Zhu Huilong, Sun Dingcheng, Zhang Shengxiang, Chen Junning, Xu Zhou
Jiangsu Key Laboratory of New Drug Research and Clinical Pharmacy, School of Pharmacy, Xuzhou Medical University, Xuzhou, China.
Chemistry. 2024 Sep 25;30(54):e202401830. doi: 10.1002/chem.202401830. Epub 2024 Sep 9.
The catalytic direct hydroarylation of alkynamides is a highly efficient approach for accessing functionalized trisubstituted arylalkenes with amide groups. Herein, we report a rhodium-catalyzed pyridylation of alkynamides with pyridylboronic acids, producing a variety of primary, secondary, and tertiary enamides with high yields (up to 94 %). This reaction demonstrates broad tolerance towards various alkyl and aryl functional groups, providing convenient access to a diverse array of alkenylpyridine derivatives. To demonstrate potential applications in late-stage hydropyridylation, we synthesized α,β-unsaturated ketones, aldehydes, and esters with high yields from the pyridylation product of Weinreb amides. This indirect expansion of the substrate scope enhances the practicality of this strategy. Additionally, the α,β-unsaturated ketone obtained can be further reduced to yield a chiral alcohol with a 99 % ee, further demonstrating the versatility and potential utility of this approach.
炔酰胺的催化直接氢芳基化是一种高效合成带有酰胺基的官能化三取代芳基烯烃的方法。在此,我们报道了一种铑催化的炔酰胺与吡啶硼酸的吡啶化反应,可高产率(高达94%)地生成各种伯、仲和叔烯酰胺。该反应对各种烷基和芳基官能团具有广泛的耐受性,为多种烯基吡啶衍生物的合成提供了便利。为了证明在后期氢吡啶化中的潜在应用,我们从Weinreb酰胺的吡啶化产物高产率地合成了α,β-不饱和酮、醛和酯。底物范围的这种间接扩展提高了该策略的实用性。此外,所得的α,β-不饱和酮可进一步还原得到ee值为99%的手性醇,进一步证明了该方法的多功能性和潜在实用性。