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LPMO-mediated oxidation increases cellulose wettability, surface water retention and hydrolysis yield at high dry matter

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Abstract

The cellulose-water interface is a dynamic environment mostly dominated by interactions between water molecules and hydroxyl groups protruding from the top layer of the polysaccharide chains. This interface has attracted increasing interest within the context of hydrolysis with glycosyl hydrolases, and studies on the role of tightly bound and free water has emerged. At the molecular level, cellulose-bound water has been considered important to allow enzymatic hydrolysis at industrial relevant conditions, i.e. at high dry matter (HDM) contents. In the presence of lytic polysaccharide monooxygenase enzymes, the hydrolysis can with effective yields be run at well beyond the dry matter limit previously set by the 1st generation of enzyme preparations lacking LPMOs. The oxidative cleavage of the cellulose chain performed by LPMOs allow a higher level of synergism with GH in terms of accessibility of the cellulose surface. In this work, we studied how cellulose oxidation by LPMO increases the cellulose-water interaction and the impact of this on cellulose saccharification. Low-field NMR, water constraint and enzyme kinetics at high dry matter contents were used to characterize the cellulose-water interaction and its implications in enzymatic cellulose hydrolysis.

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Acknowledgments

The authors wish to acknowledge the funding bodies for their support.

Funding

The authors acknowledge the following grants: Innoviris-Bridge Re4Bru project for sustaining SM and DC; FNRS-MIS LUX-project F.4502.19 starting grant to D.C.; FNRS PINT-BILAT-M R.M012.18 for sustaining DC; DFF-FTP for having sustained DC; FAPESP-Sprint for having sustained IP; DFF for having sustained the visiting stay in Denmark for TJ and NK.

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Authors and Affiliations

  1. Geosciences and Natural Resource Management, University of Copenhagen, Copenhagen, Denmark

    David Cannella, Noha Weiss, Carmen Hsieh, Justyna Kuska, Lisbeth G. Thygesen, Claus Felby & Henning Jørgensen

  2. PhotoBioCatalysis Unit – CPBL, and Biomass Transformation Lab, Université Libre de Bruxelles, Brussels, Belgium

    David Cannella, Silvia Magri & Marco Zarattini

  3. São Carlos Institute of Physics, University of São Paulo, São Paulo, Brazil

    Igor Polikarpov

  4. Biological and Agricultural Engineering, University of California, Davis, USA

    Tina Jeoh

  5. Department of Biotechnology, Faculty of Engineering and Industrial Technology, Silpakorn University, Nakhon Pathom, 73000, Thailand

    Nardrapee Karuna

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  1. David Cannella
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Contributions

DC, HJ conceptualized the work, analyzed data carried enzymatic hydrolysis, and wrote the manuscript; DC, CH, JK, IP, ZM, SM prepared cellulose samples, produced the enzymes, and carried out cellulose treatments; DC, NW carried out water retention value analysis; CH, LT, CF carried out low-field NMR analysis T2; TJ, NW, NK, LT carried out T1/T2 LFNMR analysis. All authors read the manuscript and participated in its revision.

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Correspondence to David Cannella.

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Cannella, D., Weiss, N., Hsieh, C. et al. LPMO-mediated oxidation increases cellulose wettability, surface water retention and hydrolysis yield at high dry matter. Cellulose 30, 6259–6272 (2023). https://doi.org/10.1007/s10570-023-05271-z

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