Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 38, Pages 13532-13539Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201906475
Keywords
electrocatalysis; CO2 reduction; cobalt; heterogenization; linkage effect
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Funding
- National Research Foundation (NRF), Prime Minister's Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program
- academic research fund AcRF tier 1 [M4011784 RG6/17, M4012076 RG118/18]
- Ministry of Education, Singapore [M4081887]
- College of Engineering, Nanyang Technological University
- Tender Energy Absorption Spectroscopy Beamline of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
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Immobilization of planar Co-II-2,3-naphthalocyanine (NapCo) complexes onto doped graphene resulted in a heterogeneous molecular Co electrocatalyst that was active and selective to reduce CO2 into CO in aqueous solution. A systematic study revealed that graphitic sulfoxide and carboxyl dopants of graphene were the efficient binding sites for the immobilization of NapCo through axial coordination and resulted in active Co sites for CO2 reduction. Compared to carboxyl dopants, the sulfoxide dopants further improved the electron communication between NapCo and graphene, which led to the increase of turnover frequency of the Co sites by about 3 times for CO production with a Faradic efficiency up to 97 %. Pristine NapCo in the absence of a graphene support did not display efficient electron communication with the electrode and thus failed to serve as the electrochemical active site for CO2 reduction under the identical conditions.
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