Revealing the effect of double bond-modified Li6.75La3Zr1.75Ta0.25O12 on the Li-ion conduction of composite solid electrolytes

Lithium metal batteries with polyethylene oxide (PEO) electrolytes have shown great potential to be one of the next-generation energy candidates. As the branch family of PEO electrolytes, poly(ethylene glycol) acrylates (PEGAs) attract more attention owing to their better electrochemical properties than that of PEO electrolytes. Introducing double bond-modified Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 fillers (KH@LLZTO) has been a popular method to improve the electrochemical properties of PEGAs electrolytes due to the homogeneous dispersion of LLZTO. However, in this work, an inverse phenomenon is discovered. The electrochemical properties of PEGAs electrolytes get worse when introducing KH@LLZTO. By exploring the Li + transport mechanism, the reason for the inverse phenomenon is revealed. More importantly, the design principle of PEGAs electrolytes with fast ionic conductor fillers is presented. Double bond-modified LLZTO can decrease the electrochemical properties of PEGAs electrolytes instead when there are low-molecular weight monomers that can participate in the PEGAs polymer network and interact with Li + , while the double bond-modified LLZTO can improve the electrochemical properties of PEGAs electrolytes when there are not aforementioned low-molecular weight monomers. This work provides a new understanding for componential design and optimization of PEGAs electrolytes with fast ionic conductors, hoping to promote the practical application of PEGAs electrolytes.