Journal
ENERGY STORAGE MATERIALS
Volume 51, Issue -, Pages 19-28Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2022.06.025
Keywords
Organic; inorganic interphase; Coupling effect; Agglomeration-free structure; Enhanced interphase kinetics; All -solid -state system
Funding
- National Key Research and Develop- ment Program of China [2021YFB2500100]
- National Natural Sci- ence Foundation of China [51872196, 22109114]
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Polymer composite electrolytes have garnered attention for their safety and flexibility, but the compatibility issues at the organic/inorganic interface can lead to agglomeration of ceramic particles and hinder Li+ transport. In this study, a silane coupling agent was introduced to build a bridge model at the interface, resulting in improved dispersion, enhanced Li+ conductivity, and broader electrochemical window. The in-situ built bridge model was also applied to various cathodes, leading to uniform morphology and enhanced Li+ diffusion coefficient. These findings offer a universal strategy to address interphase issues and have implications for other composite systems.
Polymer composite electrolytes are receiving ever-increasing attention due to the favorable safety and flexibility, while inferior organic/inorganic interphase compatibility inevitably leads to serious agglomeration of ceramic particles and severely blocked Li+ transport in bulky electrolytes, especially for polymer-in-ceramic (PIC) systems with ultrahigh ceramic content. Herein, a silane coupling agent 3-Isocyanatopropyltriethoxysilane (IPTS) is introduced into PIC electrolyte to build bridge model at organic/inorganic interphase. Via in-situ coupling reaction, conventional weak physical contact between organic/inorganic components has been successfully transformed into stronger chemical interaction, resulting in homogeneous ceramic dispersion, enhanced Li+ conductivity (0.6 mS cm-1 at room temperature) and transference number (0.87) with broadened electrochemical window (5.2 V vs. Li+/Li). Moreover, the in-situ built bridge model can also be applied into various cathodes. Notably, the IPTS modified LiCoO2 (SLCO) and LiNi0.8Co0.15Al0.05O2 (SNCA) deliver uniform morphology and enhanced Li+ apparent diffusion coefficient. In this case, both all-solid-state symmetric and full cells exhibit prolonged cycling life at wide operation temperature. This work provides a universal strategy to optimize the long-ignored tough issues around the interphase for both composite electrolytes and cathodes, also enlightening other composite systems to overcome their intrinsic incompatibility.
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