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Article

Ether Oxidation by an Evolved Fungal Heme-Peroxygenase: Insights into Substrate Recognition and Reactivity

1
Departamento de Ingeniería Celular y Biocatálisis, Instituto de Biotecnología Universidad Nacional Autónoma de México, Cuernavaca 62210, Morelos, Mexico
2
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 / Revised: 28 June 2021 / Accepted: 30 June 2021 / Published: 28 July 2021
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. View Full-Text
Keywords: fungal peroxygenase; biodegradation; suicide inactivation; ether oxidation; xenobiotic transformation 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 Style

Mireles, 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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