Journal
NATURE CATALYSIS
Volume 2, Issue 8, Pages 709-717Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-019-0308-5
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Funding
- Ministry of Science and Technology of China [2016YFA0200702]
- National Natural Science Foundation of China [21671162, 21471126, 21721001]
- US DOE [DE-AC02-06CH11357]
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Selective conversion of CO2 to ethanol is of great interest but presents a significant challenge in forming a C-C bond while keeping a C-O bond intact throughout the process. Here, we report cooperative Cu-I sites on a Zr-12 cluster of a metal-organic framework (MOF) for selective hydrogenation of CO2 to ethanol. With the assistance of an alkali cation, the spatially proximate Zr-12-supported Cu-I centres activate hydrogen via bimetallic oxidative addition and promote C-C coupling to produce ethanol. The Cs+-modified MOF catalyst, in 10 hours, produces ethanol with >99% selectivity and a turnover number (based on all Cu atoms) of 4,080 in supercritical CO2, with 30 MPa of CO2 and 5 MPa of H-2 at 85 degrees C, or a turnover number of 490 at 2 MPa of CO2/H-2 (1/3) and 100 degrees C. Our work highlights the potential of using MOFs as a tunable platform to design earth-abundant metal catalysts for CO2 conversion.
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