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231225s2020 xx |||||o 00| ||eng c |
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|a 10.1002/adma.201907690
|2 doi
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|a pubmed24n1030.xml
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|a (DE-627)NLM309308240
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|a (NLM)32346928
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|a DE-627
|b ger
|c DE-627
|e rakwb
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|a eng
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|a Liu, Yan
|e verfasserin
|4 aut
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|a A Highly Efficient Metal-Free Electrocatalyst of F-Doped Porous Carbon toward N2 Electroreduction
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|c 2020
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
|b c
|2 rdamedia
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|a ƒa Online-Ressource
|b cr
|2 rdacarrier
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|a Date Revised 30.09.2020
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
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|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
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|a Journal Article
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|a F-doped carbon
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|a N2 electroreduction
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|a NH3 product
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|a metal-free catalysts
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1 |
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|a Li, Qiuyao
|e verfasserin
|4 aut
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1 |
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|a Guo, Xu
|e verfasserin
|4 aut
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1 |
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|a Kong, Xiangdong
|e verfasserin
|4 aut
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1 |
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|a Ke, Jingwen
|e verfasserin
|4 aut
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1 |
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|a Chi, Mingfang
|e verfasserin
|4 aut
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|a Li, Qunxiang
|e verfasserin
|4 aut
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|a Geng, Zhigang
|e verfasserin
|4 aut
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|a Zeng, Jie
|e verfasserin
|4 aut
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0 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 32(2020), 24 vom: 17. Juni, Seite e1907690
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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|g volume:32
|g year:2020
|g number:24
|g day:17
|g month:06
|g pages:e1907690
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|u http://dx.doi.org/10.1002/adma.201907690
|3 Volltext
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