activity of Local Hydrogen Radical

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Author(s)

  • Yuanyuan Yang
  • Cejun Hu
  • Chuanqi Cheng
  • Lili Han
  • Xinzhe Li
  • Ruguang Wang
  • Wei Xie
  • Yao Zheng
  • Tao Ling

Detail(s)

Original languageEnglish
Article numbere202300989
Journal / PublicationAngewandte Chemie - International Edition
Volume62
Issue number20
Online published17 Mar 2023
Publication statusPublished - 8 May 2023
Externally publishedYes

Abstract

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. © 2023 Wiley-VCH GmbH.

Research Area(s)

  • Carbon Materials, Electrocatalysis, Metal-Free Catalysts, Nitrogen Reduction Reaction

Citation Format(s)

Electrocatalytically Activating and Reducing N2 Molecule by Tuning Activity of Local Hydrogen Radical. / Yang, Yuanyuan; Hu, Cejun; Shan, Jieqiong et al.
In: Angewandte Chemie - International Edition, Vol. 62, No. 20, e202300989, 08.05.2023.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review