Ether Oxidation by an Evolved Fungal Heme-Peroxygenase: Insights into Substrate Recognition and Reactivity
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Departamento de Ingeniería Celular y Biocatálisis, Instituto de Biotecnología Universidad Nacional Autónoma de México, Cuernavaca 62210, Morelos, Mexico
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Department of Biocatalysis, Institute of Catalysis and Petrochemistry, CSIC, 28049 Madrid, Spain
*
Author to whom correspondence should be addressed.
Academic Editor: Sławomir Milewski
J. Fungi 2021, 7(8), 608; https://doi.org/10.3390/jof7080608
Received: 16 June 2021
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Revised: 28 June 2021
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Accepted: 30 June 2021
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Published: 28 July 2021
(This article belongs to the Special Issue Fungal Biodegradation: Strategies, Current Understanding, and Future Prospects)
Ethers can be found in the environment as structural, active or even pollutant molecules, although their degradation is not efficient under environmental conditions. Fungal unspecific heme-peroxygenases (UPO were reported to degrade low-molecular-weight ethers through an H2O2-dependent oxidative cleavage mechanism. Here, we report the oxidation of a series of structurally related aromatic ethers, catalyzed by a laboratory-evolved UPO (PaDa-I) aimed at elucidating the factors influencing this unusual biochemical reaction. Although some of the studied ethers were substrates of the enzyme, they were not efficiently transformed and, as a consequence, secondary reactions (such as the dismutation of H2O2 through catalase-like activity and suicide enzyme inactivation) became significant, affecting the oxidation efficiency. The set of reactions that compete during UPO-catalyzed ether oxidation were identified and quantified, in order to find favorable conditions that promote ether oxidation over the secondary reactions.
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Keywords:
fungal peroxygenase; biodegradation; suicide inactivation; ether oxidation; xenobiotic transformation
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MDPI and ACS Style
Mireles, R.; Ramirez-Ramirez, J.; Alcalde, M.; Ayala, M. Ether Oxidation by an Evolved Fungal Heme-Peroxygenase: Insights into Substrate Recognition and Reactivity. J. Fungi 2021, 7, 608. https://doi.org/10.3390/jof7080608
AMA Style
Mireles R, Ramirez-Ramirez J, Alcalde M, Ayala M. Ether Oxidation by an Evolved Fungal Heme-Peroxygenase: Insights into Substrate Recognition and Reactivity. Journal of Fungi. 2021; 7(8):608. https://doi.org/10.3390/jof7080608
Chicago/Turabian StyleMireles, Raul, Joaquin Ramirez-Ramirez, Miguel Alcalde, and Marcela Ayala. 2021. "Ether Oxidation by an Evolved Fungal Heme-Peroxygenase: Insights into Substrate Recognition and Reactivity" Journal of Fungi 7, no. 8: 608. https://doi.org/10.3390/jof7080608
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