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2024 (English)In: ACS Physical Chemistry Au, E-ISSN 2694-2445, Vol. 5, no 1, p. 80-91Article in journal (Refereed) Published
Abstract [en]
In an effort to improve safety and cycling stability of liquid electrolytes, the use of dicarbonates has been explored. In this study, four dicarbonate structures with varying end groups and spacers are investigated. The effect of these structural differences on the physical and ion transport properties is elucidated, showing that the end group has a significant influence on ion transport. The solvation structure and ion transport in the dicarbonates are compared to those of the linear carbonates dimethyl carbonate (DMC) and diethyl carbonate (DEC). Although the carbonate coordination numbers (CN) are similar in the different systems, the CN from the anion is higher in dicarbonate electrolytes. At low salt concentrations, rapid solvent exchange is observed in the DMC- and DEC-containing systems, transitioning to a more correlated ion transport at high salt concentration. In contrast, the exchange of solvents around lithium ions (Li+) is limited in the dicarbonate systems regardless of the salt concentration, with only one carbonate group from each molecule participating in the coordination. In addition, according to the molecular dynamics simulations, Li+ mainly moves together with coordinating dicarbonate molecules and anion(s).
Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024
Keywords
alkyl dicarbonates, electrolyte, DMC, DEC, lithium ion, coordination number, end groups
National Category
Physical Chemistry Materials Chemistry Polymer Chemistry Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-555059 (URN)10.1021/acsphyschemau.4c00078 (DOI)001352432500001 ()39867447 (PubMedID)2-s2.0-85209392356 (Scopus ID)
Funder
Vinnova, 2019-00064EU, Horizon 2020, 771777Swedish Research Council, NAISS 2024/22-383Forte, Swedish Research Council for Health, Working Life and WelfareVinnova
2025-04-232025-04-232025-04-23Bibliographically approved