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  Electrochemical generation of catalytically active edge sites in c2n-type carbon materials for artificial nitrogen fixation

Zhang, W., Zhan, S., Qin, Q., Heil, T., Liu, X., Hwang, J., et al. (2022). Electrochemical generation of catalytically active edge sites in c2n-type carbon materials for artificial nitrogen fixation. Small, 18(42): 2204116. doi:10.1002/smll.202204116.

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Zhang, Wuyong1, Author           
Zhan, Shaoqi, Author
Qin, Qing1, Author           
Heil, Tobias2, Author           
Liu, Xiyu, Author
Hwang, Jinyeon1, Author           
Ferber, Thimo H., Author
Hofmann, Jan P., Author
Oschatz, Martin1, Author                 
Affiliations:
1Martin Oschatz, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2364733              
2Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863288              

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Free keywords: activation; electrocatalysis; nitrogen fixation; nitrogen-doped carbon
 Abstract: The electrochemical nitrogen reduction reaction (NRR) to ammonia (NH3) is a potentially carbon-neutral and decentralized supplement to the established Haber–Bosch process. Catalytic activation of the highly stable dinitrogen molecules remains a great challenge. Especially metal-free nitrogen-doped carbon catalysts do not often reach the desired selectivity and ammonia production rates due to their low concentration of NRR active sites and possible instability of heteroatoms under electrochemical potential, which can even contribute to false positive results. In this context, the electrochemical activation of nitrogen-doped carbon electrocatalysts is an attractive, but not yet established method to create NRR catalytic sites. Herein, a metal-free C2N material (HAT-700) is electrochemically etched prior to application in NRR to form active edge-sites originating from the removal of terminal nitrile groups. Resulting activated metal-free HAT-700-A shows remarkable catalytic activity in electrochemical nitrogen fixation with a maximum Faradaic efficiency of 11.4% and NH3 yield of 5.86 µg mg−1cat h−1. Experimental results and theoretical calculations are combined, and it is proposed that carbon radicals formed during activation together with adjacent pyridinic nitrogen atoms play a crucial role in nitrogen adsorption and activation. The results demonstrate the possibility to create catalytically active sites on purpose by etching labile functional groups prior to NRR.

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Language(s): eng - English
 Dates: 2022-09-162022
 Publication Status: Published in print
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 Identifiers: DOI: 10.1002/smll.202204116
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Title: Small
  Other : Small
Source Genre: Journal
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Publ. Info: Weinheim, Germany : Wiley-VCH
Pages: - Volume / Issue: 18 (42) Sequence Number: 2204116 Start / End Page: - Identifier: ISSN: 1613-6810