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卡宾和光催化剂催化的羧酸和酰基咪唑的脱羧基自由基偶联反应生成酮。

Carbene and photocatalyst-catalyzed decarboxylative radical coupling of carboxylic acids and acyl imidazoles to form ketones.

机构信息

Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Guizhou University, Huaxi District, Guiyang, China.

Division of Chemistry & Biological Chemistry, School of Physical & Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore.

出版信息

Nat Commun. 2022 May 23;13(1):2846. doi: 10.1038/s41467-022-30583-2.

Abstract

The carbene and photocatalyst co-catalyzed radical coupling of acyl electrophile and a radical precursor is emerging as attractive method for ketone synthesis. However, previous reports mainly limited to prefunctionalized radical precursors and two-component coupling. Herein, an N-heterocyclic carbene and photocatalyst catalyzed decarboxylative radical coupling of carboxylic acids and acyl imidazoles is disclosed, in which the carboxylic acids are directly used as radical precursors. The acyl imidazoles could also be generated in situ by reaction of a carboxylic acid with CDI thus furnishing a formally decarboxylative coupling of two carboxylic acids. In addition, the reaction is successfully extended to three-component coupling by using alkene as a third coupling partner via a radical relay process. The mild conditions, operational simplicity, and use of carboxylic acids as the reacting partners make our method a powerful strategy for construction of complex ketones from readily available starting materials, and late-stage modification of natural products and medicines.

摘要

卡宾和光催化剂共同催化的酰基亲电试剂和自由基前体的自由基偶联,是一种新兴的酮类化合物合成方法。然而,之前的报道主要局限于预官能化的自由基前体和两组分偶联。在此,我们公开了一种 N-杂环卡宾和光催化剂催化的羧酸和酰基咪唑的脱羧基自由基偶联反应,其中羧酸直接作为自由基前体。酰基咪唑也可以通过羧酸与 CDI 的反应原位生成,从而实现了两种羧酸的形式上的脱羧基偶联。此外,通过自由基接力过程,该反应还成功地扩展到三组分偶联,使用烯烃作为第三个偶联试剂。温和的条件、操作简单以及羧酸作为反应试剂,使我们的方法成为了一种从易得的起始原料构建复杂酮类化合物以及天然产物和药物的后期修饰的有力策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3d67/9126905/67e60aa2f32b/41467_2022_30583_Fig1_HTML.jpg

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