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

• Published in: Nature communications Vol. 15; no. 1; p. 1535
• Main Authors: Zhang, Xiaoping, Su, Rui, Li, Jingling, Huang, Liping, Yang, Wenwen, Chingin, Konstantin, Balabin, Roman, Wang, Jingjing, Zhang, Xinglei, Zhu, Weifeng, Huang, Keke, Feng, Shouhua, Chen, Huanwen
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 20.02.2024; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/131; 140/58; 639/638/11/296; 639/638/224/685; Air pollution; Ammonia; Catalysts; Cations; Chemical Sciences; Chemistry; Disproportionation; Economics; Electrodes; Energy consumption; Engineering Sciences; Environmental Sciences; Humanities and Social Sciences; Hydroxylamine; Mass spectrometry; Medical research; multidisciplinary; Neuroprotection; Nitrogen; Nitrogen fixation; Nitrogen plasma; Nitrogenation; Physics; Plasma; Pollution control; Profitability; Reaction products; Science; Science (multidisciplinary); Scientific imaging; Sustainable development; ammonia; nitroxyl; water dimer radical cation; nitrogen fixation; plasma; hydroxylamine
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-45832-9

The growth and sustainable development of humanity is heavily dependent upon molecular nitrogen (N 2 ) fixation. Herein we discover ambient catalyst-free disproportionation of N 2 by water plasma which occurs via the distinctive HONH-HNOH +• intermediate to yield economically valuable nitroxyl (HNO) and hydroxylamine (NH 2 OH) products. Calculations suggest that the reaction is prompted by the coordination of electronically excited N 2 with water dimer radical cation, (H 2 O) 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 NH 2 OH and 0.37 μg cm –2 h –1 for HNO. Potential applications of these compounds are demonstrated to make ammonia (for NH 2 OH), as well as to chemically react and convert cysteine, and serve as a neuroprotective agent (for HNO). The conversion of N 2 into HNO and NH 2 OH by water plasma could offer great profitability and reduction of polluting emissions, thus giving an entirely look and perspectives to the problem of green N 2 fixation. The growth and sustainable development of humanity is heavily dependent upon N 2 fixation. Herein, authors developed an ambient catalyst-free disproportionation of N 2 by water plasma to yield economically valuable nitroxyl and hydroxylamine products.