Interactions of CO 2 Anion Radicals with Electrolyte Environments from First-Principles Simulations.

Autor: Cencer MM; Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Li C; Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Agarwal G; Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Gomes Neto RJ; Pritzker School of Molecular Engineering, The University of Chicago, Chicago, Illinois 60637, United States., Amanchukwu CV; Pritzker School of Molecular Engineering, The University of Chicago, Chicago, Illinois 60637, United States.; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Assary RS; Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States.
Jazyk: angličtina
Zdroj: ACS omega [ACS Omega] 2022 May 17; Vol. 7 (21), pp. 18131-18138. Date of Electronic Publication: 2022 May 17 (Print Publication: 2022).
DOI: 10.1021/acsomega.2c01733
Abstrakt: Successful transformation of carbon dioxide (CO 2 ) into value-added products is of great interest, as it contributes in part to the circular carbon economy. Understanding chemical interactions that stabilize crucial reaction intermediates of CO 2 is important, and in this contribution, we employ atom centered density matrix propagation (ADMP) molecular dynamics simulations to investigate interactions between CO 2 - anion radicals with surrounding solvent molecules and electrolyte cations in both aqueous and nonaqueous environments. We show how different cations and solvents affect the stability of the CO 2 - anion radical by examining its angle and distance to a coordinating cation in molecular dynamics simulations. We identify that the strength of CO 2 - interactions can be tailored through choosing an appropriate cation and solvent combination. We anticipate that this fundamental understanding of cation/solvent interactions can facilitate the optimization of a chemical pathway that results from selective stabilization of a crucial reaction intermediate.
Competing Interests: The authors declare no competing financial interest.
(© 2022 Chicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society.)
Databáze: MEDLINE
Externí odkaz: