Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 42, Pages 22672-22677Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202107648
Keywords
ion transport mechanism; polyvinylidene fluoride-hexafluoropropylene; quasi-solid polymer electrolyte; spectroscopic characterization
Categories
Funding
- National Key R&D Program of China [2017YFA0206700, 2018YFB1502101]
- National Natural Science Foundation of China [22005155, 52072186, 52001170]
- 111 Project from the Ministry of Education of China [B12015]
- NCC Fund [NCC2020FH03]
- Young Elite Scientists Sponsorship Program by CAST [2019QNRC001]
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The quasi-solid polymer electrolytes features a unique structure that fully solvates Li+ ions, which helps to improve the energy density and safety of batteries.
Quasi-solid polymer electrolytes (QPE) composed of Li salts, polymer matrix, and solvent, are beneficial for improving the security and energy density of batteries. However, the ionic conduction mechanism, existential form of solvent molecules, and interactions between different components of QPE remain unclear. Here we develop a multispectral characterization strategy combined with first-principles calculations to unravel aforesaid mysteries. The results indicate that the existential state of solvent in QPE is quite different from that in liquid electrolyte. The Li cations in gel polymer electrolyte are fully solvated by partial solvent molecules to form a local high concentration of Li+, while the other solvent molecules are fastened by polymer matrix in QPE. As a result, the solvation structure and conduction mechanism of Li+ are similar to those in high-concentrated liquid electrolyte. This work provides a new insight into the ionic conduction mechanism of QPE and will promote its application for safe and high-energy batteries.
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