A Solvent‐Free, Dry‐Processed Li‐Ion Battery Enabled by Dual Binders and Nanostructured Aluminum Current Collectors

Abstract Conventional dry‐processed electrode (DPE) fabrication using polytetrafluoroethylene (PTFE) or polyvinylidene fluoride (PVDF) offers a solvent‐free alternative to wet‐coating processes that rely on toxic N ‐methyl‐2‐pyrrolidone. However, traditional DPE systems often struggle with a trade‐off between internal cohesion and interfacial adhesion, limiting electrode integrity and electrochemical performance under high‐loading conditions. Herein, an advanced dual‐binder DPE (DB‐DPE) architecture that integrates PTFE and PVDF with a nanostructured aluminum current collector (NSA) is presented. This synergistic system leverages PTFE's fibrillation‐induced cohesion and PVDF's adhesive strength, while the NSA's nanoporous morphology enables robust mechanical interlocking at the electrode–collector interface. The resulting electrodes, fabricated with an ultrahigh active material content of 96 wt.% and minimal binder content of 2 wt.%, exhibit reduced interfacial resistance, excellent mechanical integrity, and enhanced ionic and electronic conductivity. This architecture enables the fabrication of high‐mass‐loading cathodes (up to 64 mg cm −2 , 12.5 mAh cm −2 ) with superior performance, achieving a high volumetric energy density of 712.7 Wh L −1 .