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Integrated, Cascading Enzyme‐/Chemocatalytic Cellulose Conversion using Catalysts based on Mesoporous Silica Nanoparticles
Author(s) -
Lee YiChun,
Dutta Saikat,
Wu Kevin C.W.
Publication year - 2014
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201402605
Subject(s) - cellulase , chemistry , cellulose , catalysis , mesoporous silica , aqueous solution , mesoporous material , nanoparticle , fructose , surface modification , solvent , yield (engineering) , green chemistry , immobilized enzyme , organic chemistry , heterogeneous catalysis , materials science , enzyme , nanotechnology , reaction mechanism , metallurgy
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 Fe 3 O 4 ) and for functionalization of various acid groups (i.e., H 2 PO 3 , COOH, and SO 3 H). We separately applied the synthesized biocatalysts (i.e., cellulase‐Fe 3 O 4 @MSN and isomerase‐Fe 3 O 4 @MSN) and chemical catalysts (i.e., HSO 3 ‐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.

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