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Title: Characterization of alkylguaiacol-degrading cytochromes P450 for the biocatalytic valorization of lignin

Abstract

Upgrading lignin, an underutilized component of biomass, is essential for the sustainability of biorefineries. Biocatalysis has considerable potential for upgrading lignin, but our lack of knowledge of relevant enzymes and pathways has limited its application. Herein, we describe a microbial pathway responsible for catabolizing alkylguaiacols, a major component of several industrial lignin streams. Catabolism is initiated by a cytochrome P450, with related P450s catalyzing the O-demethylation of different lignin-derived guaiacols and subsequent catabolism depending on the substitution pattern of the guaiacol. Importantly, the alkylguaiacol catabolic pathway enables bacterial growth on corn stover lignin produced by reductive catalytic fractionation. Overall, these insights greatly facilitate the engineering of P450s and bacteria to biocatalytically upgrade lignin.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of British Columbia, Vancouver, BC (Canada)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office (BETO)
OSTI Identifier:
1726039
Report Number(s):
NREL/JA-2800-77914
Journal ID: ISSN 0027-8424; MainId:31823;UUID:8ffde6ac-d3c6-4346-99c8-b37e82b09c30;MainAdminID:18846
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 117; Journal Issue: 41; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; biocatalysis; cytochrome P450; guaiacol; lignin valorization; O-demethylase

Citation Formats

Fetherolf, Morgan M., Levy-Booth, David J., Navas, Laura E., Liu, Jie, Grigg, Jason C., Wilson, Andrew, Katahira, Rui, Beckham, Gregg T., Mohn, William W., and Eltis, Lindsay D. Characterization of alkylguaiacol-degrading cytochromes P450 for the biocatalytic valorization of lignin. United States: N. p., 2020. Web. doi:10.1073/pnas.1916349117.
Fetherolf, Morgan M., Levy-Booth, David J., Navas, Laura E., Liu, Jie, Grigg, Jason C., Wilson, Andrew, Katahira, Rui, Beckham, Gregg T., Mohn, William W., & Eltis, Lindsay D. Characterization of alkylguaiacol-degrading cytochromes P450 for the biocatalytic valorization of lignin. United States. https://doi.org/10.1073/pnas.1916349117
Fetherolf, Morgan M., Levy-Booth, David J., Navas, Laura E., Liu, Jie, Grigg, Jason C., Wilson, Andrew, Katahira, Rui, Beckham, Gregg T., Mohn, William W., and Eltis, Lindsay D. Mon . "Characterization of alkylguaiacol-degrading cytochromes P450 for the biocatalytic valorization of lignin". United States. https://doi.org/10.1073/pnas.1916349117. https://www.osti.gov/servlets/purl/1726039.
@article{osti_1726039,
title = {Characterization of alkylguaiacol-degrading cytochromes P450 for the biocatalytic valorization of lignin},
author = {Fetherolf, Morgan M. and Levy-Booth, David J. and Navas, Laura E. and Liu, Jie and Grigg, Jason C. and Wilson, Andrew and Katahira, Rui and Beckham, Gregg T. and Mohn, William W. and Eltis, Lindsay D.},
abstractNote = {Upgrading lignin, an underutilized component of biomass, is essential for the sustainability of biorefineries. Biocatalysis has considerable potential for upgrading lignin, but our lack of knowledge of relevant enzymes and pathways has limited its application. Herein, we describe a microbial pathway responsible for catabolizing alkylguaiacols, a major component of several industrial lignin streams. Catabolism is initiated by a cytochrome P450, with related P450s catalyzing the O-demethylation of different lignin-derived guaiacols and subsequent catabolism depending on the substitution pattern of the guaiacol. Importantly, the alkylguaiacol catabolic pathway enables bacterial growth on corn stover lignin produced by reductive catalytic fractionation. Overall, these insights greatly facilitate the engineering of P450s and bacteria to biocatalytically upgrade lignin.},
doi = {10.1073/pnas.1916349117},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 41,
volume = 117,
place = {United States},
year = {Mon Sep 28 00:00:00 EDT 2020},
month = {Mon Sep 28 00:00:00 EDT 2020}
}

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