In‐Situ Crosslinkable Graphite for Mechanically Robust Dry‐Processed Lithium‐Ion Battery Electrodes

The carbon footprint of lithium‐ion battery (LIB) manufacturing is an emerging concern with the rapid expansion of LIBs into electric vehicles and large‐scale energy storage systems. In this context, dry electrode processing, enabled by polytetrafluoroethylene (PTFE) binders, offers a solvent‐free, energy‐efficient alternative to conventional slurry‐based fabrication methods. Moreover, the unique fibril morphology of PTFE supports high‐mass‐loading electrodes without sacrificing ion transport or rate capability. However, PTFE's low intrinsic adhesion compromises the mechanical integrity of dry‐processed electrodes, hindering practical application. Herein, we introduce a surface modification strategy based on polydopamine–poly(acrylic acid) coatings on graphite, enabling in‐situ crosslinking during dry‐processed electrode fabrication. This approach enhances the electrode adhesion strength without degrading electrochemical performance. The crosslinked electrodes exhibit superior mechanical stability and retain 87.1% of their initial capacity after 500 cycles at 1 C (4.3 mA cm −2 ), demonstrating a scalable route to robust, high‐performance dry‐processed electrodes.