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Controlling the Reactivity of Enzymes in Mechanochemistry: Inert Surfaces Protect β-Glucosidase Activity During Ball Milling

preprint
submitted on 30.07.2019 and posted on 31.07.2019 by Fabien Hammerer, Shaghayeh Ostadjoo, Tomislav Friscic, Karine Auclair
Although cellulose has been identified as the foremost candidate for the replacement of fossil fuels, its recalcitrant nature prevents the full deployment of technologies based on its saccharification. We recently reported a possible strategy to resolve this conundrum: using cellulases under “RAging” - a solvent-free process that utilizes enzymes under mechanochemical conditions - to achieve fast, efficient hydrolytic depolymerization of cellulosic materials into glucose. β-Glucosidases catalyze the last and often limiting step of this process, i.e. the formation of glucose from cellobiose. Here, we reveal the high sensitivity of β-glucosidases to ball milling, as well as an unexpected stabilization effect of inert surfaces, enabling the protection of β-glucosidases under mechanochemical treatment. This approach provides an unexpected strategy to control the reactivity of enzymes under mechanochemical conditions. Finally, our results also provide the very first demonstration of enzymatic equilibrium under mechanochemical conditions.

Funding

NSERC I2I 508646-17

NSERC E. W. R. Steacie Memorial Fellowship 507347-17

History

Email Address of Submitting Author

karine.auclair@mcgill.ca

Institution

McGill University

Country

Canada

ORCID For Submitting Author

0000-0003-0933-7956

Declaration of Conflict of Interest

Some of the herein presented work is a part of the patent application US 62/465,443 filed 1 March 2017.

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