First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene
The CO oxidation mechanism on graphene with divacancy (DG) embedded with transition metal from Sc to Zn has been studied by using first principles calculations. The results indicate that O2 molecule is preferentially adsorbed on Sc, Ti, V, Cr, Mn, and Fe-DG, which can avoid the CO poisoning problem...
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2018-05-01
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doaj-dd64f4334b0f44fc93e6ef8c9a1665992020-11-25T00:17:28ZengFrontiers Media S.A.Frontiers in Chemistry2296-26462018-05-01610.3389/fchem.2018.00187348132First Principles Study on the CO Oxidation on Mn-Embedded Divacancy GrapheneQuanguo Jiang0Jianfeng Zhang1Zhimin Ao2Huajie Huang3Haiyan He4Yuping Wu5College of Mechanics and Materials, Hohai University, Nanjing, ChinaCollege of Mechanics and Materials, Hohai University, Nanjing, ChinaGuangzhou Key Laboratory of Environmental Catalysis and Pollution Control, Institute of Environmental Health and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, ChinaCollege of Mechanics and Materials, Hohai University, Nanjing, ChinaCollege of Mechanics and Materials, Hohai University, Nanjing, ChinaCollege of Mechanics and Materials, Hohai University, Nanjing, ChinaThe CO oxidation mechanism on graphene with divacancy (DG) embedded with transition metal from Sc to Zn has been studied by using first principles calculations. The results indicate that O2 molecule is preferentially adsorbed on Sc, Ti, V, Cr, Mn, and Fe-DG, which can avoid the CO poisoning problem that many catalysts facing and is beneficial to the CO oxidation progress. Further study indicates that Mn-DG shows the best catalytic properties for CO oxidation with consideration of both Langmuir-Hinshelwood (LH) and Eley-Rideal (ER) oxidation mechanisms. Along the ER mechanism, the reaction energy barrier for the first step (CO free + O2pre-adsorbed → OOCO) is 0.96 eV. Along the LH mechanism, the energy barrier for the rate limiting step (CO adsorbed + O2adsorbed → OOCO) is only 0.41 eV, indicating that the CO oxidation on Mn-DG will occur along LH mechanism. The Hirshfeld charge distributions of O2 and CO molecules is tuned by the embedded Mn atom, and the charge transfer from the embedded Mn atom to the adsorbed molecules plays an important role for the CO oxidation. The result shows that the Mn-embedded divacancy graphene is a noble-metal free and efficient catalyst for CO oxidation at low temperature.https://www.frontiersin.org/article/10.3389/fchem.2018.00187/fullgraphenedivacancyMn-embeddedCO oxidationfirst principles calculations |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Quanguo Jiang Jianfeng Zhang Zhimin Ao Huajie Huang Haiyan He Yuping Wu |
spellingShingle |
Quanguo Jiang Jianfeng Zhang Zhimin Ao Huajie Huang Haiyan He Yuping Wu First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene Frontiers in Chemistry graphene divacancy Mn-embedded CO oxidation first principles calculations |
author_facet |
Quanguo Jiang Jianfeng Zhang Zhimin Ao Huajie Huang Haiyan He Yuping Wu |
author_sort |
Quanguo Jiang |
title |
First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene |
title_short |
First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene |
title_full |
First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene |
title_fullStr |
First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene |
title_full_unstemmed |
First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene |
title_sort |
first principles study on the co oxidation on mn-embedded divacancy graphene |
publisher |
Frontiers Media S.A. |
series |
Frontiers in Chemistry |
issn |
2296-2646 |
publishDate |
2018-05-01 |
description |
The CO oxidation mechanism on graphene with divacancy (DG) embedded with transition metal from Sc to Zn has been studied by using first principles calculations. The results indicate that O2 molecule is preferentially adsorbed on Sc, Ti, V, Cr, Mn, and Fe-DG, which can avoid the CO poisoning problem that many catalysts facing and is beneficial to the CO oxidation progress. Further study indicates that Mn-DG shows the best catalytic properties for CO oxidation with consideration of both Langmuir-Hinshelwood (LH) and Eley-Rideal (ER) oxidation mechanisms. Along the ER mechanism, the reaction energy barrier for the first step (CO free + O2pre-adsorbed → OOCO) is 0.96 eV. Along the LH mechanism, the energy barrier for the rate limiting step (CO adsorbed + O2adsorbed → OOCO) is only 0.41 eV, indicating that the CO oxidation on Mn-DG will occur along LH mechanism. The Hirshfeld charge distributions of O2 and CO molecules is tuned by the embedded Mn atom, and the charge transfer from the embedded Mn atom to the adsorbed molecules plays an important role for the CO oxidation. The result shows that the Mn-embedded divacancy graphene is a noble-metal free and efficient catalyst for CO oxidation at low temperature. |
topic |
graphene divacancy Mn-embedded CO oxidation first principles calculations |
url |
https://www.frontiersin.org/article/10.3389/fchem.2018.00187/full |
work_keys_str_mv |
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