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Cited by 172

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Revealing the Origin of Activity in Nitrogen‐Doped Nanocarbons towards Electrocatalytic Reduction of Carbon Dioxide

Xu, Junyuan, Kan, Yuhe, Huang, Rui, Zhang, Bingsen, Wang, Bolun, Wu, Kuang‐Hsu, Lin, Yangming, Sun, Xiaoyan, Li, Qingfeng, Centi, Gabriele, Su, Dangsheng·2016·ChemSusChem

Abstract

Carbon nanotubes (CNTs) are functionalized with nitrogen atoms for reduction of carbon dioxide (CO 2). The investigation explores the origin of the catalyst′s activity and the role of nitrogen chemical states therein. The catalysts show excellent performances, with about 90 % current efficiency for CO formation and stability over 60 hours. The Tafel analyses and density functional theory calculations suggest that the reduction of CO 2 proceeds through an initial rate‐determining transfer of one electron to CO 2, which leads to the formation of carbon dioxide radical anion (CO 2.−). The initial reduction barrier is too high on pristine CNTs, resulting in a very high overpotentials at which the hydrogen evolution reaction dominates over CO 2 reduction. The doped nitrogen atoms stabilize the radical anion, thereby lowering the initial reduction barrier and improving the intrinsic activity. The most efficient nitrogen chemical state for this reaction is quaternary nitrogen, followed by pyridinic and pyrrolic nitrogen.

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Crossref · 10.1002/cssc.201600202

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Metadata

Authors
Xu, J., Kan, Y., Huang, R., Zhang, B., Wang, B., Wu, K., Lin, Y., Sun, X., Li, Q., Centi, G., & Su, D.
Venue
ChemSusChem
Publisher
Wiley
Published
2016-04-21
Volume
9
Issue
10
Pages
1085-1089
ISSN
  • 1864-5631 (ISSN-L)
  • 1864-564X
OpenAlex
W2337608824
Cited by
172
References
6
FWCI
6.61
Type
journal article
Language
en
Open access
closed

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