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Enhancing CO 2 Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc–Nitrogen–Carbon Tandem Catalyst
Author(s) -
Lin Long,
Liu Tianfu,
Xiao Jianping,
Li Hefei,
Wei Pengfei,
Gao Dunfeng,
Nan Bing,
Si Rui,
Wang Guoxiong,
Bao Xinhe
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202009191
Subject(s) - catalysis , cobalt , chemistry , tandem , electrochemistry , inorganic chemistry , phthalocyanine , copper , nitrogen , zinc , methane , carbon fibers , materials science , electrode , organic chemistry , composite number , composite material
Developing copper‐free catalysts for CO 2 conversion into hydrocarbons and oxygenates is highly desirable for electrochemical CO 2 reduction reaction (CO 2 RR). Herein, we report a cobalt phthalocyanine (CoPc) and zinc–nitrogen–carbon (Zn‐N‐C) tandem catalyst for CO 2 RR to CH 4 . This tandem catalyst shows a more than 100 times enhancement of the CH 4 /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 CO 2 RR 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.