生物启发镧系-邻醌催化好氧二硫化物形成

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-03-03 DOI:10.1021/acscatal.5c00165

Runze Zhang, Keting Zhou, Yu Xia, Sanzhong Luo

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引用次数: 0

摘要

硫醇氧化形成二硫键是生物系统中一个至关重要的反应。受甲醇脱氢酶（MDH）的启发，我们开发了一种生物启发醌催化的硫醇氧化成二硫化物的好氧氧化反应。在机理研究的基础上，我们证实了由镧离子配位的半醌自由基阴离子作为关键中间体。巯基醌氧化还原穿梭进一步被证明在醇的有氧氧化中介导mdh样活性。

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Bioinspired Lanthanide-ortho-Quinone-Catalyzed Aerobic Disulfide Formation

The oxidation of thiols to form disulfide bonds is a crucial reaction in biological systems. Inspired by methanol dehydrogenase (MDH), we developed a bioinspired quinone-catalyzed aerobic oxidation reaction for thiol oxidation to disulfides. Based on mechanistic studies, we have confirmed that a semiquinone radical anion, coordinated by a lanthanum ion, serves as the critical intermediate. The thiol-quinone redox shuttle was further shown to mediate the MDH-like activity in the aerobic oxidation of alcohols.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.