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

Journal Article · · Nature Communications
 [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)

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.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1458818
Report Number(s):
NREL/JA-5100-71206
Journal Information:
Nature Communications, Vol. 9, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 89 works
Citation information provided by
Web of Science

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Cited By (19)

Specificity and mechanism of carbohydrate demethylation by cytochrome P450 monooxygenases text January 2018
Enabling microbial syringol conversion through structure-guided protein engineering journal June 2019
Exploiting enzyme promiscuity to shape plant specialized metabolism journal January 2019
Recent advances in lignin valorization with bacterial cultures: microorganisms, metabolic pathways, and bio-products journal February 2019
Genomics and biochemistry investigation on the metabolic pathway of milled wood and alkali lignin-derived aromatic metabolites of Comamonas serinivorans SP-35 journal December 2018
Catabolism of Alkylphenols in Rhodococcus via a Meta-Cleavage Pathway Associated With Genomic Islands journal August 2019
Identification of the two-component guaiacol demethylase system from Rhodococcus rhodochrous and expression in Pseudomonas putida EM42 for guaiacol assimilation journal March 2019
The Hot and the Colorful: Understanding the Metabolism, Genetics and Evolution of Consumer Preferred Metabolic Traits in Pepper and Related Species journal November 2019
Biotransformation of Phthalate Plasticizers and Bisphenol A by Marine-Derived, Freshwater, and Terrestrial Fungi journal February 2020
Exploring the Selective Demethylation of Aryl Methyl Ethers with a Pseudomonas Rieske Monooxygenase journal December 2018
Environmental sustainability: challenges and viable solutions journal December 2018
Enzymatic demethylation of Kraft lignin for lignin-based phenol-formaldehyde resin applications journal April 2019
Influence of organic amendments used for benz[a]anthracene remediation in a farmland soil: pollutant distribution and bacterial changes journal June 2019
Bacterial conversion of depolymerized Kraft lignin journal March 2019
Specificity and mechanism of carbohydrate demethylation by cytochrome P450 monooxygenases journal December 2018
Modular Engineering of Biomass Degradation Pathways journal April 2019
Bacterial cytochrome P450-catalyzed regio- and stereoselective steroid hydroxylation enabled by directed evolution and rational design journal January 2020
Passive membrane transport of lignin-related compounds journal October 2019
Mapping the diversity of microbial lignin catabolism: experiences from the eLignin database journal April 2019

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