Supported Pt Enabled Proton-Driven NAD(P)+ Regeneration for Biocatalytic Oxidation.
Supported Pt Enabled Proton-Driven NAD(P)+ Regeneration for Biocatalytic Oxidation.
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DOI：
10.1021/acsami.2c01743
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发表时间：
2022-04
影响因子：
9.5
通讯作者：
Joseph W. H. Burnett;Hui Chen;Jianwei Li;Ying Li;Shouying Huang;Jiafu Shi;A. Mccue;R. Howe;S. Minteer;Xiaodong Wang
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文献类型：
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作者：
Joseph W. H. Burnett;Hui Chen;Jianwei Li;Ying Li;Shouying Huang;Jiafu Shi;A. Mccue;R. Howe;S. Minteer;Xiaodong Wang
生物催化氧化的利用已从 21 世纪初的小众应用发展成为广泛认可的通用化学合成工具。阻碍商业化的主要缺点之一是对昂贵的烟酰胺腺嘌呤二核苷酸（NAD（P）+）辅因子的依赖，因此它们的再生至关重要。在这里，我们报告了碳负载 Pt 催化剂的设计，该催化剂可以通过质子驱动的 NAD(P)H 氧化并同时形成氢气来再生 NAD(P)+。对碳载体进行修饰以调节 Pt 纳米颗粒的电子性质，结果发现 NAD(P)+ 再生 (TOF = 581 h-1) 的最佳催化剂是碳载富电子 Pt。最后，将多相Pt催化剂应用于不同醇脱氢酶催化的多种醇的生物催化氧化。 Pt催化剂与生物催化体系表现出良好的相容性。其NAD(P)+再生功能成功支持从醇到相应酮或内酯产品的生物催化转化。这项工作为利用协同无机酶催化系统通过 NAD(P)+ 依赖性途径进行化学合成提供了一种有前途的策略。
The utilization of biocatalytic oxidations has evolved from the niche applications of the early 21st century to a widely recognized tool for general chemical synthesis. One of the major drawbacks that hinders commercialization is the dependence on expensive nicotinamide adenine dinucleotide (NAD(P)+) cofactors, and so, their regeneration is essential. Here, we report the design of carbon-supported Pt catalysts that can regenerate NAD(P)+ by proton-driven NAD(P)H oxidation with concurrent hydrogen formation. The carbon support was modified to tune the electronic nature of the Pt nanoparticles, and it was found that the best catalyst for NAD(P)+ regeneration (TOF = 581 h-1) was electron-rich Pt on carbon. Finally, the heterogeneous Pt catalyst was applied in the biocatalytic oxidation of a variety of alcohols catalyzed by different alcohol dehydrogenases. The Pt catalyst exhibited good compatibility with the biocatalytic system. Its NAD(P)+ regeneration function successfully supported biocatalytic conversion from alcohols to corresponding ketone or lactone products. This work provides a promising strategy for chemical synthesis via NAD(P)+-dependent pathways utilizing a cooperative inorganic-enzymatic catalytic system.