An efficient catalytic route in haem peroxygenases mediated by O2/small-molecule reductant pairs for sustainable applications

IF 42.8 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2025-01-28 DOI:10.1038/s41929-024-01281-7

Di Deng, Zhihui Jiang, Lixin Kang, Langxing Liao, Xiaodong Zhang, Yuben Qiao, Yang Zhou, Liulin Yang, Binju Wang, Aitao Li

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引用次数: 0

Abstract

Haem peroxygenases are attractive biocatalysts for incorporating oxygen into organic molecules using H₂O₂. However, their practical applications are hindered by irreversible oxidative inactivation due to exogenous H₂O₂ usage. Here we present an alternative catalytic route in haem peroxygenases that uses O₂ and small-molecule reductants such as ascorbic acid and dehydroascorbic acid (DHA) to drive reactions. Our experimental and computational studies indicated that DHAA, the hydrated form of DHA, serves as the key co-substrate that activates oxygen to generate the active oxyferryl haem compound I. We also demonstrate the broad applicability of this O₂/reductant-dependent route across various haem peroxygenases, highlighting its biological significance for mono-oxygenase functionality. Importantly, this innovative route avoids the use of H₂O₂, thereby preventing the risk of irreversible enzyme inactivation. Finally, scaled-up reactions yielded chiral, value-added products with excellent productivity, underscoring the synthetic potential of this developed peroxygenase technology for sustainable chemical transformations.

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.