Facile, Solvent‐Free Preparation of High Density, High Mass Loading Sulfur Cathodes Enabled by Dry‐Pressable Holey Graphene Scaffolds

For lithium‐sulfur (Li−S) batteries to be practically applicable in large scale, high mass loading and high S content are required for the sulfur (S) cathodes. Most reported S cathode preparation procedures, such as melt infiltration of S into carbon scaffolds followed by conventional solvent‐based slurry casting, are time‐consuming, costly, and lack control with respect to the electrode composition and quality. Here we report the use of a facile room‐temperature procedure that is especially useful in the preparation of high density, high mass loading S cathodes with convenient control of S content and electrode architecture. The solvent‐free and binder‐free procedure is enabled by the use of holey graphene (hG) as a unique dry‐pressable electrode scaffold host to effectively encapsulate S in the conductive matrix. The entire process can be completed within just a few minutes at room temperature, in comparison to much longer time required for most other methods. With effective S utilization, the high mass loadings and high densities of the dry‐pressed hG‐hosted S cathodes result in excellent areal (up to 20 mAh/cm 2 ) and volumetric performance (1787 mAh/cm 3 is the highest reported to date), respectively. The hG‐enabled dry‐press method therefore offers an attractive processing option for S composite cathode fabrication toward practical applications.