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端炔烃向E-烯烃取代的稳定硫鎓叶立德的无催化剂直接烃基化反应

Catalyst-Free Direct Hydrocarbonation of Terminal Alkynes Toward E-Alkene Substituted Stabilized Sulfoxonium Ylides.

作者信息

Wu Haiting, Xu Yougen, Lin An, Liu Jingyuan, Chen Huanjun, Xie Shimin, Su Lebin

机构信息

School of Pharmaceutical Sciences, Guangzhou Laboratory, Guangzhou Medical University, Guangzhou, 511436, China.

Bioland Laboratory, Guangzhou, 510005, China.

出版信息

Adv Sci (Weinh). 2025 Jun;12(22):e2417362. doi: 10.1002/advs.202417362. Epub 2025 Apr 2.

DOI:10.1002/advs.202417362
PMID:40171892
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12165105/
Abstract

Amide and alkene moieties are frequently found in natural products and are privileged structures in pharmaceuticals and agrochemicals. Moreover, vinyl sulfoxonium ylide can be converted into a broad range of high-value compounds, thus they have been widely employed in organic synthesis. However, the synthesis of alkene-substituted amide-sulfoxonium ylides via intermolecular hydrocarbonation of alkynes remains underexplored. This study describes the development of a high-throughput approach to provide diverse functionalized E-alkene substituted (hetero)amide-sulfoxonium ylides. The reaction occurs under mild metal-free conditions, employing amide-sulfoxonium ylides as highly effective nucleophiles, which participate in Michael addition reactions with various substituted alkynes, such as esters, thioesters, ketones, amides, and sulfones. This low-cost, operationally simple approach has a broad substrate scope, high functional group compatibility, and excellent regio- and stereoselectivity, making it suitable for the transformation of structurally complex molecules. Furthermore, the obtained stabilized sulfoxonium ylide products are directly useful for the synthesis of diverse valuable 1,5-dicarbonyl and thiabenzene 1-oxide compounds.

摘要

酰胺和烯烃部分在天然产物中经常出现,并且是药物和农用化学品中的优势结构。此外,乙烯基砜叶立德可以转化为多种高价值化合物,因此它们已被广泛应用于有机合成中。然而,通过炔烃的分子间烃化反应合成烯烃取代的酰胺-砜叶立德仍未得到充分研究。本研究描述了一种高通量方法的开发,以提供多种功能化的E-烯烃取代的(杂)酰胺-砜叶立德。该反应在温和的无金属条件下进行,使用酰胺-砜叶立德作为高效亲核试剂,其与各种取代的炔烃,如酯、硫酯、酮、酰胺和砜,发生迈克尔加成反应。这种低成本、操作简单的方法具有广泛的底物范围、高官能团兼容性以及出色的区域和立体选择性,使其适用于结构复杂分子的转化。此外,所得到的稳定砜叶立德产物可直接用于合成多种有价值的1,5-二羰基和噻苯1-氧化物化合物。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/de4829006701/ADVS-12-2417362-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/0dde81e75e8d/ADVS-12-2417362-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/5ceee961b045/ADVS-12-2417362-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/6dc2917663f1/ADVS-12-2417362-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/8c7843c17b9c/ADVS-12-2417362-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/333ccf839f64/ADVS-12-2417362-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/b69ad179c567/ADVS-12-2417362-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/de4829006701/ADVS-12-2417362-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/0dde81e75e8d/ADVS-12-2417362-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/5ceee961b045/ADVS-12-2417362-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/6dc2917663f1/ADVS-12-2417362-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/8c7843c17b9c/ADVS-12-2417362-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/333ccf839f64/ADVS-12-2417362-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/b69ad179c567/ADVS-12-2417362-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/525c/12165105/de4829006701/ADVS-12-2417362-g007.jpg

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