Localized high-concentration electrolytes get more localized through micelle-like structures.

Autor: Efaw CM; Energy and Environmental Science and Technology Directorate, Idaho National Laboratory, Idaho Falls, ID, USA.; Micron School of Materials Science and Engineering, Boise State University, Boise, ID, USA., Wu Q; School of Engineering, Brown University, Providence, RI, USA., Gao N; Energy and Environmental Science and Technology Directorate, Idaho National Laboratory, Idaho Falls, ID, USA., Zhang Y; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, USA., Zhu H; Micron School of Materials Science and Engineering, Boise State University, Boise, ID, USA., Gering K; Energy and Environmental Science and Technology Directorate, Idaho National Laboratory, Idaho Falls, ID, USA., Hurley MF; Micron School of Materials Science and Engineering, Boise State University, Boise, ID, USA., Xiong H; Micron School of Materials Science and Engineering, Boise State University, Boise, ID, USA., Hu E; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA., Cao X; Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA., Xu W; Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA., Zhang JG; Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA., Dufek EJ; Energy and Environmental Science and Technology Directorate, Idaho National Laboratory, Idaho Falls, ID, USA., Xiao J; Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA.; Materials Science and Engineering Department, University of Washington, Seattle, WA, USA., Yang XQ; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA., Liu J; Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA.; Materials Science and Engineering Department, University of Washington, Seattle, WA, USA., Qi Y; School of Engineering, Brown University, Providence, RI, USA. yueqi@brown.edu., Li B; Energy and Environmental Science and Technology Directorate, Idaho National Laboratory, Idaho Falls, ID, USA. lib2@ornl.gov.; Micron School of Materials Science and Engineering, Boise State University, Boise, ID, USA. lib2@ornl.gov.; Energy Science and Technology Directorate, Oak Ridge National Laboratory, Oak Ridge, TN, USA. lib2@ornl.gov.
Jazyk: angličtina
Zdroj: Nature materials [Nat Mater] 2023 Dec; Vol. 22 (12), pp. 1531-1539. Date of Electronic Publication: 2023 Nov 06.
DOI: 10.1038/s41563-023-01700-3
Abstrakt: Liquid electrolytes in batteries are typically treated as macroscopically homogeneous ionic transport media despite having a complex chemical composition and atomistic solvation structures, leaving a knowledge gap of the microstructural characteristics. Here, we reveal a unique micelle-like structure in a localized high-concentration electrolyte, in which the solvent acts as a surfactant between an insoluble salt in a diluent. The miscibility of the solvent with the diluent and simultaneous solubility of the salt results in a micelle-like structure with a smeared interface and an increased salt concentration at the centre of the salt-solvent clusters that extends the salt solubility. These intermingling miscibility effects have temperature dependencies, wherein a typical localized high-concentration electrolyte peaks in localized cluster salt concentration near room temperature and is used to form a stable solid-electrolyte interphase on a Li metal anode. These findings serve as a guide to predicting a stable ternary phase diagram and connecting the electrolyte microstructure with electrolyte formulation and formation protocols of solid-electrolyte interphases for enhanced battery cyclability.
(© 2023. The Author(s), under exclusive licence to Springer Nature Limited.)
Databáze: MEDLINE