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首页> 外文期刊>Catalysis science & technology >Heterogeneous photoredox synthesis of N-hydroxy-oxazolidinones catalysed by metal-organic frameworks
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Heterogeneous photoredox synthesis of N-hydroxy-oxazolidinones catalysed by metal-organic frameworks

机译：异构photoredox合成N-hydroxy-oxazolidinones催化了有机框架

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摘要

The photoredox conversion of organic functional groups into useful products without the reliance on expensive transition metal-based catalysts has been a major challenge. Here we report the photocatalytic conversion of N-hydroxy-carbamates into N-hydroxy-oxazolidinones using simple metal organic frameworks (MOFs) such as MIL-125-NH2 and UiO-66-NH2 as catalysts in aerobic conditions, with efficiencies and yields comparable to those performed using ground state catalysts. Through sampling increasingly complex structures of carbamates, we found that MOFs induce diasteroselectivities similar to those obtained in solution, which is pivotal in synthesizing natural products and pharmaceuticals, and that the photo-conversion occurred on or near the surface of MOF particles. To provide better mechanistic interpretations on these observations, kinetics studies, quantum yield measurements, and the determination of the photogenerated reactive species were performed. The temperature dependency in the kinetic studies enabled us to identify the photo-redox process as the rate-limiting step of the reaction, a trend that is consistent with using non-porous heterogeneous catalysts like TiO2. The structural traits of the studied MOFs explain how porosity and light absorption can be tuned for better photocatalysts for achieving high yields and selectivities.
机译：photoredox转换的有机功能不依赖组织成有用的产品使用昂贵的过渡金属催化剂是一个重大的挑战。光催化转化N-hydroxy-carbamates到N-hydroxy-oxazolidinones使用简单的金属有机框架(mof)如mil - 125 -氨基和uio - 66 - nh2作为催化剂在有氧条件下,效率和产量可比的使用基态执行催化剂。抽样日益复杂的结构氨基甲酸盐,我们发现mof诱导diasteroselectivities类似在溶液中,它是合成的关键天然产物和药物,photo-conversion发生在或附近财政部粒子的表面。在这些机械的解释观察,动力学研究,量子产率测量的决心photogenerated活性物种进行。温度依赖性的动力学研究使我们能够识别photo-redox过程病原反应步骤的反应,一种趋势这是使用无孔一致异构催化剂二氧化钛。的特点研究了财政部解释孔隙度和更好的光吸收的强度是可以调节的论文的实现高收益选择性。

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