Grantham Helena F, Lee Robert J, Wardas Grzegorz M, Mistry Jai-Ram, Elsegood Mark R J, Wright Iain A, Pritchard Gareth J, Kimber Marc C
Department of Chemistry, School of Science, Loughborough University, Loughborough LE11 3TU, U.K.
The School of Chemistry, University of Edinburgh, Joseph Black Building, Edinburgh EH9 3FJ, U.K.
J Org Chem. 2024 Jan 5;89(1):484-497. doi: 10.1021/acs.joc.3c02237. Epub 2023 Dec 24.
The direct transformation of 1,3-dienes into valuable 2,5-diarylfurans using transition-metal-free conditions is presented. By employing a simple oxidation─dehydration sequence on readily accessible 1,3-dienes, important 2,5-diarylfuran building blocks frequently used in medicinal and material chemistry are prepared. The oxidation step is realized using singlet oxygen, and the intermediate endoperoxide is dehydrated under metal-free conditions and at ambient temperature using the Appel reagent. Notably, this sequence can be streamlined into continuous flow, thereby eliminating the isolation of the intermediate, often unstable endoperoxide. This leads to a significant improvement in isolated yields (ca. 27% average increase) of the 2,5-diarylfurans while also increasing safety and reducing waste. Our transition-metal-free synthetic approach to 2,5-diarylfurans delivers several important furan building blocks used commonly in medicinal chemistry and as optoelectronic materials, including short-chain linearly conjugated furan oligomers. Consequently, we also complete a short study of the optical and electrochemical properties of a selection of these novel materials.
本文介绍了在无过渡金属条件下将1,3 - 二烯直接转化为有价值的2,5 - 二芳基呋喃的方法。通过对易于获得的1,3 - 二烯进行简单的氧化 - 脱水步骤,制备了在药物化学和材料化学中常用的重要2,5 - 二芳基呋喃结构单元。氧化步骤使用单线态氧实现,中间的内过氧化物在无金属条件下和室温下使用阿佩尔试剂进行脱水。值得注意的是,该步骤可以简化为连续流动过程,从而避免了通常不稳定的中间内过氧化物的分离。这使得2,5 - 二芳基呋喃的分离产率显著提高(平均提高约27%),同时还提高了安全性并减少了废物产生。我们用于合成2,5 - 二芳基呋喃的无过渡金属方法提供了几种在药物化学中常用的重要呋喃结构单元以及用作光电材料的结构单元,包括短链线性共轭呋喃低聚物。因此,我们还对这些新型材料中的一部分进行了光学和电化学性质的简短研究。