Design of Frustrated Lewis Pair Catalysts for Direct Hydrogenation of CO2
Dr. Shubhajit Das
Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorDr. Roland C. Turnell-Ritson
Laboratory of Organometallic and Medicinal Chemistry, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorCorresponding Author
Prof. Dr. Paul J. Dyson
Laboratory of Organometallic and Medicinal Chemistry, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorCorresponding Author
Prof. Dr. Clémence Corminboeuf
Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorDr. Shubhajit Das
Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorDr. Roland C. Turnell-Ritson
Laboratory of Organometallic and Medicinal Chemistry, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorCorresponding Author
Prof. Dr. Paul J. Dyson
Laboratory of Organometallic and Medicinal Chemistry, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorCorresponding Author
Prof. Dr. Clémence Corminboeuf
Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Federale de Lausanne, 1015 Lausanne, Switzerland
Search for more papers by this authorAbstract
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.
Open Research
Data Availability Statement
The data that support the findings of this study are openly available in zenodo at https://doi.org/10.5281/zenodo.6994552.
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