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Constructing FeN4/graphitic nitrogen atomic interface for high-efficiency electrochemical CO2 reduction over a broad potential window
Liu, Chuhao1; Wu, Yue1; Sun, Kaian1; Fang, Jinjie2; Huang, Aijian1,3; Pan, Yuan4; Cheong, Weng Chon5; Zhuang, Zewen1; Zhuang, Zhongbin2; Yuan, Qiuhua6; Xin, Huolin L.7; Zhang, Chao8; Zhang, Jiangwei9; Xiao, Hai1; Chen, Chen1; Li, Yadong1
2021-05-13
Source PublicationChem
ISSN2451-9308
Volume7Issue:5Pages:1297-1307
Abstract

Atomically dispersed Fe–N–C catalyst has shown great performance in the CO-to-CO conversion, yet the high CO selectivity is achieved only within a rather narrow potential range, which cannot well meet the requirements for the following CO dimerization or hydrogenation. Here, we developed a hydrogen-pyrolysis etching strategy to precisely manipulate the uncoordinated N dopants in the Fe–N–C catalyst. This strategy could preferentially eliminate pyridinic and pyrrolic N atoms while leaving graphitic N. The resulting catalyst gave a CO faradaic efficiency (FE) above 90% over a broad window from −0.3 to −0.8 V (versus RHE) (in particular, FE > 97% at −0.6 V). In situ ATR-SEIRAS and first-principle calculations further revealed that this strategy can not only suppress the parasitic H generation but also promote CO activation and protonation with the assistance of co-adsorbed HO on the “atomic interface” of “FeN/graphitic N.”

KeywordAtomic Interface Electrochemical Reduction Of Co2 Fen4/graphitic n Hydrogen-pyrolysis Etching Sdg7: Affordable And Clean Energy
DOI10.1016/j.chempr.2021.02.001
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaChemistry
WOS IDWOS:000652330400014
Scopus ID2-s2.0-85103090616
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Cited Times [WOS]:8   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
CollectionDEPARTMENT OF PHYSICS AND CHEMISTRY
Corresponding AuthorZhang, Jiangwei; Chen, Chen
Affiliation1.Department of Chemistry, Tsinghua University, Beijing, 100084, China
2.Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China
3.School of Electronics Science and Engineering, Center for Public Security Technology, University of Electronic Science and Technology of China, Chengdu, 610054, China
4.State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580, China
5.Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao, China
6.College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060, China
7.Department of Physics and Astronomy, University of California Irvine, 94720, United States
8.Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering, Tianjin University of Technology, Tianjin, 300384, China
9.Dalian National Laboratory for Clean Energy & State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences (CAS), Dalian, 116023, China
Recommended Citation
GB/T 7714
Liu, Chuhao,Wu, Yue,Sun, Kaian,et al. Constructing FeN4/graphitic nitrogen atomic interface for high-efficiency electrochemical CO2 reduction over a broad potential window[J]. Chem,2021,7(5):1297-1307.
APA Liu, Chuhao,Wu, Yue,Sun, Kaian,Fang, Jinjie,Huang, Aijian,Pan, Yuan,Cheong, Weng Chon,Zhuang, Zewen,Zhuang, Zhongbin,Yuan, Qiuhua,Xin, Huolin L.,Zhang, Chao,Zhang, Jiangwei,Xiao, Hai,Chen, Chen,&Li, Yadong.(2021).Constructing FeN4/graphitic nitrogen atomic interface for high-efficiency electrochemical CO2 reduction over a broad potential window.Chem,7(5),1297-1307.
MLA Liu, Chuhao,et al."Constructing FeN4/graphitic nitrogen atomic interface for high-efficiency electrochemical CO2 reduction over a broad potential window".Chem 7.5(2021):1297-1307.
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