Nanoscale structure of a hybrid aqueous–nonaqueous electrolyte
Abstract
A new class of electrolytes have been reported, hybridizing aqueous with non-aqueous solvents, which combines non-flammability and non-toxicity characteristics of aqueous electrolytes with the superior electrochemical stability of non-aqueous systems. Here, we report measurements of the structure of an electrolyte composed of an equal-mass mixture of 21 m LiTFSI-water and 9 m LiTFSI-dimethyl carbonate using high-energy x-ray diffraction and polarized neutron diffraction with isotope substitution. Neutron structure factors from partially and fully deuterated samples exhibit peaks at low scattering vector Q that we ascribe to long-range correlations involving both solvent molecules and TFSI− anions. We compare both sets of measurements with results of molecular dynamics simulations based on a polarizable force field. The structures derived from simulations are generally in agreement with those measured, except that neutron structure factors predicted for two partially deuterated samples show very intense scattering increasing up to the low-Q limit of simulation, indicating a partial segregation between the two solvents not observed in experimental measurements.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Mar 22, 2023
- Source ID
- 10.1063/5.0138382
Entities
People
- Andrew Wildes
- B. Farago
- David L. Price
- Lucile Mangin-Thro
- Marie-Louise Saboungi
- Miguel A Gonzalez
- Oleg Borodin
- Osamu Yamamuro
- Shinji Kohara
Organizations
- Institut Laue–Langevin
- National Institute for Materials Science
- United States Department of Energy
- University of Orléans
- University of Tokyo