Solid-state polymer-particle hybrid electrolytes: Structure and electrochemical properties

Utomo, Nyalaliska W.; Hong, Shifeng; Sinha, Ritwick; Kim, Keun-il; Deng, Yue; Ochonma, Prince; Kitahata, Minori G.; Garcia-Mendez, Regina; Joo, Yong L.; Archer, Lynden A.

doi:10.1126/sciadv.ado4719

Solid-state polymer-particle hybrid electrolytes: Structure and electrochemical properties

Journal Article · Fri Jul 05 00:00:00 EDT 2024 · Science Advances

DOI:https://doi.org/10.1126/sciadv.ado4719· OSTI ID:2471850

^[1]; ^[2]; ^[2]; Kim, Keun-il ^[2]; ^[2]; ^[2]; Kitahata, Minori G. ^[2]; ^[2]; ^[2]; ^[2]

Cornell Univ., Ithaca, NY (United States); Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States)

Solid-state electrolytes (SSEs) are challenged by complex interfacial chemistry and poor ion transport through the interfaces they form with battery electrodes. Here, we investigate a class of SSE composed of micrometer-sized lithium oxide (Li₂O) particles dispersed in a polymerizable 1,3-dioxolane (DOL) liquid. Ring-opening polymerization (ROP) of the DOL by Lewis acid salts inside a battery cell produces polymer-inorganic hybrid electrolytes with gradient properties on both the particle and battery cell length scales. These electrolytes sustain stable charge-discharge behavior in Li||NCM811 and anode-free Cu||NCM811 electrochemical cells. On the particle length scale, Li₂O retards ROP, facilitating efficient ion transport in a fluid-like region near the particle surface. On battery cell length scales, gravity-assisted settling creates physical and electrochemical gradients in the hybrid electrolytes. By means of electrochemical and spectroscopic analyses, we find that Li₂O particles participate in a reversible redox reaction that increases the effective CE in anode-free cells to values approaching 100%, enhancing battery cycle life.

View Accepted Manuscript (DOE)

Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0016082

OSTI ID:: 2471850

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 27 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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