Design of Frustrated Lewis Pair Catalysts for Direct Hydrogenation of CO2. (17th October 2022)

• Record Type: Journal Article
• Authors: Das, Shubhajit; Turnell‐Ritson, Roland C.; Dyson, Paul J.; Corminboeuf, Clémence
• Is Part Of: Angewandte Chemie. Volume 134:Number 46(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-10-17
• Subjects: Boranes -- CO2 Hydrogenation -- Frustrated Lewis Pairs -- Scaling Relationships -- Volcano Plots; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202208987
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: 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. Abstract : The chemical composition of frustrated Lewis pairs is mapped to their performance in catalytic direct hydrogenation of CO2 to formate using linear scaling relationships. This map highlights the need for appropriately balancing the acidity and basicity of the components for enhanced activity, which led to the demonstration of hitherto unreported catalytic turnover for this transformation.