Open AccessInteractions of CO2 Anion Radicals with Electrolyte Environments from First-Principles Simulations
Author(s) -
Morgan M. Cencer,
Chenyang Li,
Garvit Agarwal,
Reginaldo Jose Gomes Neto,
Chibueze V. Amanchukwu,
Rajeev S. Assary
Publication year - 2022
Publication title -
acs omega
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.779
H-Index - 40
ISSN - 2470-1343
DOI - 10.1021/acsomega.2c01733
Subject(s) - molecular dynamics , radical , solvent , chemistry , electrolyte , aqueous solution , ion , chemical physics , molecule , computational chemistry , carbon dioxide , chemical stability , atom (system on chip) , organic chemistry , computer science , electrode , embedded system
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.