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A promiscuous cytochrome P450 aromatic O-demethylase for lignin bioconversion

Author

Listed:
  • Sam J. B. Mallinson

    (University of Portsmouth)

  • Melodie M. Machovina

    (National Renewable Energy Laboratory
    Montana State University)

  • Rodrigo L. Silveira

    (National Renewable Energy Laboratory
    University of Campinas)

  • Marc Garcia-Borràs

    (University of California at Los Angeles)

  • Nathan Gallup

    (National Renewable Energy Laboratory
    University of California at Los Angeles)

  • Christopher W. Johnson

    (National Renewable Energy Laboratory)

  • Mark D. Allen

    (University of Portsmouth)

  • Munir S. Skaf

    (University of Campinas)

  • Michael F. Crowley

    (National Renewable Energy Laboratory)

  • Ellen L. Neidle

    (University of Georgia)

  • Kendall N. Houk

    (University of California at Los Angeles)

  • Gregg T. Beckham

    (National Renewable Energy Laboratory)

  • Jennifer L. DuBois

    (Montana State University)

  • John E. McGeehan

    (University of Portsmouth)

Abstract

Microbial aromatic catabolism offers a promising approach to convert lignin, a vast source of renewable carbon, into useful products. Aryl-O-demethylation is an essential biochemical reaction to ultimately catabolize coniferyl and sinapyl lignin-derived aromatic compounds, and is often a key bottleneck for both native and engineered bioconversion pathways. Here, we report the comprehensive characterization of a promiscuous P450 aryl-O-demethylase, consisting of a cytochrome P450 protein from the family CYP255A (GcoA) and a three-domain reductase (GcoB) that together represent a new two-component P450 class. Though originally described as converting guaiacol to catechol, we show that this system efficiently demethylates both guaiacol and an unexpectedly wide variety of lignin-relevant monomers. Structural, biochemical, and computational studies of this novel two-component system elucidate the mechanism of its broad substrate specificity, presenting it as a new tool for a critical step in biological lignin conversion.

Suggested Citation

  • Sam J. B. Mallinson & Melodie M. Machovina & Rodrigo L. Silveira & Marc Garcia-Borràs & Nathan Gallup & Christopher W. Johnson & Mark D. Allen & Munir S. Skaf & Michael F. Crowley & Ellen L. Neidle & , 2018. "A promiscuous cytochrome P450 aromatic O-demethylase for lignin bioconversion," Nature Communications, Nature, vol. 9(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04878-2
    DOI: 10.1038/s41467-018-04878-2
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    Cited by:

    1. Zhu, Daochen & Qaria, Majjid A. & Zhu, Bin & Sun, Jianzhong & Yang, Bin, 2022. "Extremophiles and extremozymes in lignin bioprocessing," Renewable and Sustainable Energy Reviews, Elsevier, vol. 157(C).

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