2026-10-11T11:56:42Z https://api.figshare.com/v2/oai

oai:figshare.com:article/34018163 2026-09-28T18:10:46Z category_4 category_13 category_873 category_45 category_734 portal_63 item_type_6 month_year_09_2026

Competitive Coordination Decouples Charge Transport from Viscous Relaxation in Water-in-Salt Electrolytes Meron Y. Tadesse (20841031) Tarkan Ayata (25132955) Akash K Meel (25132958) Santosh Mogurampelly (1611562) Graham Leverick (6797345) Matthew J. Panzer (1475440) Venkat Ganesan (1278237) Biochemistry Genetics Chemical Sciences not elsewhere classified Sociology Biological Sciences not elsewhere classified zwitterion additives lower tune solvation structure sup >–</ sup sup >+</ sup competitive coordination provides competing coordination effects also weakening li superionic walden behavior redistributing water away strong ion correlations viscosity become governed concentrated litfsi electrolytes salt electrolytes water ion correlations concentrated electrolytes transference behavior viscous relaxation results demonstrate raman spectroscopy decoupling arises coupled transport Water-in-salt electrolytes provide wide electrochemical stability but suffer from high viscosity and strong ion correlations. Here, we examine how zwitterionic additives alter transport in concentrated LiTFSI electrolytes. Conductivity, viscosity, Raman spectroscopy, and atomistic molecular dynamics simulations show that zwitterion additives lower the absolute conductivity but shift the electrolytes from subionic to superionic Walden behavior. This decoupling arises from competing coordination effects: zwitterionic anionic groups coordinate Li⁺ and reduce its mobility, while also weakening Li⁺–TFSI^– association, promoting TFSI^––ZI⁺ contacts, and redistributing water away from TFSI^–. Consequently, conductivity and viscosity become governed by increasingly distinct molecular responses. Our results demonstrate that competitive coordination provides a route to tune solvation structure, ion correlations, transference behavior, and viscosity-coupled transport in concentrated electrolytes. 2026-09-28T00:00:00Z Text Journal contribution 10.1021/jacs.6c11585.s001 https://figshare.com/articles/journal_contribution/Competitive_Coordination_Decouples_Charge_Transport_from_Viscous_Relaxation_in_Water-in-Salt_Electrolytes/34018163 CC BY-NC 4.0