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Identifying Active Sites of Nitrogen‐Doped Carbon Materials for the CO 2 Reduction Reaction
Author(s) -
Liu Song,
Yang Hongbin,
Huang Xiang,
Liu Linghui,
Cai Weizheng,
Gao Jiajian,
Li Xuning,
Zhang Tao,
Huang Yanqiang,
Liu Bin
Publication year - 2018
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201800499
Subject(s) - overpotential , materials science , faraday efficiency , catalysis , electrochemical reduction of carbon dioxide , electrochemistry , dopant , carbon fibers , x ray photoelectron spectroscopy , nitrogen , graphene , selectivity , active site , gibbs free energy , inorganic chemistry , doping , chemical engineering , nanotechnology , electrode , chemistry , carbon monoxide , organic chemistry , optoelectronics , composite number , composite material , physics , quantum mechanics , engineering
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 CO 2 electrochemical reduction activity, reaching a specific current of 15.4 A g catalyst −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 CO 2 adsorption, *COOH formation, and *CO removal in CO 2 reduction.