Cargando…

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...

Descripción completa

Detalles Bibliográficos
Autor principal: Sun, Xiaoxu
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Frontiers Media S.A. 2021
Materias:
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
_version_ 1783748225385103360
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