Cellulose nanocrystals (CNCs) can be extracted from cellulosic materials through the degradation of non-crystalline cellulose domains in the feedstock via acid hydrolysis. However, the sugars released from the hydrolysis process cannot be easily recovered from the acid waste stream. In this study, cellulases were used to preferentially degrade non-crystalline domains with the objectives of recovering sugars and generating a feedstock with concentrated CNC precursors for a more efficient acid hydrolysis process. Filter paper and wood pulp substrates were enzyme-treated for 2–10 h to recover 20–40 wt % glucose. Substantial xylose yield (6–12 wt %) was generated from wood pulp. CNC yields from acid hydrolysis of cellulases-treated filter paper, and wood pulp improved by 8–18% and 58–86%, respectively, when compared with the original substrate. It was thought that CNC precursors accumulated in the cellulases-treated feedstock due to enzymatic digestion of the more accessible non-crystalline celluloses. Therefore, acid hydrolysis from enzyme-treated feedstock will require proportionally less water and reagents resulting in increased efficiency and productivity in downstream processes. This study demonstrates that an enzymatically-mediated process allows recovery of fermentable sugars and improves acid hydrolysis efficiency for CNC production.
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