Abstract
Due to their high conductivity and interface formability, sulfide electrolytes are attractive for use in high energy density all-solid-state batteries. However, electrode volume changes during charge-discharge cycling typically cause mechanical contact losses at the electrode/electrolyte interface, which leads to capacity fading. Here, to suppress this contact loss, isolated PS43- anions are reacted with iodine to prepare a sulfide polymer electrolyte that forms a sticky gel during dispersion in anisole and drying of the resulting supernatant. This polymer, featuring flexible (–P–S–S–)n chains and enhanced solubility in anisole, is applied as a lithium-ion-conductive binder in sheet-type all-solid-state batteries, creating cells with low resistance and high capacity retention.
Highlights
Due to their high conductivity and interface formability, sulfide electrolytes are attractive for use in high energy density all-solid-state batteries
Powder X-ray diffraction (PXRD) patterns acquired after the reaction with I2 revealed the presence of LiI (PDF#01-075-5397) (Fig. 2(a)), and indicated the occurrence of Li3PS4 polymerization
The above cell featured high cycling performance (Fig. 7(c)), retaining 93.8% of its capacity between cycles 5 and 200. These results suggest that the prepared Li3PS4-I2 polymer can be used as an ion-conductive binder for sheet-type all-solid-state batteries (ASSBs)
Summary
Due to their high conductivity and interface formability, sulfide electrolytes are attractive for use in high energy density all-solid-state batteries. The improvement of existing processing technologies is vital for ASSB commercialization, with wet slurry coating recognized as a practical and scalable way of fabricating sheet-type ASSBs31 In this process, binders help to adhere the composites (containing the electrode active materials, solid electrolytes, and carbon-based conductive additives) to the current collector, make the composite sheets flexible, and allow roll-to-roll manufacturing. We demonstrated the mechanochemical and liquid-phase syntheses of the sulfide polymer This polymer was compared with previously reported structures like P2S74− to provide useful suggestions for the design of cathode/electrolyte interfaces in ASSBs and was used as a binder in sheet-type ASSBs. LiI, a by-product of the above reaction, is a Li-ion conductor[40] and can enhance the ionic conductivity of sulfide electrolytes[41,42] which suggests that sulfide polymer-LiI composites hold great promise as solid electrolytes
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