Supercritical mechano-exfoliation process.

Abstract

The intricate balance among cost, output, and quality has substantially hindered the practical application of graphene within the downstream industry chain. Here we present a scalable and green supercritical CO₂-assisted mechano-exfoliation (SCME) process that omits the use of organic solvents and oxidants throughout the production lifecycle, including exfoliation, separation, and purification. The SCME process achieves graphene powder space-time yields exceeding 40 kg/(m³·day) at laboratory (0.06-0.2 kg) and pilot scales ( > 4 kg), with resultant free-standing films showing conductivities up to 5.26 × 10⁵ S/m. Further kinetic investigations propose general guidelines for grinding-assisted exfoliation: (1) the macroscopic optimizing ability of mechanotechnics for mass transfer frequency and stress distribution and (2) the microscopic multiplication ability of exfoliation medium for shear-delamination. The comprehensive techno-economic analysis also underscores the economic viability of the SCME process for large-scale production.