Cellulose nanomaterials, as an increasingly available and highly renewable material, are poised to be used in a wide breadth of applications. Strong, potentially very cheap, and chemically active, CNs are being investigated in applications ranging from material reinforcement to advanced materials and composites for sensing, fuel cells, and catalysis. The hydroxyl-rich surface of CNs has widely been demonstrated as an excellent substrate for a variety of chemical modification. Carefully designed mesoporous silica supports are an example of advanced materials with features carefully tuned for applications in catalysis. These types of supports have been used to produce highly tunable enzyme-inspired organocatalysts with cooperative amine and hydroxyl moieties, active in a variety of acid-base catalyzed reactions. In this study, cellulose nanomaterials. including nanocrystals and nanofibrils. are analogously designed and modified to be effective alternative supports for organocatalysts. Control of surface acid and base content through chemical treatment and functionalization allows for a variety of catalyst materials and chemistries to be investigated. Building on previous work demonstrating CNs to be useful catalyst support materials, careful control of surface chemistry spacing and fibril geometry and networks is used to design highly active, stable catalyst materials for acid-base catalyzed reactions. Material activity is reported and studied considering the loading of surface acid and base species. CN catalysts were characterized by FTIR spectroscopy, CP-MAS 13C NMR, conductometric titration, elemental analysis, and other techniques. Kinetics studies, alongside chemical and structural design, were used to evaluate and describe the catalytic behavior of the CN surfaces.
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