The hydrophilicity of cellulose, arising from the presence of large number of hydroxyl groups, reduces its potential in nanocomposites containing nanocellulose (typically <10 wt%). In order to manufacture nanocomposites containing nanocellulose with improved properties, chemical modification is often needed. This chapter summarizes the chemical modification of nanoscale cellulose and its impact on the fiber-matrix interface, as well as the mechanical performance of the resulting polymer nanocomposites. We start with the discussion of conventional esterification of nanocellulose via acetylations reaction with acetic anhydrides and carboxylic acids. Methods for direct and indirect quantification of the fiber-matrix interface are reported. Green(er) esterification reactions in the gas phase and utilizing ionic liquids as the solvent and catalyst for the modification of nanocellulose are also discussed. In addition to this, this chapter also discusses the recent work on the carboxymethylation of nanocellulose and the deformation mechanism of bacterial cellulose networks within a composite.
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