具有过氧化物酶和氧化酶活性的铜-白蛋白人工酶，用于立体选择性氧化反应

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-10-22 DOI:10.1021/acscatal.4c0573210.1021/acscatal.4c05732

Maham Liaqat, Emma McDonald, Robert Jervine Valdez Ortega, Aaron Lopes, Flavia Codreanu, Hannah Carlisle, Challa V. Kumar, Xudong Yao, James F. Rusling and Jie He*,

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引用次数: 0

摘要

我们在此报告了一种人工酶的设计方法，即在无催化作用的牛血清白蛋白（Cu-BSA）中加入合成铜复合物，以进行立体选择性氧化。这种以稳定结合的铜络合物为辅助因子的 Cu-BSA 催化剂具有类似过氧化物酶的活性，可催化苯乙烯的环氧化反应，并以高手性选择性（99%）生成 R-苯乙烯环氧化物。随着 Cu2+ 向 Cu+ 的电化学转化，Cu-BSA 还表现出类似氧化酶的活性，可选择性地将氧气还原成过氧化氢（H2O2），这种活性可与其过氧化物酶功能相结合，利用空气推动 C═C 键的氧化。这种人工酶系统有望用于非天然物质的手性选择性转化，并凸显了非催化蛋白质在人工酶设计中的多功能性。

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Cu-Albumin Artificial Enzymes with Peroxidase and Oxidase Activity for Stereoselective Oxidations

We herein report a design of artificial enzymes by incorporating a synthetic copper complex into noncatalytic bovine serum albumin (Cu-BSA) to carry out stereoselective oxidation. This Cu-BSA catalyst with stably bound Cu complex as a cofactor shows peroxidase-like activity to catalyze epoxidation of styrene with high chiral selectivity (>99%) to R-styrene epoxide. With the electrochemical conversion of Cu²⁺ to Cu⁺, Cu-BSA also exhibits oxidase-like activity to selectively reduce oxygen to hydrogen peroxide (H₂O₂), which can be combined with its peroxidase function to drive oxidation of C═C bonds using air. This artificial enzymatic system holds promise for chiral-selective transformations of non-natural substances and highlights the versatility of noncatalytic proteins in the design of artificial enzymes.

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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.