Simmons, Thomas J, Frandsen, Kristian E H, Ciano, Luisa orcid.org/0000-0002-1667-0856 et al. (12 more authors) (2017) Structural and electronic determinants of lytic polysaccharide monooxygenase reactivity on polysaccharide substrates. Nature Communications. 1064 (2017). ISSN 2041-1723
Abstract
Lytic polysaccharide monooxygenases (LPMOs) are industrially important copper-dependent enzymes that oxidatively cleave polysaccharides. Here we present a functional and structural characterization of two closely related AA9-family LPMOs from Lentinus similis (LsAA9A) and Collariella virescens (CvAA9A). LsAA9A and CvAA9A cleave a range of polysaccharides, including cellulose, xyloglucan, mixed-linkage glucan and glucomannan. LsAA9A additionally cleaves isolated xylan substrates. The structures of CvAA9A and of LsAA9A bound to cellulosic and non-cellulosic oligosaccharides provide insight into the molecular determinants of their specificity. Spectroscopic measurements reveal differences in copper co-ordination upon the binding of xylan and glucans. LsAA9A activity is less sensitive to the reducing agent potential when cleaving xylan, suggesting that distinct catalytic mechanisms exist for xylan and glucan cleavage. Overall, these data show that AA9 LPMOs can display different apparent substrate specificities dependent upon both productive protein–carbohydrate interactions across a binding surface and also electronic considerations at the copper active site.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © The Author(s) 2017. |
Keywords: | Catalytic Domain,Copper/chemistry,Electron Spin Resonance Spectroscopy,Fungal Proteins/chemistry,Mixed Function Oxygenases/chemistry,Models, Molecular,Polyporaceae/enzymology,Polysaccharides/chemistry,Sordariales/enzymology,Substrate Specificity |
Dates: |
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Institution: | The University of York |
Academic Units: | The University of York > Faculty of Sciences (York) > Chemistry (York) |
Funding Information: | Funder Grant number BBSRC (BIOTECHNOLOGY AND BIOLOGICAL SCIENCES RESEARCH COUNCIL) BB/L000423/1 |
Depositing User: | Pure (York) |
Date Deposited: | 09 Nov 2017 14:19 |
Last Modified: | 13 Jan 2025 00:06 |
Published Version: | https://doi.org/10.1038/s41467-017-01247-3 |
Status: | Published |
Refereed: | Yes |
Identification Number: | 10.1038/s41467-017-01247-3 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:123812 |
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