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通过对光可活化连接体的系统评估揭示可持续且高度可控的芳基偶联反应。

Sustainable and highly controlled aryl couplings revealed by systematic assessment of photoactivatable linkers.

作者信息

Haensch Veit G, Neuwirth Toni, Bergner Alexander, Bruhnke Jakob, Kloss Florian, Hertweck Christian

机构信息

Department of Biomolecular Chemistry, Leibniz Institute for Natural Product Research and Infection Biology (HKI) Beutenbergstr. 11a 07745 Jena Germany

Transfer Group Anti-infectives, Leibniz Institute for Natural Product Research and Infection Biology (HKI) 07745 Jena Germany.

出版信息

Chem Sci. 2022 Apr 13;13(19):5680-5686. doi: 10.1039/d2sc00886f. eCollection 2022 May 18.

Abstract

The controlled synthesis of biphenyls, which play a prominent role in pharmaceuticals, agrochemicals, and liquid crystals, typically requires hazardous organometallic reagents, aryl halides, and heavy metal catalysts. We recently reported a metal-free, photochemical alternative ("photosplicing") for the selective preparation of a wide range of pharmaceutically important biphenyls. Whereas the traceless sulfonamide linker enables and controls the aryl coupling, unwanted toxic byproducts are released. Therefore, we designed over 25 different temporary linkers and tested them for their suitability for the photosplicing reaction in a flow reactor. We found that a surprisingly high number of functional groups enable light-induced aryl fusion and identified a number of linkers for environmentally friendly procedures. We also report that a thiol-ene (click) - photosplicing sequence enables a convenient route to biaryls such as liquid crystals. This work sheds light on thus far neglected photochemistry of temporary linkers, reduces toxic byproducts, and expands the available starting materials for metal-free biphenyl synthesis.

摘要

联苯在药物、农用化学品和液晶中起着重要作用,其可控合成通常需要危险的有机金属试剂、芳基卤化物和重金属催化剂。我们最近报道了一种无金属的光化学替代方法(“光拼接”),用于选择性制备多种具有药学重要性的联苯。虽然无痕磺酰胺连接基能够实现并控制芳基偶联,但会释放出 unwanted 有毒副产物。因此,我们设计了25种以上不同的临时连接基,并在流动反应器中测试了它们对光拼接反应的适用性。我们发现,数量惊人的官能团能够实现光诱导的芳基融合,并确定了一些用于环境友好型工艺的连接基。我们还报道,硫醇-烯(点击)-光拼接序列为合成液晶等联芳基化合物提供了一条便捷途径。这项工作揭示了迄今为止被忽视的临时连接基的光化学,减少了有毒副产物,并扩大了无金属联苯合成可用的起始原料范围。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c9ec/9116350/59a89c413097/d2sc00886f-s5.jpg

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