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原料化学品二氯甲烷作为用于化学选择性多组分合成有价值的1,4,2-二恶唑的C1源。

Feedstock chemical dichloromethane as the C1 source for the chemoselective multicomponent synthesis of valuable 1,4,2-dioxazoles.

作者信息

Xie Meng-Jun, Li Xuan, Li Xin-Xin, Wen Li-Hua, Xie Shu-Li, Zhang Ke-Wei, Duan Ya-Nan, Zhang Yao, Li Dong, Xia Hai-Dong

机构信息

College of Chemistry and Chemical Engineering and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Guangdong, 515063, China.

Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031, P. R. China.

出版信息

Commun Chem. 2024 Nov 21;7(1):273. doi: 10.1038/s42004-024-01364-3.

DOI:10.1038/s42004-024-01364-3
PMID:39572701
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11582729/
Abstract

The development of mild and practical strategies to produce value-added fine chemicals directly from inexpensive and readily available commodity chemicals is actively pursued by chemists. However, the application of feedstock chemical dichloromethane (DCM) as the C1 source in organic synthesis is still in its infancy. Herein, we describe a multicomponent strategy for the chemoselective synthesis of valuable 1,4,2-dioxazoles by using DCM as a C1 source. Critical to the success of this process is tuning of the type of nucleophiles to inhibit the easily-occurring side reactions. This approach features mild and simple conditions, excellent chemoselectivity, metal free, and broad substrate scope covering different types of nucleophiles. Furthermore, its synthetic utility is further demonstrated by the preparation of deuterated 1,4,2-dioxazoles, the late-stage functionalization of complex molecules and large-scale synthesis. Preliminary mechanistic studies indicate the dual roles of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) as both a proton scavenger and a nucleophilic catalyst. This work provides not only a platform for DCM application, but also an excellent complementary strategy to the established 1,4,2-dioxazoles synthesis.

摘要

化学家们积极探索开发温和且实用的策略,以直接从廉价易得的商品化学品中生产增值精细化学品。然而,原料化学品二氯甲烷(DCM)作为有机合成中的C1源的应用仍处于起步阶段。在此,我们描述了一种多组分策略,通过使用DCM作为C1源化学选择性合成有价值的1,4,2-二恶唑。该过程成功的关键在于调节亲核试剂的类型以抑制容易发生的副反应。这种方法具有温和简单的条件、出色的化学选择性、无金属以及涵盖不同类型亲核试剂的广泛底物范围。此外,通过制备氘代1,4,2-二恶唑、复杂分子的后期官能团化和大规模合成进一步证明了其合成实用性。初步机理研究表明1,8-二氮杂双环[5.4.0]十一碳-7-烯(DBU)兼具质子清除剂和亲核催化剂的双重作用。这项工作不仅为DCM的应用提供了一个平台,也是已有的1,4,2-二恶唑合成的出色补充策略。

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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/493f/11582729/3923e28cd68a/42004_2024_1364_Sch3_HTML.jpg
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本文引用的文献

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J Org Chem. 2024 May 17;89(10):7047-7057. doi: 10.1021/acs.joc.4c00439. Epub 2024 Apr 26.
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Amidative β-Scission of Alcohols Enabled by Dual Catalysis of Photoredox Proton-Coupled Electron Transfer and Inner-Sphere Ni-Nitrenoid Transfer.光氧化还原质子耦合电子转移与内球镍氮宾转移双催化实现醇的氧化β-裂解
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Vitamin B -Photocatalyzed Cyclopropanation of Electron-Deficient Alkenes Using Dichloromethane as the Methylene Source.
维生素B——以二氯甲烷为亚甲基源对缺电子烯烃进行光催化环丙烷化反应
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Nucleophilic Carbenes Derived from Dichloromethane.源自二氯甲烷的亲核卡宾
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