Integrated, cascading enzyme-/chemocatalytic cellulose conversion using catalysts based on mesoporous silica nanoparticles.

Abstract

This article reports a novel approach to deconstructing cellulose into 5-hydroxymethylfurfural (HMF) with a high yield (46.1%) by integrating a sequential enzyme cascade technique in an aqueous system with solid acid catalysis in an organic-solvent system. We executed the rational design and synthesis of mesoporous silica nanoparticles (MSNs) with various pore sizes and surface functionalities, which proved to be useful for the immobilization of various enzymes (i.e., cellulase and isomerase) and nanoparticles (i.e., magnetic Fe3 O4 ) and for functionalization of various acid groups (i.e., H2 PO3 , COOH, and SO3 H). We separately applied the synthesized biocatalysts (i.e., cellulase-Fe3 O4 @MSN and isomerase-Fe3 O4 @MSN) and chemical catalysts (i.e., HSO3 -MSN) in a sequential cellulose-to-glucose, glucose-to-fructose, and fructose-to-HMF conversion, respectively, across both aqueous- and organic-solvent systems after the optimization of reaction conditions (e.g., reaction temperature, water ratio, catalyst amount). The integrated enzymatic and chemocatalytic concept in this study could be an effective and economically friendly process for various catalytic applications.