Efficient catalyst-free N2 fixation by water radical cations under ambient conditions

Xiaoping Zhang, Rui Su, Jingling Li, Liping Huang, Wenwen Yang, Konstantin Chingin, Roman Balabin, Jingjing Wang, Xinglei Zhang, Weifeng Zhu, Keke Huang, Shouhua Feng and Huanwen Chen ()
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Xiaoping Zhang: East China University of Technology
Rui Su: Jiangxi University of Chinese Medicine
Jingling Li: East China University of Technology
Liping Huang: Jiangxi University of Chinese Medicine
Wenwen Yang: East China University of Technology
Konstantin Chingin: Jiangxi University of Chinese Medicine
Jingjing Wang: Jiangxi University of Chinese Medicine
Xinglei Zhang: East China University of Technology
Weifeng Zhu: Jiangxi University of Chinese Medicine
Keke Huang: Jilin University
Shouhua Feng: Jilin University
Huanwen Chen: East China University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract The growth and sustainable development of humanity is heavily dependent upon molecular nitrogen (N2) fixation. Herein we discover ambient catalyst-free disproportionation of N2 by water plasma which occurs via the distinctive HONH-HNOH+• intermediate to yield economically valuable nitroxyl (HNO) and hydroxylamine (NH2OH) products. Calculations suggest that the reaction is prompted by the coordination of electronically excited N2 with water dimer radical cation, (H2O)2+•, in its two-center-three-electron configuration. The reaction products are collected in a 76-needle array discharge reactor with product yields of 1.14 μg cm–2 h–1 for NH2OH and 0.37 μg cm–2 h–1 for HNO. Potential applications of these compounds are demonstrated to make ammonia (for NH2OH), as well as to chemically react and convert cysteine, and serve as a neuroprotective agent (for HNO). The conversion of N2 into HNO and NH2OH by water plasma could offer great profitability and reduction of polluting emissions, thus giving an entirely look and perspectives to the problem of green N2 fixation.

Date: 2024
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DOI: 10.1038/s41467-024-45832-9

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