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Design of thiol-lithium ion interaction in metal-organic framework for high-performance quasi-solid lithium metal batteries.

Metal-organic frameworks (MOFs) have recently emerged as promising solid electrolytes (SEs) for solid-state batteries (SSBs). Developing MOFs with high-density functional groups may improve the spatial density of hopping sites and facilitate ion transport. Herein we synthesized a new series of ion conductive MOFs, Zr-MA-M (M = Li+, Na+, K+, Zn2+), with high density -SH groups functionalized in small pores and metal ions adsorbed on the thiol groups. Taking advantage of the interaction between S and metal ions, such ion conductors show high ionic conductivity, low interfacial resistance, high lithium ion (Li+) transference number (0.63) and wide electrochemical window up (4.6 V). Moreover, the SSBs assembled with Zr-MA-Li+ based SE exhibit excellent rate performance (106 mA h g-1 at 2C) and remarkable cyclic stability (low decay rate of 0.21‰ per cycle for 700 cycles at 2C). Thus, this study provides a new route for developing high-performance MOF-based SEs via the application of host-guest interaction.