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    Molecular-Scale Investigations of Cellulose Microstructure during Enzymatic Hydrolysis
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    Biological and Agricultural Engineering, University of California, One Shields Avenue, Davis, California 95616
    * To whom correspondence should be addressed. E-mail: [email protected]
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    Biomacromolecules

    Cite this: Biomacromolecules 2010, 11, 8, 2000–2007
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    https://doi.org/10.1021/bm100366h
    Published June 29, 2010
    Copyright © 2010 American Chemical Society
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    Abstract

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    Changes in cellulose microstructure have been proposed to occur throughout hydrolysis that impact enzyme access and hydrolysis rates. However, there are very few direct observations of such changes in ongoing reactions. In this study, changes in the microstructure of cellulose are measured by simultaneous confocal and atomic force microscopy and are correlated to hydrolysis extents and quantities of bound enzyme in the reaction. Minimally processed and never-dried cellulose I was hydrolyzed by a purified cellobiohydrolase, Trichoderma reesei Cel7A. Early in the reaction (∼30% hydrolysis), at high hydrolysis rates and high bound cellulase quantities, untwisting of cellulose microfibrils was observed. As the hydrolysis reaction neared completion (>80% hydrolysis), extensively thinned microfibrils (diameters of 3−5 nm) and channels (0.3−0.6 nm deep) along the lengths of the microfibrils were observed. The prominent microstructural changes in cellulose due to cellobiohydrolase action are discussed in the context of the overall hydrolysis reaction.

    Copyright © 2010 American Chemical Society

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    Data on the enzymatic conversion of native versus DTAF-grafted bacterial cellulose, AFM data for undigested controls, and larger scans and height AFM data of the figures presented in this manuscript. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Biomacromolecules

    Cite this: Biomacromolecules 2010, 11, 8, 2000–2007
    Click to copy citationCitation copied!
    https://doi.org/10.1021/bm100366h
    Published June 29, 2010
    Copyright © 2010 American Chemical Society
    Request reuse permissions

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