Scalable Nondestructive Exfoliation of Layered Materials Into Monolayers via Shear-Transducing Interfaces

Mechanochemical exfoliation via ball milling holds great promise for scalable production of two-dimensional (2D) materials, but it is fundamentally hindered by impact-induced fragmentation and thermo-oxidative degradation during high-energy milling. Herein, we report a shear-dominated exfoliation (SDE) strategy using viscoelastic green polymer as an active energy regulator that redirects destructive impact into beneficial shear. This enables the construction of a shear-conducting interface, promoting interlayer delamination, suppressing chaotic fragmentation, and achieving in situ thermal-oxidation protection. The SDE approach achieves hundred-gram-scale monolayer fluorinated graphene (FGr) with well-preserved fluorine integrity, and demonstrates broad universality for diverse layered materials. Remarkably, the FGr affords high-rate energy densities in 25 Ah Li/CF_x cells (832.0 Wh kg^-1 at 0.1 C; 737.5 Wh kg^-1 at 0.5 C). Meanwhile, the unoxidized monolayer MXene and black phosphorus demonstrate excellent electromagnetic interference shielding and superior rate capability for Li⁺ storage. Our work bridges scalability, integrity, and green chemistry for industrial manufacturing of 2D materials.