Silicon-polymer composites in all-solid-state batteries: Interfacial chemistry, mechanical buffering, and scalable design

초록

Silicon offers an unparalleled theoretical capacity for all-solid-state batteries (ASSBs); however, its pronounced volumetric expansion and the fragility of solid-solid interfaces severely limit practical implementation. Polymers have emerged as pivotal enablers capable of reconciling these mechanical and chemical incompatibilities. This review systematically analyzes polymer-mediated strategies for stabilizing silicon anodes across sulfide-, oxide-, and polymer-based electrolytes. We categorize representative systems, including conductive polymers, elastomeric networks, self-healing chemistries, and ion-conducting polymer electrolytes, and delineate their electrolyte-dependent performance priorities in regulating interfacial chemistry, sustaining Li+ transport, and accommodating mechanical strain. Comparative evaluation reveals that conductive polymers are particularly advantageous in oxide-based architectures where electronic percolation and interfacial impedance dominate, whereas elastomeric and self-healing polymers demonstrate superior efficacy in sulfide systems by mitigating chemo-mechanical mismatch and suppressing fracture evolution. In polymer-based solid electrolytes, ionconducting matrices primarily govern lithium transport, while structural polymers stabilize electrode morphology and interphase integrity. Emphasis is placed on dynamic covalent and hydrogen-bonding networks, artificial interphase engineering, and hybrid polymer-ceramic frameworks that couple ionic conductivity with mechanical resilience. Advances in solvent-free processing and scalable roll-to-roll fabrication further highlight the translational relevance of these materials. By integrating electrochemical, interfacial, and mechanical design principles, this review establishes an electrolyte-aware framework for rationally engineering polymer-enabled silicon anodes toward durable, high-energy, and manufacturable solid-state batteries.

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