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Impact of Interfacial Electron Transfer on Electrochemical CO 2 Reduction on Graphitic Carbon Nitride/Doped Graphene
Author(s) -
Zhi Xing,
Jiao Yan,
Zheng Yao,
Qiao ShiZhang
Publication year - 2019
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.201804224
Subject(s) - overpotential , electron transfer , graphene , catalysis , materials science , graphitic carbon nitride , heteroatom , electrochemistry , doping , adsorption , carbon fibers , carbon nitride , chemical engineering , nanotechnology , electrode , chemistry , photocatalysis , optoelectronics , composite material , organic chemistry , composite number , ring (chemistry) , engineering
Effective electrocatalysts are required for the CO 2 reduction reaction (CRR), while the factors that can impact their catalytic activity are yet to be discovered. In this article, graphitic carbon nitride (g‐C 3 N 4 ) is used to investigate the feasibility of regulating its CRR catalytic performance by interfacial electron transfer. A series of g‐C 3 N 4 /graphene with and without heteroatom doping (C 3 N 4 /XG, XG = BG, NG, OG, PG, G) is comprehensively evaluated for CRR through computational methods. Variable adsorption energetics and electronic structures are observed among different doping cases, demonstrating that a higher catalytic activity originates from more interfacial electron transfer. An activity trend is obtained to show the best catalytic performance of CRR to methane on C 3 N 4 /XG with an overpotential of 0.45 V (i.e., −0.28 V vs reverse hydrogen electrode [RHE]). Such a low overpotential has never been achieved on any previously reported metallic CRR electrocatalysts, therefore indicating the availability of C 3 N 4 /XG for CO 2 reduction and the applicability of electron transfer modulation to improve CRR catalytic performance.