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Regulating electrochemical CO2RR selectivity at industrial current densities by structuring copper@poly(ionic liquid) interface
Li, Xiao-Qiang1,2; Duan, Guo-Yi1; Chen, Jun-Wu1,2; Han, Li-Jun1; Zhang, Suo-Jiang1,2; Xu, Bao-Hua1,2
2021-11-15
Source PublicationAPPLIED CATALYSIS B-ENVIRONMENTAL
ISSN0926-3373
Volume297Pages:13
AbstractIonic liquid-based electrocatalytic CO2 reduction faces the challenge of achieving high selectivity toward value-added C2+ products at high reaction rate (>= 100 mA cm(-2)). Herein, novel copper@poly(ionic liquid) (Cu@PIL) hybrids demonstrate multi-electron reduction (> 2e(-)) with current densities >= 300 mA cm(-2). Remarkably, Cu@PIL with F- anion exhibits high C2+ faradaic efficiency of 58 % with a high partial current density of 174 mA cm(-2). Further, a highest C2+ partial current density of 233 mA cm(-2) was also achieved. Experimental combined theoretical investigations reveal that the "individual" ionic pairs in the outer PIL layer enrich local CO2 concentration, thereby promoting the CO2 supply. Besides, an interfacial electric field is induced by the unbonded imidazolium moieties at Cu-PIL interface, which stabilize intermediates. Anions, differing in the electron-donating number to the imidazolium moieties, influence both the enrichment of CO2 and the stabilization of intermediates, thus regulating current density and product selectivity.
KeywordCO2 Utilization Value-added chemical synthesis Electrocatalysis Organic-inorganic hybrids
DOI10.1016/j.apcatb.2021.120471
Language英语
WOS KeywordX-RAY PHOTOELECTRON ; CARBON-DIOXIDE ; IONIC LIQUIDS ; POLY(IONIC LIQUIDS) ; REDUCTION ; COPPER ; ELECTROREDUCTION ; XPS ; DERIVATIVES ; ELECTRODES
Funding ProjectKey Research Program of Frontier Sciences, CAS[ZDBS-LY-JSC022] ; Excellent Young Scientists Fund[22022815] ; National Natural Science Foundation of China[U1704251] ; National Natural Science Foundation of China[21776291] ; Zhengzhou High Level Talent Certificate[20180200052]
WOS Research AreaChemistry ; Engineering
WOS SubjectChemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
Funding OrganizationKey Research Program of Frontier Sciences, CAS ; Excellent Young Scientists Fund ; National Natural Science Foundation of China ; Zhengzhou High Level Talent Certificate
WOS IDWOS:000696992600001
PublisherELSEVIER
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Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/50232
Collection中国科学院过程工程研究所
Corresponding AuthorXu, Bao-Hua
Affiliation1.Chinese Acad Sci, Inst Proc Engn, Beijing Key Lab Ion Liquids Clean Proc, CAS Key Lab Green Proc & Engn,State Key Lab Multi, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Coll Chem & Chem Engn, Beijing 100049, Peoples R China
Recommended Citation
GB/T 7714
Li, Xiao-Qiang,Duan, Guo-Yi,Chen, Jun-Wu,et al. Regulating electrochemical CO2RR selectivity at industrial current densities by structuring copper@poly(ionic liquid) interface[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2021,297:13.
APA Li, Xiao-Qiang,Duan, Guo-Yi,Chen, Jun-Wu,Han, Li-Jun,Zhang, Suo-Jiang,&Xu, Bao-Hua.(2021).Regulating electrochemical CO2RR selectivity at industrial current densities by structuring copper@poly(ionic liquid) interface.APPLIED CATALYSIS B-ENVIRONMENTAL,297,13.
MLA Li, Xiao-Qiang,et al."Regulating electrochemical CO2RR selectivity at industrial current densities by structuring copper@poly(ionic liquid) interface".APPLIED CATALYSIS B-ENVIRONMENTAL 297(2021):13.
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