Abstract

Solid-state lithium metal batteries have attracted broad interest as a promising energy storage technology because of the high energy density and enhanced safety that are highly desired in the markets of consumer electronics and electric vehicles. However, there are still many challenges before the practical application of the new battery. One of the major challenges is the poor interface between lithium metal electrodes and solid electrolytes, which eventually lead to the exceptionally high internal resistance of the cells and limited output. The interface issue arises largely due to the poor contact between solid and solid, and the mechanical/electrochemical instability of the interface. In this work, an in situ “welding” strategy is developed to address the interfacial issue in solid-state batteries. Microliter-level of liquid electrolyte is transformed into an organic–inorganic composite buffer layer, offering a flexible and stable interface and promoting enhanced electrochemical performance. Symmetric lithium–metal batteries with the new interface demonstrate good cycling performance for 400 h and withstand the current density of 0.4 mA cm−2. Full batteries developed with lithium–metal anode and LiFePO4 cathode also demonstrate significantly improved cycling endurance and capacity retention.

Highlights

  • The energy density of lithium-ion batteries (LIBs) has increased continually over the past 30 years, LIBs are still difficult to meet the future requirement of long endurance in energy storage and transportation (Yoshio et al, 2009; Zubi et al, 2018)

  • The front and cross-sectional of the solid-state electrolytes (SSEs) pellets in lithium metal symmetric cells after 20 cycles were characterized by field-emission scanning electron microscope (FESEM) to study the mechanism of liquid electrolytes (LEs)-optimization

  • The unique morphology could be attributed to the sintering process of the electrolyte particles during the pressing–annealing process

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Summary

INTRODUCTION

The energy density of lithium-ion batteries (LIBs) has increased continually over the past 30 years, LIBs are still difficult to meet the future requirement of long endurance in energy storage and transportation (Yoshio et al, 2009; Zubi et al, 2018). The Li2OHX (X Cl, Br, I) electrolytes possess high lithium content and a similar crystal structure to Li3OX but with higher phase stability and can be prepared from low-price starting materials (Hood et al, 2016; Li et al, 2016; Koedtruad et al, 2020; Lu et al, 2020; Deng et al, 2021; Guo et al, 2021) They have displayed remarkable chemical and electrochemical stabilities toward lithium metals even at elevated temperatures (Guo et al, 2021; Lai et al, 2021). PGSTAT 302F performed the electrochemical tests, and LAND CT 2001A performed the cycle test of the batteries at 80°C

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