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Kinetics of Hydride Transfer from Catalytic Metal-Free Hydride Donors to CO2

Selective reduction of CO2 to formate represents an ongoing challenge in photoelectrocatalysis. To provide mechanistic insights, we investigate the kinetics of hydride transfer (HT) from a series of metal-free hydride donors to CO2. The observed dependence of experimental and calculated HT barriers...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2021-03, Vol.12 (9), p.2306-2311
Main Authors: Weerasooriya, Ravindra B, Gesiorski, Jonathan L, Alherz, Abdulaziz, Ilic, Stefan, Hargenrader, George N, Musgrave, Charles B, Glusac, Ksenija D
Format: Article
Language:English
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Summary:Selective reduction of CO2 to formate represents an ongoing challenge in photoelectrocatalysis. To provide mechanistic insights, we investigate the kinetics of hydride transfer (HT) from a series of metal-free hydride donors to CO2. The observed dependence of experimental and calculated HT barriers on the thermodynamic driving force was modeled by using the Marcus hydride transfer formalism to obtain the insights into the effect of reorganization energies on the reaction kinetics. Our results indicate that even if the most ideal hydride donor were discovered, the HT to CO2 would exhibit sluggish kinetics (
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.0c03662