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Design of Frustrated Lewis Pair Catalysts for Direct Hydrogenation of CO<sub>2</sub>

Shubhajit Das, Roland C. Turnell‐Ritson, Paul J. Dyson, Clémence Corminbœuf

2022Angewandte Chemie International Edition45 citationsDOIOpen Access PDF

Abstract

Abstract Despite recent progress in the chemistry of frustrated Lewis pairs (FLPs), direct FLP‐catalyzed hydrogenation of CO 2 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 CO 2 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.

Topics & Concepts

Frustrated Lewis pairCatalysisFormateChemistryScalingCatalytic cycleLewis acids and basesComputational chemistryCombinatorial chemistryOrganic chemistryMathematicsGeometryOrganoboron and organosilicon chemistryCarbon dioxide utilization in catalysisMetal-Organic Frameworks: Synthesis and Applications
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