期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 46, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202208987
关键词
Boranes; CO2 Hydrogenation; Frustrated Lewis Pairs; Scaling Relationships; Volcano Plots
资金
- GAZNAT
Despite recent progress in the chemistry of frustrated Lewis pairs (FLPs), direct FLP-catalyzed hydrogenation of CO2 remains elusive. The authors propose a mapping method to link the chemical composition of FLPs with their activity in catalytic hydrogenation of CO2, and they experimentally validate a combination with high catalytic turnover.
Despite recent progress in the chemistry of frustrated Lewis pairs (FLPs), direct FLP-catalyzed hydrogenation of CO2 remains elusive. From a near-infinite array of plausible Lewis pairs, it is challenging to identify individual combinations that are appropriate for catalyzing this reaction. To this end, we propose a mapping of the chemical composition of FLPs to their activity towards direct catalytic hydrogenation of CO2 into formate. The maps, built upon linear scaling relationships, pinpoint specific FLP combinations with the proper complementary acidity and basicity to optimally balance the energetics of the catalytic cycle. One such combination was experimentally validated to achieve hitherto unreported catalytic turnover for this transformation.
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