聚七嗪亚胺上Rb-Ir催化对上甘油不对称光氧化制羟基乙酸的研究

IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Zhenyuan Teng, Zhenzong Zhang, Ying Tu, Qitao Zhang, Nan Jian, Liujun Yang, Jiadong Xiao, Jie Ding, Longzhen Huang, Ohno Teruhsia, Chengyin Wang, Dengsong Zhang, Han Yu, Jianmei Lu, Chenliang Su, Bin Liu
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引用次数: 0

摘要

甘油(GLY)选择性不对称氧化合成羟基乙酸(HPA)为手性药物合成提供了一种有吸引力的方法,但该方法具有很高的挑战性。在此,我们开发了一种光催化方法,通过修饰在聚七嗪亚胺框架上的铷(Rb)和铱(Ir)催化对,实现了GLY非均相选择性光氧化制HPA。Rb位点通过末端的-OH基团有效吸附GLY分子,从而抑制其在光反应过程中的氧化,而Ir位点增强氧还原反应,Ir上原位生成的表面氧还原自由基可以保护光氧化过程中产生的活性c中心自由基中间体。Rb和Ir位点的空间排列有利于氢的提取——GLY光氧化的重要速率决定步骤——并保护C3自由基中间体免于过度氧化。该光催化体系在可见光照射下合成HPA的效率很高(每克光催化剂每小时约8000 μmol HPA)。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Asymmetric photooxidation of glycerol to hydroxypyruvic acid over Rb–Ir catalytic pairs on poly(heptazine imides)

Asymmetric photooxidation of glycerol to hydroxypyruvic acid over Rb–Ir catalytic pairs on poly(heptazine imides)

Selective asymmetric oxidation of glycerol (GLY) to hydroxypyruvic acid (HPA) offers an attractive approach for chiral drug synthesis, but this process is highly challenging. Here we develop a photocatalytic method to achieve heterogeneous selective photooxidation of GLY to HPA over rubidium (Rb) and iridium (Ir) catalytic pairs decorated on a poly(heptazine imide) framework. The Rb sites effectively adsorb GLY molecules through the terminal –OH groups, thus inhibiting their oxidation during photoreaction, while the Ir sites enhance the oxygen reduction reaction and the in situ generated surficial oxygen-reduction radicals on Ir can protect the reactive C-centred radical intermediates produced during photooxidation. The spatial arrangement of Rb and Ir sites facilitates hydrogen extraction—an essential rate-determining step for GLY photooxidation—and protects C3 radical intermediates from overoxidation. This photocatalytic system achieves a remarkable productivity for HPA synthesis (~8,000 μmol of HPA per gram of photocatalyst per hour) under visible-light illumination.

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来源期刊
Nature nanotechnology
Nature nanotechnology 工程技术-材料科学:综合
CiteScore
59.70
自引率
0.80%
发文量
196
审稿时长
4-8 weeks
期刊介绍: Nature Nanotechnology is a prestigious journal that publishes high-quality papers in various areas of nanoscience and nanotechnology. The journal focuses on the design, characterization, and production of structures, devices, and systems that manipulate and control materials at atomic, molecular, and macromolecular scales. It encompasses both bottom-up and top-down approaches, as well as their combinations. Furthermore, Nature Nanotechnology fosters the exchange of ideas among researchers from diverse disciplines such as chemistry, physics, material science, biomedical research, engineering, and more. It promotes collaboration at the forefront of this multidisciplinary field. The journal covers a wide range of topics, from fundamental research in physics, chemistry, and biology, including computational work and simulations, to the development of innovative devices and technologies for various industrial sectors such as information technology, medicine, manufacturing, high-performance materials, energy, and environmental technologies. It includes coverage of organic, inorganic, and hybrid materials.
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