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Reduction of CO~2~ with Hydrated Electrons: Ab Initio Computational Studies for Finite-Size Cluster Models by Sebastian Pios; Wolfgang Domcke is a Chemistry article available to read on EtoBox.

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In the present work, the mechanisms of the reduction of the CO 2 molecule with hydrated electrons to the hydroxyl-formyl (HOCO) radical were studied with ab initio computational methods. Hydrated hydronium radicals, H 3 O-(H 2 O) n (n = 0,3,6), are considered as finite-size models of the hydrated electron in liquid water. The investigation of cluster models allows the application of high-accuracy electronic-structure methods, which are not computationally feasible in condensedphase simulations. Reaction paths and potential-energy (PE) profiles of the proton-coupled electron-transfer reaction from hydrated H 3 O radicals to the CO 2 molecule were explored on the ground-state PE surface. The computationally efficient unrestricted second-order Møller−Plesset method is employed, and its accuracy has been carefully benchmarked in comparison with complete-active-space self-consistent-field and multi-reference second-order perturbation calculations. The results provide insights into the interplay of electron transfer from the diffuse Rydberg-type unpaired electron of H 3 O to the CO 2 molecule, the contraction of the electron cloud by the re-hybridization of the carbon atom of CO 2 , and

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Author

Sebastian Pios; Wolfgang Domcke

Publisher

American Chemical Society (ACS)

Published

2023

Language

EN

Field

Chemistry (Physical Sciences)