Journal
NATURE CATALYSIS
Volume 1, Issue 10, Pages 743-747Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-018-0140-3
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Funding
- US Department of Energy, Office of Science, Basic Energy Sciences, Catalysis Science Program [DE-SC0009376]
- NNSF of China [21676134, 21576129]
- US Department of Education
- Japan Society for the Promotion of Science
- Solvay
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The reduction of CO2 into formic acid or its conjugate base, using dihydrogen, is an attractive process. While catalysts based on noble metals have shown high turnover numbers, the use of abundant first-row metals is underdeveloped. The key steps of the reaction are CO2 insertion into a metal hydride and regeneration of the metal hydride with H-2, along with the concomitant production of formate. For the first step, copper is known as one of the most efficient metals, as shown by the numerous copper-catalysed carboxylation reactions, but this metal has difficulties activating H-2 to achieve the second step. Here, we report a catalytic system involving a stable copper hydride that activates CO2, working in tandem with a Lewis pair that heterolytically splits H-2. In this system, unprecedented turnover numbers for copper are obtained. Surprisingly, through a combination of stoichiometric and catalytic reactions, we show that classical Lewis pairs outperform frustrated Lewis pairs in this process.
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