Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 20, Pages 6595-6599Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201900499
Keywords
carbon nanotubes; CO2 reduction; electroreduction; grafting; porphyrin
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Funding
- National Key R&D Program of China [2018YFB0605803]
- National Natural Science Foundation of China [21576084]
- Fundamental Research Funds for the Central Universities [222201718002]
- Start-up Grant of the East China University of Science and Technology [SG1503A003]
- Start-up Grant of the City University of Hong Kong [7200600]
- CityU New Research Initiatives/Infrastructure Support from Central [APRC 9610426]
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Molecular complexes with inexpensive transition-metal centers have drawn extensive attention, as they show a high selectivity in the electrochemical conversion of CO2 to CO. In this work, we propose a new strategy to covalently graft cobalt porphyrin onto the surface of a carbon nanotube by a substitution reaction at the metal center. Material characterization and electrochemical studies reveal that the porphyrin molecules are well dispersed at a high loading of 10wt.%. As a result, the turnover frequency for CO formation is improved by a factor of three compared to traditional physically-mixed catalysts with the same cobalt content. This leads to an outstanding overall current density of 25.1mAcm(-2) and a Faradaic efficiency of 98.3% at 490mV overpotential with excellent long-term stability. This work provides an effective pathway for the improvement of the performance of electrocatalysts that could inspire rational design of molecular catalysts in the future.
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