A Highly Efficient Metal-Free Electrocatalyst of F-Doped Porous Carbon toward N2 Electroreduction

© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 32(2020), 24 vom: 17. Juni, Seite e1907690
1. Verfasser: Liu, Yan (VerfasserIn)
Weitere Verfasser: Li, Qiuyao, Guo, Xu, Kong, Xiangdong, Ke, Jingwen, Chi, Mingfang, Li, Qunxiang, Geng, Zhigang, Zeng, Jie
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2020
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article F-doped carbon N2 electroreduction NH3 product metal-free catalysts
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520 |a N2 electroreduction into NH3 represents an attractive prospect for N2 utilization. Nevertheless, this process suffers from low Faraday efficiency (FE) and yield rate for NH3 . In this work, a highly efficient metal-free catalyst is developed by introducing F atoms into a 3D porous carbon framework (F-doped carbon) toward N2 electroreduction. At -0.2 V versus reversible hydrogen electrode (RHE), the F-doped carbon achieves the highest FE of 54.8% for NH3 , which is 3.0 times as high as that (18.3%) of pristine carbon frameworks. Notably, at -0.3 V versus RHE, the yield rate of F-doped carbon for NH3 reaches 197.7 µgNH3 mg-1 cat. h-1 . Such a value is more than one order of magnitude higher than those of other metal-free electrocatalysts under the near-ambient conditions for NH3 product to date. Mechanistic studies reveal that the improved performance in N2 electroreduction for F-doped carbon originates from the enhanced binding strength of N2 and the facilitated dissociation of N2 into *N2 H. F bonding to C atom creates a Lewis acid site due to the different electronegativity between the F and C atoms. As such, the repulsive interaction between the Lewis acid site and proton H suppresses the activity of H2 evolution reaction, thus enhancing the selectivity of N2 electroreduction into NH3 
650 4 |a Journal Article 
650 4 |a F-doped carbon 
650 4 |a N2 electroreduction 
650 4 |a NH3 product 
650 4 |a metal-free catalysts 
700 1 |a Li, Qiuyao  |e verfasserin  |4 aut 
700 1 |a Guo, Xu  |e verfasserin  |4 aut 
700 1 |a Kong, Xiangdong  |e verfasserin  |4 aut 
700 1 |a Ke, Jingwen  |e verfasserin  |4 aut 
700 1 |a Chi, Mingfang  |e verfasserin  |4 aut 
700 1 |a Li, Qunxiang  |e verfasserin  |4 aut 
700 1 |a Geng, Zhigang  |e verfasserin  |4 aut 
700 1 |a Zeng, Jie  |e verfasserin  |4 aut 
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773 1 8 |g volume:32  |g year:2020  |g number:24  |g day:17  |g month:06  |g pages:e1907690 
856 4 0 |u http://dx.doi.org/10.1002/adma.201907690  |3 Volltext 
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