石墨烯
催化作用
电催化剂
硝基苯
金属
选择性
氢
化学
材料科学
过渡金属
异质结
异核分子
无机化学
纳米技术
电化学
组合化学
光化学
电极
分子
物理化学
有机化学
光电子学
作者
Shiqian Chen,Hao Yuan,Sergey I. Morozov,Lei Ge,Li Li,Lai Xu,William A. Goddard
标识
DOI:10.1021/acs.jpclett.0c00642
摘要
Recently, the reduction of CO2 to fuels has been the subject of numerous studies, but the selectivity and activity remain inadequate. Progress has been made on single-site two-dimensional catalysts based on graphene coupled to a metal and nitrogen for the CO2 reduction reaction (CO2RR); however, the product is usually CO, and the metal–N environment remains ambiguous. We report a novel two-dimensional graphene nitrene heterostructure (grafiN6) providing well-defined active sites (N6) that can bind one to three metals for the CO2RR. We find that homobimetallic FeFe–grafiN6 could reduce CO2 to CH4 at −0.61 V and to CH3CH2OH at −0.68 V versus reversible hydrogen electrode, with high product selectivity. Moreover, the heteronuclear FeCu–grafiN6 system may be significantly less affected by hydrogen evolution reaction, while maintaining a low limiting potential (−0.68 V) for C1 and C2 mechanisms. Binding metals to one N6 site but not the other could promote efficient electron transport facilitating some reaction steps. This framework for single or multiple metal sites might also provide unique catalytic sites for other catalytic processes.
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