دورية أكاديمية
Engineering a Cytochrome P450 for Demethylation of Lignin-Derived Aromatic Aldehydes.
العنوان: | Engineering a Cytochrome P450 for Demethylation of Lignin-Derived Aromatic Aldehydes. |
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المؤلفون: | Ellis ES; Department of Chemistry and Biochemistry, Montana State University, 103 Chemistry and Biochemistry Building, PO Box 173400, Bozeman, Montana 59717, United States., Hinchen DJ; Centre for Enzyme Innovation, School of Biological Sciences, Institute of Biological and Biomedical Sciences, University of Portsmouth, Portsmouth PO1 2DY, United Kingdom., Bleem A; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States.; Center for Bioenergy Innovation, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Bu L; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Mallinson SJB; Centre for Enzyme Innovation, School of Biological Sciences, Institute of Biological and Biomedical Sciences, University of Portsmouth, Portsmouth PO1 2DY, United Kingdom., Allen MD; Centre for Enzyme Innovation, School of Biological Sciences, Institute of Biological and Biomedical Sciences, University of Portsmouth, Portsmouth PO1 2DY, United Kingdom., Streit BR; Department of Chemistry and Biochemistry, Montana State University, 103 Chemistry and Biochemistry Building, PO Box 173400, Bozeman, Montana 59717, United States., Machovina MM; Department of Chemistry and Biochemistry, Montana State University, 103 Chemistry and Biochemistry Building, PO Box 173400, Bozeman, Montana 59717, United States., Doolin QV; Department of Chemistry and Biochemistry, Montana State University, 103 Chemistry and Biochemistry Building, PO Box 173400, Bozeman, Montana 59717, United States., Michener WE; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Johnson CW; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Knott BC; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Beckham GT; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States.; Center for Bioenergy Innovation, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., McGeehan JE; Centre for Enzyme Innovation, School of Biological Sciences, Institute of Biological and Biomedical Sciences, University of Portsmouth, Portsmouth PO1 2DY, United Kingdom., DuBois JL; Department of Chemistry and Biochemistry, Montana State University, 103 Chemistry and Biochemistry Building, PO Box 173400, Bozeman, Montana 59717, United States. |
المصدر: | JACS Au [JACS Au] 2021 Feb 04; Vol. 1 (3), pp. 252-261. Date of Electronic Publication: 2021 Feb 04 (Print Publication: 2021). |
نوع المنشور: | Journal Article |
اللغة: | English |
بيانات الدورية: | Publisher: American Chemical Society Country of Publication: United States NLM ID: 101775714 Publication Model: eCollection Cited Medium: Internet ISSN: 2691-3704 (Electronic) Linking ISSN: 26913704 NLM ISO Abbreviation: JACS Au Subsets: PubMed not MEDLINE |
أسماء مطبوعة: | Original Publication: Washington, DC : American Chemical Society, [2021]- |
مستخلص: | Biological funneling of lignin-derived aromatic compounds is a promising approach for valorizing its catalytic depolymerization products. Industrial processes for aromatic bioconversion will require efficient enzymes for key reactions, including demethylation of O -methoxy-aryl groups, an essential and often rate-limiting step. The recently characterized GcoAB cytochrome P450 system comprises a coupled monoxygenase (GcoA) and reductase (GcoB) that catalyzes oxidative demethylation of the O- methoxy-aryl group in guaiacol. Here, we evaluate a series of engineered GcoA variants for their ability to demethylate o -and p -vanillin, which are abundant lignin depolymerization products. Two rationally designed, single amino acid substitutions, F169S and T296S, are required to convert GcoA into an efficient catalyst toward the o - and p -isomers of vanillin, respectively. Gain-of-function in each case is explained in light of an extensive series of enzyme-ligand structures, kinetic data, and molecular dynamics simulations. Using strains of Pseudomonas putida KT2440 already optimized for p -vanillin production from ferulate, we demonstrate demethylation by the T296S variant in vivo . This work expands the known aromatic O- demethylation capacity of cytochrome P450 enzymes toward important lignin-derived aromatic monomers. Competing Interests: The authors declare no competing financial interest. (© 2021 The Authors. Published by American Chemical Society.) |
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معلومات مُعتمدة: | R35 GM136390 United States GM NIGMS NIH HHS |
تواريخ الأحداث: | Date Created: 20210901 Latest Revision: 20240814 |
رمز التحديث: | 20240814 |
مُعرف محوري في PubMed: | PMC8395679 |
DOI: | 10.1021/jacsau.0c00103 |
PMID: | 34467290 |
قاعدة البيانات: | MEDLINE |
تدمد: | 2691-3704 |
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DOI: | 10.1021/jacsau.0c00103 |