Incorporation of Nitrogen Defects for Efficient Reduction of CO2 via Two-Electron Pathway on Three-Dimensional Graphene Foam

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• 作者：Jingjie Wu ; Mingjie Liu ; Pranav P. Sharma ; Ram Manohar Yadav ; Lulu Ma ; Yingchao Yang ; Xiaolong Zou ; Xiao-Dong Zhou ; Robert Vajtai ; Boris I. Yakobson ; Jun Lou ; Pulickel M. Ajayan
• 刊名：Nano Letters
• 出版年：2016
• 出版时间：January 13, 2016
• 年：2016
• 卷：16
• 期：1
• 页码：466-470
• 全文大小：348K
• ISSN：1530-6992

文摘

The practical recycling of carbon dioxide (CO₂) by the electrochemical reduction route requires an active, stable, and affordable catalyst system. Although noble metals such as gold and silver have been demonstrated to reduce CO₂ into carbon monoxide (CO) efficiently, they suffer from poor durability and scarcity. Here we report three-dimensional (3D) graphene foam incorporated with nitrogen defects as a metal-free catalyst for CO₂ reduction. The nitrogen-doped 3D graphene foam requires negligible onset overpotential (?0.19 V) for CO formation, and it exhibits superior activity over Au and Ag, achieving similar maximum Faradaic efficiency for CO production (～85%) at a lower overpotential (?0.47 V) and better stability for at least 5 h. The dependence of catalytic activity on N-defect structures is unraveled by systematic experimental investigations. Indeed, the density functional theory calculations confirm pyridinic N as the most active site for CO₂ reduction, consistent with experimental results.