Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 18, Pages 7615-7621Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b02997
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Funding
- National Natural Science Foundation of China [51672046, 51672047, 21403238]
- Natural Science Foundation of Fujian Province of China [2019J01226, 2019J01648]
- Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment [SKLPEE-KF 201815, SKLPEE-KF201813]
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Photocatalytic reduction of CO2 into energy-rich carbon compounds has attracted increasing attention. However, it is still a challenge to selectively and effectively convert CO2 to a desirable reaction product. Herein, we report a design of a synergistic photocatalyst for selective reduction of CO2 to CO by using a covalent organic framework bearing single Ni sites (Ni-TpBpy), in which electrons transfer from photosensitizer to Ni sites for CO production by the activated CO2 reduction under visible-light irradiation. Ni-TpBpy exhibits an excellent activity, giving a 4057 mu mol g(-1) of CO in a 5 h reaction with a 96% selectivity over H-2 evolution. More importantly, when the CO2 partial pressure was reduced to 0.1 atm, 76% selectivity for CO production is still obtained. Theoretical calculations and experimental results suggest that the promising catalytic activity and selectivity are ascribed to synergistic effects of single Ni catalytic sites and TpBpy, in which the TpBpy not only serves as a host for CO2 molecules and Ni catalytic sites but also facilitates the activation of CO2 and inhibits the competitive H-2 evolution.
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