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Title: A promiscuous cytochrome P450 aromatic O-demethylase for lignin bioconversion

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. Here, 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.
Authors:
 [1] ; ORCiD logo [2] ;  [3] ; ORCiD logo [4] ;  [5] ; ORCiD logo [6] ;  [1] ; ORCiD logo [7] ; ORCiD logo [6] ; ORCiD logo [8] ;  [4] ; ORCiD logo [6] ;  [9] ; ORCiD logo [1]
  1. Univ. of Portsmouth, Portsmouth (United Kingdom)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Montana State Univ., Bozeman, MT (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Campinas, Sao Paulo (Brazil)
  4. Univ. of California at Los Angeles, Los Angeles, CA (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of California at Los Angeles, Los Angeles, CA (United States)
  6. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  7. Univ. of Campinas, Sao Paulo (Brazil)
  8. Univ. of Georgia, Athens, GA (United States)
  9. Montana State Univ., Bozeman, MT (United States)
Publication Date:
Report Number(s):
NREL/JA-5100-71206
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; enzyme discovery; protein family; enzyme characterization; lignin conversion
OSTI Identifier:
1458818