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Insights into the oxidative degradation of cellulose by a copper metalloenzyme that exploits biomass components

Open access
Quinlan, R. Jason, Sweeney, Matt D., Lo Leggio, Leila, Otten, Harm, Poulsen, Jens-Christian N., Johansen, Katja Salomon, Krogh, Kristian B. R. M., Jørgensen, Christian Isak, Tovborg, Morten, Anthonsen, Annika, Tryfona, Theodora, Walter, Clive P., Dupree, Paul, Xu, Feng, Davies, Gideon J., Walton, Paul H.·2011·Proceedings of the National Academy of Sciences

Abstract

The enzymatic degradation of recalcitrant plant biomass is one of the key industrial challenges of the 21st century. Accordingly, there is a continuing drive to discover new routes to promote polysaccharide degradation. Perhaps the most promising approach involves the application of “cellulase-enhancing factors,” such as those from the glycoside hydrolase (CAZy) GH61 family. Here we show that GH61 enzymes are a unique family of copper-dependent oxidases. We demonstrate that copper is needed for GH61 maximal activity and that the formation of cellodextrin and oxidized cellodextrin products by GH61 is enhanced in the presence of small molecule redox-active cofactors such as ascorbate and gallate. By using electron paramagnetic resonance spectroscopy and single-crystal X-ray diffraction, the active site of GH61 is revealed to contain a type II copper and, uniquely, a methylated histidine in the copper's coordination sphere, thus providing an innovative paradigm in bioinorganic enzymatic catalysis.

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Metadata

Authors
Quinlan, R. J., Sweeney, M. D., Lo Leggio, L., Otten, H., Poulsen, J.-C. N., Johansen, K. S., Krogh, K. B. R. M., Jørgensen, C. I., Tovborg, M., Anthonsen, A., Tryfona, T., Walter, C. P., Dupree, P., Xu, F., Davies, G. J., & Walton, P. H.
Venue
Proceedings of the National Academy of Sciences
Published
2011-08-29
Volume
108
Issue
37
Pages
15079-15084
ISSN
  • 0027-8424 (ISSN-L)
  • 1091-6490
OpenAlex
W1967796434
Cited by
1,036
References
1
FWCI
37.56
Type
journal article
Language
en
Open access
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CoChat. (2026). Citation check: Insights into the oxidative degradation of cellulose by a copper metalloenzyme that exploits biomass components. https://app.cochat.ai/papers/10.1073/pnas.1105776108
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Quinlan, R. J., Sweeney, M. D., Lo Leggio, L., Otten, H., Poulsen, J.-C. N., Johansen, K. S., Krogh, K. B. R. M., Jørgensen, C. I., Tovborg, M., Anthonsen, A., Tryfona, T., Walter, C. P., Dupree, P., Xu, F., Davies, G. J., & Walton, P. H. (2011). Insights into the oxidative degradation of cellulose by a copper metalloenzyme that exploits biomass components. Proceedings of the National Academy of Sciences. https://doi.org/10.1073/pnas.1105776108

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Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).

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