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Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene
The CO(2) electrochemical reduction reaction (CO(2)RR) has been a promising conversion method for CO(2) utilization. Currently, the lack of electrocatalysts with favorable stability and high efficiency hindered the development of CO(2)RR. Nitrogen-doped graphene nanocarbons have great promise in rep...
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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Frontiers Media S.A.
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8416613/ https://www.ncbi.nlm.nih.gov/pubmed/34490215 http://dx.doi.org/10.3389/fchem.2021.734460 |
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author | Sun, Xiaoxu |
author_facet | Sun, Xiaoxu |
author_sort | Sun, Xiaoxu |
collection | PubMed |
description | The CO(2) electrochemical reduction reaction (CO(2)RR) has been a promising conversion method for CO(2) utilization. Currently, the lack of electrocatalysts with favorable stability and high efficiency hindered the development of CO(2)RR. Nitrogen-doped graphene nanocarbons have great promise in replacing metal catalysts for catalyzing CO(2)RR. By using the density functional theory (DFT) method, the catalytic mechanism and activity of CO(2)RR on 11 types of nitrogen-doped graphene have been explored. The free energy analysis reveals that the zigzag pyridinic N- and zigzag graphitic N-doped graphene possess outstanding catalytic activity and selectivity for HCOOH production with an energy barrier of 0.38 and 0.39 eV, respectively. CO is a competitive product since its free energy lies only about 0.20 eV above HCOOH. The minor product is CH(3)OH and CH(4) for the zigzag pyridinic N-doped graphene and HCHO for zigzag graphitic N-doped graphene, respectively. However, for Z-pyN, CO(2)RR is passivated by too strong HER. Meanwhile, by modifying the pH value of the electrolyte, Z-GN could be selected as a promising nonmetal electrocatalyst for CO(2)RR in generating HCOOH. |
format | Online Article Text |
id | pubmed-8416613 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | Frontiers Media S.A. |
record_format | MEDLINE/PubMed |
spelling | pubmed-84166132021-09-05 Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene Sun, Xiaoxu Front Chem Chemistry The CO(2) electrochemical reduction reaction (CO(2)RR) has been a promising conversion method for CO(2) utilization. Currently, the lack of electrocatalysts with favorable stability and high efficiency hindered the development of CO(2)RR. Nitrogen-doped graphene nanocarbons have great promise in replacing metal catalysts for catalyzing CO(2)RR. By using the density functional theory (DFT) method, the catalytic mechanism and activity of CO(2)RR on 11 types of nitrogen-doped graphene have been explored. The free energy analysis reveals that the zigzag pyridinic N- and zigzag graphitic N-doped graphene possess outstanding catalytic activity and selectivity for HCOOH production with an energy barrier of 0.38 and 0.39 eV, respectively. CO is a competitive product since its free energy lies only about 0.20 eV above HCOOH. The minor product is CH(3)OH and CH(4) for the zigzag pyridinic N-doped graphene and HCHO for zigzag graphitic N-doped graphene, respectively. However, for Z-pyN, CO(2)RR is passivated by too strong HER. Meanwhile, by modifying the pH value of the electrolyte, Z-GN could be selected as a promising nonmetal electrocatalyst for CO(2)RR in generating HCOOH. Frontiers Media S.A. 2021-08-19 /pmc/articles/PMC8416613/ /pubmed/34490215 http://dx.doi.org/10.3389/fchem.2021.734460 Text en Copyright © 2021 Sun. https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms. |
spellingShingle | Chemistry Sun, Xiaoxu Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene |
title | Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene |
title_full | Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene |
title_fullStr | Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene |
title_full_unstemmed | Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene |
title_short | Achieving Selective and Efficient Electrocatalytic Activity for CO(2) Reduction on N-Doped Graphene |
title_sort | achieving selective and efficient electrocatalytic activity for co(2) reduction on n-doped graphene |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8416613/ https://www.ncbi.nlm.nih.gov/pubmed/34490215 http://dx.doi.org/10.3389/fchem.2021.734460 |
work_keys_str_mv | AT sunxiaoxu achievingselectiveandefficientelectrocatalyticactivityforco2reductiononndopedgraphene |