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

• Published in: Dalton transactions : an international journal of inorganic chemistry Vol. 5; no. 8; pp. 2928 - 2935
• Main Authors: Zhang, Qi, Xiao, Yingbo, Li, Qi, Wang, Jia, Guo, Sijia, Li, Xin, Ouyang, Yuan, Zeng, Qinghan, He, Wenchao, Huang, Shaoming
• Format: Journal Article
• Language: English
• Published: England Royal Society of Chemistry 02.03.2021
• Subjects: Chemical synthesis; Conductors; Decay rate; Functional groups; Ion currents; Ion transport; Ions; Lithium; Lithium ions; Metal ions; Metal-organic frameworks; Molten salt electrolytes; Rechargeable batteries; Solid electrolytes; Zirconium
• ISSN: 1477-9226; 1477-9234
• DOI: 10.1039/d0dt03336g

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 + , Zn 2+ ), 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. A metal-organic framework (Zr-MA) was designed to serve as high-performance solid electrolyte in quasi-solid lithium metal batteries. Both the high-density thiol groups and narrow channels in framework contributed to the improved ion transport.