Nitrogen coordinated silicon-doped graphene as a potential alternative metal-free catalyst for CO oxidation

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• 作者：Yanan Tang^a ; ^{yntang2010@163.com" class="auth_mail" title="E-mail the corresponding author} ; Weiguang Chen^a ; Zigang Shen^a ; ; Shanshan Chang^b ; Mingyu Zhao^b ; Xianqi Dai^a ; ^b ; ^{liebao100@sina.com" class="auth_mail" title="E-mail the corresponding author} ; ^{xqdaizs@163.com" class="auth_mail" title="E-mail the corresponding author}
• 刊名：Carbon
• 出版年：2017
• 出版时间：January 2017
• 年：2017
• 卷：111
• 期：Complete
• 页码：448-458
• 全文大小：2827 K

文摘

Metal-free catalysts have attracted more attention due to their highly active in catalytic oxidation reactions. The outstanding stability and catalytic activity of a single-atom Si incorporated N4 centers in graphene (Si-GN4) are investigated using first-principles calculations. It is found that the Si-GN4 configuration can be stable at high temperature, the positively charged Si dopant as the active center can effectively regulate the adsorption of reactive gases (CO and O₂). Besides, the possible reaction processes of CO oxidations on the Si-GN4 surface through the Eley−Rideal (ER) mechanism are comparably analyzed. In the CO oxidation reactions, the preadsorbed O₂ reacts with CO to form OOCO complex with smaller energy barrier (0.57 eV) than those of the formed CO₃ complex (1.08 eV) and the dissociated O₂ reaction (0.74 eV), indicating that this reaction as starting stare is an energetically more favorable process. This result indicates that the much stable Si-GN4 sheet will be a highly efficient catalyst for CO oxidation, which is comparable to that of the noble metal catalyst.