Construction of P450 scaffold biocatalysts for the biodegradation of five chloroanilines.

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Hauptverfasser: Yang, Ridong, Shoji, Osami, Lin, Yingwu, Wang, Fang, Che, Hongxia, Xu, Jiakun
Format: Artículo científico
Sprache:en
Veröffentlicht: Journal of hazardous materials 2025
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author Yang, Ridong
Shoji, Osami
Lin, Yingwu
Wang, Fang
Che, Hongxia
Xu, Jiakun
author_facet Yang, Ridong
Shoji, Osami
Lin, Yingwu
Wang, Fang
Che, Hongxia
Xu, Jiakun
Yang, Ridong
Shoji, Osami
Lin, Yingwu
Wang, Fang
Che, Hongxia
Xu, Jiakun
collection PubMed - marine biology
contents Construction of P450 scaffold biocatalysts for the biodegradation of five chloroanilines. Yang, Ridong Shoji, Osami Lin, Yingwu Wang, Fang Che, Hongxia Xu, Jiakun Aniline Compounds Biodegradation, Environmental Cytochrome P-450 Enzyme System Biocatalysis Environmental Pollutants Chloroanilines represent a class of persistent and highly toxic environmental pollutants, posing significant challenges for green remediation strategies. While P450BM3 monooxygenases are renowned for their ability to catalyze the monooxidation of inert C-H bonds, costly NAD(P)H and complex electron transport systems required for P450BM3 catalysis limit their practical applications. This study pioneers the development of innovative artificial biocatalysts by strategically engineering the active site of P450BM3. Specifically, the substitution of the highly conserved threonine 268 with aspartic acid effectively induces peroxygenase activity, allowing for enhanced catalytic efficiency. Remarkably, the engineered P450BM3 mutants achieved degradation rates of 98.38-99.18 % for five chloroanilines (4-chloroaniline, 2-chloroaniline, 2,4-dichloroaniline, 3,4-dichloroaniline, and 3,5-dichloroaniline) in just 10-15 min, all without the need for NAD(P)H or dual-functional small molecules. Comprehensive degradation mechanism analysis via UPLC-MS corroborated the remarkable performance of these biocatalysts. This research not only demonstrates a novel approach for engineering P450 monooxygenases to exhibit peroxygenase activity but also significantly broadens their potential applications in synthetic chemistry and synthetic biology, paving the way for greener and more sustainable remediation technologies.
format Artículo científico
id pubmed_39854990
institution PubMed
language en
publishDate 2025
publisher Journal of hazardous materials
record_format pubmed
spellingShingle Construction of P450 scaffold biocatalysts for the biodegradation of five chloroanilines.
Yang, Ridong
Shoji, Osami
Lin, Yingwu
Wang, Fang
Che, Hongxia
Xu, Jiakun
Aniline Compounds
Biodegradation, Environmental
Cytochrome P-450 Enzyme System
Biocatalysis
Environmental Pollutants
Construction of P450 scaffold biocatalysts for the biodegradation of five chloroanilines. Yang, Ridong Shoji, Osami Lin, Yingwu Wang, Fang Che, Hongxia Xu, Jiakun Aniline Compounds Biodegradation, Environmental Cytochrome P-450 Enzyme System Biocatalysis Environmental Pollutants Chloroanilines represent a class of persistent and highly toxic environmental pollutants, posing significant challenges for green remediation strategies. While P450BM3 monooxygenases are renowned for their ability to catalyze the monooxidation of inert C-H bonds, costly NAD(P)H and complex electron transport systems required for P450BM3 catalysis limit their practical applications. This study pioneers the development of innovative artificial biocatalysts by strategically engineering the active site of P450BM3. Specifically, the substitution of the highly conserved threonine 268 with aspartic acid effectively induces peroxygenase activity, allowing for enhanced catalytic efficiency. Remarkably, the engineered P450BM3 mutants achieved degradation rates of 98.38-99.18 % for five chloroanilines (4-chloroaniline, 2-chloroaniline, 2,4-dichloroaniline, 3,4-dichloroaniline, and 3,5-dichloroaniline) in just 10-15 min, all without the need for NAD(P)H or dual-functional small molecules. Comprehensive degradation mechanism analysis via UPLC-MS corroborated the remarkable performance of these biocatalysts. This research not only demonstrates a novel approach for engineering P450 monooxygenases to exhibit peroxygenase activity but also significantly broadens their potential applications in synthetic chemistry and synthetic biology, paving the way for greener and more sustainable remediation technologies.
title Construction of P450 scaffold biocatalysts for the biodegradation of five chloroanilines.
topic Aniline Compounds
Biodegradation, Environmental
Cytochrome P-450 Enzyme System
Biocatalysis
Environmental Pollutants
url https://pubmed.ncbi.nlm.nih.gov/39854990/