Universal F4-modified Strategy on Metal Organic Framework to Chemical Stabilize Pvdf-Hfp as Quasi-Solid-State Electrolyte

Solid-state electrolytes (SSEs) based on metal organic framework (MOF) and polymer mixed matrix membranes (MMMs) have shown great promotions in both lithium-ion conduction and interfacial resistance in lithium metal batteries (LMBs). However, the unwanted structural evolution and the and the obscure electrochemical reaction mechanism among two phases limit their further optimization and commercial application. Herein, fluorine-modified zirconium MOF with diverse F-quantities is synthesized, denoted as Zr-BDC-Fx (x = 0, 2, 4), to assemble high performance quais-solid-state electrolytes (QSSEs) with PVDF-HFP. The chemical complexation of F-sites in Zr-BDC-F4 stabilized PVDF-HFP chains in β-phase and disordered oscillation with enhanced charge transfer and Li transmit property. Besides, the porous confinement and electronegativity of F-groups enhanced the capture and dissociation of TFSI- anions and the homogeneous deposition of LiF solid electrolyte interphase (SEI), promoting the high-efficient transport of Li+ ions and inhibiting the growth of Li dendrites. The superb specific capacities in high-loaded Li.

This work received financial support from National Natural Science Foundation of China (22001156, 22271178), International Cooperation Key Project of Science and Technology Department of Shaanxi, China (2022KWZ-06), the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province (20210602), Research project of Xi'an Science and Technology Bureau (2022GXFW0011), and Science and Technology New Star in Shaanxi Province (2023KJXX-045). Shaanxi Provincial Department of Education service local special project, industrialization cultivation project (23JC007).


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