Identifying Active Sites of Nitrogen‐Doped Carbon Materials for the CO2 Reduction Reaction |
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| Authors: | Song Liu Hongbin Yang Xiang Huang Linghui Liu Weizheng Cai Jiajian Gao Xuning Li Tao Zhang Yanqiang Huang Bin Liu |
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| Affiliation: | 1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China;2. University of Chinese Academy of Sciences, Beijing, China;3. School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, Singapore;4. School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, China |
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| Abstract: | Nitrogen‐doped carbon materials are proposed as promising electrocatalysts for the carbon dioxide reduction reaction (CRR), which is essential for renewable energy conversion and environmental remediation. Unfortunately, the unclear cognition on the CRR active site (or sites) hinders further development of high‐performance electrocatalysts. Herein, a series of 3D nitrogen‐doped graphene nanoribbon networks (N‐GRW) with tunable nitrogen dopants are designed to unravel the site‐dependent CRR activity/selectivity. The N‐GRW catalyst exhibits superior CO2 electrochemical reduction activity, reaching a specific current of 15.4 A gcatalyst?1 with CO Faradaic efficiency of 87.6% at a mild overpotential of 0.49 V. Based on X‐ray photoelectron spectroscopy measurements, it is experimentally demonstrated that the pyridinic N site in N‐GRW serves as the active site for CRR. In addition, the Gibbs free energy calculated by density functional theory further illustrates the pyridinic N as a more favorable site for the CO2 adsorption, *COOH formation, and *CO removal in CO2 reduction. |
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| Keywords: | active sites carbon dioxide reduction carbon monoxide electrocatalysts nitrogen‐doped graphene |
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