Via the first principles calculations, we predict that Cu doped graphene oxide (GO) is a much better nanocatalyst in terms of activity and feasibility. The high activity of Cu doped graphene oxides may be attributed to the charge transfer between the GO and Cu atom, resulting in an activated Cu atom. In the ER mechanism, the CO molecules directly react with the activated O2, then forming a metastable carbonate-like intermediate state (OOCO). The reaction may proceed via two reaction paths of OOCO → CO2 + O and CO + OOCO → 2CO2, respectively. The calculated results show that the latter path is relatively more thermodynamically favorable with a modest energy barrier, so it should be more preferred. We expect our theoretical predictions to open a new avenue to fabricate carbon-based catalysts for CO oxidation with lower cost and higher activity.
Abstract：Via the first principles calculations, we predict that Cu doped graphene oxide (GO) is a much better nanocatalyst in terms of activity and feasibility. The high activity of Cu doped graphene oxides may be attributed to the charge transfer between the GO and Cu atom, resulting in an activated Cu atom. In the ER mechanism, the CO molecules directly react with the activated O2, then forming a metastable carbonate-like intermediate state (OOCO). The reaction may proceed via two reaction paths of OOCO → CO2 + O and CO + OOCO → 2CO2, respectively. The calculated results show that the latter path is relatively more thermodynamically favorable with a modest energy barrier, so it should be more preferred. We expect our theoretical predictions to open a new avenue to fabricate carbon-based catalysts for CO oxidation with lower cost and higher activity.
This project was supported by the National Natural Science Foundation of China (No. 21004009) and the Foundation of Jiangxi Educational Committee (No. GJJ14485)
通讯作者:
黄斌
E-mail: binhuang@xmu.edu.cn
引用本文:
黄斌;辛育东;陈荣. CO Catalytic Oxide over Cu Atom Supported on Graphene Oxides from the First Principles[J]. 结构化学, 2015, 34(4): 624-631.
HUANG Bin;XIN Yu-Dong;CHEN Rong. CO Catalytic Oxide over Cu Atom Supported on Graphene Oxides from the First Principles. CHINESE JOURNAL OF STRUCTURAL CHEMISTRY, 2015, 34(4): 624-631.
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