Authors
Jie Li, Guangming Zhan, Jianhua Yang, Fengjiao Quan, Chengliang Mao, Yang Liu, Bo Wang, Fengcai Lei, Lejing Li, Alice WM Chan, Liangpang Xu, Yanbiao Shi, Yi Du, Weichang Hao, Po Keung Wong, Jianfang Wang, Shi-Xue Dou, Lizhi Zhang, Jimmy C Yu
Publication date
2020/3/30
Journal
Journal of the american chemical society
Volume
142
Issue
15
Pages
7036-7046
Publisher
American Chemical Society
Description
The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat–1 h–1), a small partial current density (<1 mA cm–2), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat–1 h–1) than the Haber–Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen–hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower …
Total citations
20202021202220232024474152240166
Scholar articles
J Li, G Zhan, J Yang, F Quan, C Mao, Y Liu, B Wang… - Journal of the american chemical society, 2020