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Enhancing CO(2)Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc-Nitrogen-Carbon Tandem Catalyst
Lin, L; Liu, TF; Xiao, JP; Li, HF; Wei, PF; Gao, DF; Nan, B; Si, R; Wang, GX; Bao, XH
2020
Source PublicationANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN1433-7851
Volume59Issue:50Pages:22408-22413
Subtype期刊论文
AbstractDeveloping copper-free catalysts for CO(2)conversion into hydrocarbons and oxygenates is highly desirable for electrochemical CO(2)reduction reaction (CO2RR). Herein, we report a cobalt phthalocyanine (CoPc) and zinc-nitrogen-carbon (Zn-N-C) tandem catalyst for CO2RR to CH4. This tandem catalyst shows a more than 100 times enhancement of the CH4/CO production rate ratio compared with CoPc or Zn-N-C alone. Density functional theory (DFT) calculations and electrochemical CO reduction reaction results suggest that CO(2)is first reduced into CO over CoPc and then CO diffuses onto Zn-N-C for further conversion into CH(4)over Zn-N(4)site, decoupling complicated CO2RR pathway on single active site into a two-step tandem reaction. Moreover, mechanistic analysis indicates that CoPc not only generates CO but also enhances the availability of *H over adjacent N sites in Zn-N-4, which is the key to achieve the high CH(4)production rate and understand the intriguing electrocatalytic behavior which is distinctive to copper-based tandem catalysts.
KeywordSINGLE-ATOM CATALYSTS CO2 REDUCTION ELECTROCHEMICAL REDUCTION DIOXIDE REDUCTION ELECTROREDUCTION SITES ELECTROCATALYSTS OXYGEN
DOI10.1002/anie.202009191
Indexed BySCI ; EI
Language英语
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/32859
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100039, Peoples R China
3.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
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GB/T 7714
Lin, L,Liu, TF,Xiao, JP,et al. Enhancing CO(2)Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc-Nitrogen-Carbon Tandem Catalyst[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59(50):22408-22413.
APA Lin, L.,Liu, TF.,Xiao, JP.,Li, HF.,Wei, PF.,...&Bao, XH.(2020).Enhancing CO(2)Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc-Nitrogen-Carbon Tandem Catalyst.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59(50),22408-22413.
MLA Lin, L,et al."Enhancing CO(2)Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc-Nitrogen-Carbon Tandem Catalyst".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59.50(2020):22408-22413.
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