Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 51, Pages 16811-16815Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201811545
Keywords
CO2 photoreduction; metal-organic frameworks (MOFs); monolayers; nickel; selectivity
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Funding
- National Natural Science Foundation of China [21836002, 21777046]
- Guangdong Innovative and Entrepreneurial Research Team Program [2016ZT06N569]
- Guangzhou Science and Technology Project [201803030002]
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Photocatalytic conversion of diluted CO2 into solar fuel is highly appealing yet still in its infancy. Herein, we demonstrate the metal-node-dependent performance for photoreduction of diluted CO2 by constructing Ni metal-organic framework (MOF) monolayers (Ni MOLs). In diluted CO2 (10%), Ni MOLs exhibit a highest apparent quantum yield of 1.96% with a CO selectivity of 96.8%, which not only exceeds reported systems in diluted CO2 but also is superior to most catalysts in pure CO2. Whereas isostructural Co MOLs is almost inactive in diluted CO2, indicating the performance is dependent on the metal nodes. Experimental and theoretical investigations show that strong CO2 binding affinity of Ni MOLs is the crucial factor, which stabilizes the Ni-CO2 adducts and facilitates CO2-to-CO conversion.
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