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Ag/Co-Bimetallic Cooperation in the C–H Functionalization of Aliphatic Amides with Propiolic Acids
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-12-16 , DOI: 10.1021/acscatal.4c05918
Andrés García-Viada, Emma Duro, Celia Sánchez-González, Inés Alonso, Nuria Rodríguez, Javier Adrio, Juan C. Carretero

We herein describe the high-valent cobalt-catalyzed C(sp3)–H functionalization of amide derivatives with silver acetylides generated in situ. The reaction proceeds under kinetic control at 60 °C, with a catalyst loading of 5 mol %. These extraordinarily mild conditions for Co-catalysis enable the synthesis of 5-(Z)-ethylidene pyrrolidin-2-one derivatives in good yield and selectivity. Density functional theory calculations have revealed a unique mechanism involving Co–Ag bimetallic species, rationalizing the nature of the catalytically active species and the role of each additive.

中文翻译:


Ag/Co-Bi金属合作在脂肪族酰胺与丙酸的 C-H 官能化中的作用



我们在此描述了酰胺衍生物的高价钴催化 C(sp3)–H 官能化与原位生成的乙酰银。反应在 60 °C 的动力学控制下进行,催化剂负载量为 5 mol %。这些非常温和的共催化条件能够以良好的产率和选择性合成 5-(Z)-亚乙基吡咯烷-2-酮衍生物。密度泛函理论计算揭示了涉及 Co-Ag 双金属物质的独特机制,使催化活性物质的性质和每种添加剂的作用合理化。
更新日期:2024-12-16
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