Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi

Summary: White-rot fungi (WRF) are the most efficient lignin-degrading organisms in nature. However, their capacity to use lignin-related aromatic compounds, such as 4-hydroxybenzoate, as carbon sources has only been described recently. Previously, the hydroxyquinol pathway was proposed for the bioc...

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Main Authors: Eugene Kuatsjah, Alexa Schwartz, Michael Zahn, Konstantinos Tornesakis, Zoe A. Kellermyer, Morgan A. Ingraham, Sean P. Woodworth, Kelsey J. Ramirez, Paul A. Cox, Andrew R. Pickford, Davinia Salvachúa
Format: Article
Language:English
Published: Elsevier 2024-12-01
Series:Cell Reports
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Online Access:http://www.sciencedirect.com/science/article/pii/S2211124724013536
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author Eugene Kuatsjah
Alexa Schwartz
Michael Zahn
Konstantinos Tornesakis
Zoe A. Kellermyer
Morgan A. Ingraham
Sean P. Woodworth
Kelsey J. Ramirez
Paul A. Cox
Andrew R. Pickford
Davinia Salvachúa
author_facet Eugene Kuatsjah
Alexa Schwartz
Michael Zahn
Konstantinos Tornesakis
Zoe A. Kellermyer
Morgan A. Ingraham
Sean P. Woodworth
Kelsey J. Ramirez
Paul A. Cox
Andrew R. Pickford
Davinia Salvachúa
author_sort Eugene Kuatsjah
collection DOAJ
description Summary: White-rot fungi (WRF) are the most efficient lignin-degrading organisms in nature. However, their capacity to use lignin-related aromatic compounds, such as 4-hydroxybenzoate, as carbon sources has only been described recently. Previously, the hydroxyquinol pathway was proposed for the bioconversion of these compounds in fungi, but gene- and structure-function relationships of the full enzymatic pathway remain uncharacterized in any single fungal species. Here, we characterize seven enzymes from two WRF, Trametes versicolor and Gelatoporia subvermispora, which constitute a four-enzyme cascade from 4-hydroxybenzoate to β-ketoadipate via the hydroxyquinol pathway. Furthermore, we solve the crystal structure of four of these enzymes and identify mechanistic differences with the closest bacterial and fungal structural homologs. Overall, this research expands our understanding of aromatic catabolism by WRF and establishes an alternative strategy for the conversion of lignin-related compounds to the valuable molecule β-ketoadipate, contributing to the development of biological processes for lignin valorization.
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spelling doaj-art-2fb1d490d265425194ed31fef4dc2b8e2025-08-20T01:52:42ZengElsevierCell Reports2211-12472024-12-01431211500210.1016/j.celrep.2024.115002Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungiEugene Kuatsjah0Alexa Schwartz1Michael Zahn2Konstantinos Tornesakis3Zoe A. Kellermyer4Morgan A. Ingraham5Sean P. Woodworth6Kelsey J. Ramirez7Paul A. Cox8Andrew R. Pickford9Davinia Salvachúa10Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USARenewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USA; Advanced Energy Systems Graduate Program, Colorado School of Mines, Golden, CO 80401, USACentre for Enzyme Innovation, School of the Environment and Life Sciences, University of Portsmouth, PO1 2DT Portsmouth, UKCentre for Enzyme Innovation, School of the Environment and Life Sciences, University of Portsmouth, PO1 2DT Portsmouth, UKRenewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USARenewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USARenewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USARenewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USACentre for Enzyme Innovation, School of the Environment and Life Sciences, University of Portsmouth, PO1 2DT Portsmouth, UKCentre for Enzyme Innovation, School of the Environment and Life Sciences, University of Portsmouth, PO1 2DT Portsmouth, UKRenewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO 80401, USA; Corresponding authorSummary: White-rot fungi (WRF) are the most efficient lignin-degrading organisms in nature. However, their capacity to use lignin-related aromatic compounds, such as 4-hydroxybenzoate, as carbon sources has only been described recently. Previously, the hydroxyquinol pathway was proposed for the bioconversion of these compounds in fungi, but gene- and structure-function relationships of the full enzymatic pathway remain uncharacterized in any single fungal species. Here, we characterize seven enzymes from two WRF, Trametes versicolor and Gelatoporia subvermispora, which constitute a four-enzyme cascade from 4-hydroxybenzoate to β-ketoadipate via the hydroxyquinol pathway. Furthermore, we solve the crystal structure of four of these enzymes and identify mechanistic differences with the closest bacterial and fungal structural homologs. Overall, this research expands our understanding of aromatic catabolism by WRF and establishes an alternative strategy for the conversion of lignin-related compounds to the valuable molecule β-ketoadipate, contributing to the development of biological processes for lignin valorization.http://www.sciencedirect.com/science/article/pii/S2211124724013536CP: Metabolism
spellingShingle Eugene Kuatsjah
Alexa Schwartz
Michael Zahn
Konstantinos Tornesakis
Zoe A. Kellermyer
Morgan A. Ingraham
Sean P. Woodworth
Kelsey J. Ramirez
Paul A. Cox
Andrew R. Pickford
Davinia Salvachúa
Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi
Cell Reports
CP: Metabolism
title Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi
title_full Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi
title_fullStr Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi
title_full_unstemmed Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi
title_short Biochemical and structural characterization of enzymes in the 4-hydroxybenzoate catabolic pathway of lignin-degrading white-rot fungi
title_sort biochemical and structural characterization of enzymes in the 4 hydroxybenzoate catabolic pathway of lignin degrading white rot fungi
topic CP: Metabolism
url http://www.sciencedirect.com/science/article/pii/S2211124724013536
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