Inorganic-organic hybrid solid electrolytes are promising material systems for all solid-state batteries (ASSBs). These electrolytes contain numerous solid$|$solid interfaces that govern transport pathways, electrode$|$electrolyte compatibility, and durability. This paper evaluates the role that electrode$|$electrolyte interfaces and electrolyte structure have on electrochemical performance. Atomic force microscopy techniques reveal how mechanical, adhesion, and morphological properties transform in a series of model hybrid solid electrolytes. These measurements are mapped to sub-surface microstructural features using synchrotron nano-tomography. Hybrid solid electrolytes with shorter polymer chains demonstrate a higher adhesion ($>$100 nN), Young’s Modulus (6.4 GPa), capacity (114.6 mAh/g), and capacity retention (92.9%) than hybrid electrolytes with longer polymer chains (i.e., higher molecular weight). Extrinsic interfacial properties largely dictate electrochemical performance in ASSBs. Microstructural control over inorganic constituents may provide a means for tailoring interfacial properties in hybrid solid electrolytes.

无机-有机混合固体电解质是适用于所有固态电池（ASSB）的材料系统。这些电解质包含大量固体$|$固体界面决定着运输通道，电极$|$电解液的相容性和耐久性。本文评估电极的作用$|$电解质界面和电解质结构对电化学性能都有影响。原子力显微镜技术揭示了机械，附着力和形态特性如何在一系列模型混合固体电解质中转变。使用同步加速器纳米断层扫描将这些测量结果映射到亚表面微观结构特征。具有较短聚合物链的混合固体电解质表现出较高的附着力（$>$100 nN），杨氏模量（6.4 GPa），容量（114.6 mAh / g）和容量保持率（92.9％），比具有更长聚合物链（即更高分子量）的混合电解质。外在的界面性质在很大程度上决定了ASSB中的电化学性能。对无机成分的微结构控制可以提供一种用于调节混合固体电解质中的界面性质的手段。