Abstract
Spherical carbon particles are versatile products that are of interest in polymer modification and scaffolding, catalysis, and energy storage applications. Despite various complex synthesis methods available currently, there is a need for simplified synthesis techniques to develop spherical carbon particles from sustainable feedstock. Here, we report a simple method for manufacturing micronized carbon particles from lignin, a plant biomass derived phenolic oligomer. By careful selection of a good, high boiling solvent that can fully solvate and stabilize lignin, we were able to create spherical free-flowing carbon particles from lignin by a simple solvothermal process and subsequent carbonization. During solvothermal reaction, lignin degrades into fragments via its thermally sensitive bonds. Simultaneously, the residual lignin and its fragments repolymerize, condense into highly cross-linked structures, and eventually precipitate out of solution with a spherical shape. Infrared and NMR spectroscopy data in combination with the rheological properties of thermally condensed, solvated oligomer elucidate evolution in the chemical architecture of lignin. The coarse-grained molecular dynamics simulations revealed the growth of spherical char from lignin in a good solvent through intermolecular condensation. X-ray diffraction and electron microscopy data show the morphology of the carbonized product—an increase in the carbonization temperature enhances the structural order.