Graphical Closed borders : A Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) ceramic is adopted to block the migration of polysulfides in Li−S batteries, with solvent-in-salt wetting the electrode/ceramic interfaces. Owing to suppressed dissolution of polysulfides in SIS, the semi-solid-state Li−S batteries show superior capacity retention and long cycling life. Aimed at tackling the shuttle effect in lithium-sulfur (Li−S) batteries, a Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) ceramic is adopted to block the migration of polysulfides. However, the LAGP-based Li−S battery with liquid electrolyte wetting the interfaces still suffers from rapid capacity decay, as polysulfides tend to dissolve into liquid electrolyte and get firmly adsorbed by LAGP. In this work, a dual confinement effect for polysulfides is put forward, enabled by the LAGP ceramic and solvent-in-salt (SIS), wherein the SIS can greatly suppress the dissolution of polysulfides. Owing to the synergistic effect of SIS and LAGP, the semi-solid-state Li−S batteries show superior capacity retention and long cycling life. In particular, at a current density of 0.2 C, the Li−S battery with SIS-modified LAGP ceramic electrolyte delivers a high initial reversible capacity of 1251.7 mAh g −1 and long cycle life of over 250 cycles with a decay rate of only 0.07 % per cycle.
The fossil fuel crisis and global warming are becoming more and more severe in this century, while the exploration of human survival on Mars is being pushed forward steadily. Hence, it is meaningful to effectively utilize CO2, the main greenhouse gas and a major component of the Martian atmosphere. Due to their high capacity and ability to capture CO2, Li–CO2 batteries have received much attention. However, there are problems that still need to be solved relating to Li–CO2 batteries, including the instability of the electrolyte and the non-negligible polarization caused by the formation and decomposition of Li2CO3. To address these issues, an all-solid-state Li–CO2 battery, which uses RuO2 nanoparticles combined with single-walled carbon nanotubes (SWCNTs) as the cathode material and a sodium super ionic conductor (NASICON)-type ceramic solid electrolyte, Li1.5Al0.5Ge1.5(PO4)3 (LAGP), has been developed and it operates over a broad temperature range. Under a pure CO2 atmosphere, this well-designed battery shows a discharge capacity of 2499 mA h g−1 and a charge capacity of 2137 mA h g−1 in the first cycle at 60 °C, and stable cycling performance over 30 cycles under a capacity limitation of 500 mA h g−1 at a current density of 50 mA g−1. This result enhances the possibility of the utilization of the Li–CO2 battery in the future.
A ceramic solid electrolyte of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) with high ionic conductivity (4.28 × 10 −4 S cm −1 at 30 °C) and low activation energy (0.25 eV) is prepared by a three-step method, and the interfacial properties of the ceramic solid electrolyte are further modified by an in-situ polymerization strategy with the formation of a gel-polymer electrolyte with the thickness of 8.85 μm on the surface of LAGP. The presence of the gel-polymer electrolyte on the surface of LAGP inhibits the side reactions and the growth of lithium dendrites, as evidenced by the stable cycling of the lithium symmetric cells with the modified LAGP solid electrolyte for 1000 h at 25 °C. In addition, the high ionic conductivity and the stable interface of the modified LAGP solid electrolyte enable the solid-state lithium battery with a LiFePO 4 cathode, exhibiting superior electrochemical performances which can run stably at 25 °C with initial discharge specific capacity of 159.8 mAh g −1 at 0.1C.
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