Enable Superior Performance of Solvent‐Free Electrode With Ultra‐High Loading Through Designed Conductive Binder

Abstract Compared to the traditional slurry‐coating process, the solvent‐free manufacturing process holds significant potential due to its advantages, including economic viability, thick electrodes, and avoidance of organic solvents. However, the currently dominant solvent‐free process suffers from poor mechanical properties and electrochemical instability. Herein, a conductive binder (M@EP), composed of multi‐walled carbon nanotubes (MWNT) and epoxy resin‐based binders (EP), is designed and synthesized. The functional integration of the conductive agent and binder facilitates the formation of a 3D percolation network, significantly enhancing the conductivity of electrode. The abundant ether oxygen groups and nitrogen elements in EP promote the transmission of Li⁺ ions. Consequently, the dry electrodes exhibit outstanding cycling performance and rate capability. Furthermore, the combined enhancement of electronic and ionic conductivity enables the manufacturing of high‐loading dry electrodes (HDEs‐M@EP). The HDEs‐M@EP (485 µm) have a maximum areal mass loading of 110.88 mg cm⁻², and the corresponding areal capacity reaches 20.19 mAh cm⁻². Finally, the structural design of M@EP facilitates an innovative method for the rapid recycling and reuse of spent batteries. It greatly simplifies the traditional procedure and enables the recycling of all types of electrode materials, offering new insights for future large‐scale industrial recycling methods and green recycling systems.