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

DOE OSTI · 2471850

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.

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Abstract

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 (Li 2 O) 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, Li 2 O 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 Li 2 O particles participate in a reversible redox reaction that increases the effective CE in anode-free cells to values approaching 100%, enhancing battery cycle life.

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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.. 2024-07-05. Solid-state polymer-particle hybrid electrolytes: Structure and electrochemical properties. https://doi.org/10.1126/sciadv.ado4719

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