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Synthesis and Properties of Poly-Ether/Ethylene Carbonate Electrolytes with High Oxidative Stability

Journal Article · · Chemistry of Materials
New electrolyte designs are necessary for overcoming multiple challenges posed by emerging lithium-metal battery chemistries. Task-specific viscoelastic electrolytes are specifically required that are capable of simultaneously sustaining reversible electrochemistry at the Li metal anode, maintaining high oxidative stability at the battery cathode and achieving high room-temperature ionic conductivity in the electrolyte bulk. Here, we synthesize and study a series of polymeric electrolytes composed of poly-1,3-dioxolane (poly-DOL) networks formed by ring-opening polymerization of 1,3-dioxolane/ethylene carbonate (EC) mixtures by a commonly used LiPF6 electrolyte salt. The complex kinetics of the DOL polymerization reaction in EC results in nonlinear phase behavior, including the appearance of a critical transition to an entangled, solid-like electrolyte state at 40% DOL. Additionally, the transition is mediated by a range of physicochemical regimes—from liquid-like solutions to highly viscous conducting gels. We show that poly-DOL/EC electrolytes with a high concentration of the DOL precursor exhibit improved electrochemical stability compared to conventional DOL-based electrolytes, while maintaining good room temperature ionic conductivity. We show further that the EC component imparts oxidative stability, enabling their use in rechargeable, room-temperature Li||LiNi0.6Co0.2Mn0.2O2 electrochemical cells.
Research Organization:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0016082
OSTI ID:
1802831
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 20 Vol. 31; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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