Green Synthesis of Thermoplastic Composites from a Terpenoid-Cellulose Ester

Herein we report a green route to thermoplastics from cellulose, the terpenoid geraniol, and fossil fuel byproduct sulfur with an overall atom economy of 90% over three steps. The only stoichiometric byproducts are NaCl and water. The process involves (1) oxidation of cellulose, (2) amino acid-catalyzed esterification, and (3) cross-linking of olefins with sulfur to give GCSx (x = wt % sulfur, varied from 80–90%). The thermoplastics exhibit flexural strengths and moduli competitive with some commercial materials and are recyclable without loss of strength. The method delineated herein should be applicable to many combinations of saccharide and terpenoid precursors to facilitate similarly green routes to a range of sustainably sourced materials.