State Key Laboratory of Chemo/Biosensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan 410082, P. R. China.
Angew Chem Int Ed Engl. 2022 Jul 18;61(29):e202117413. doi: 10.1002/anie.202117413. Epub 2022 May 26.
Catalytic asymmetric hydroboration of alkenes is a powerful tool for the synthesis of natural products, agrochemicals, and pharmaceuticals via the versatile transformations of chiral alkyl boronic esters. However, the scope of available alkenes is limited to styrenes, activated alkenes, and compounds with directing groups. The catalytic enantioselective hydroboration of heteroatom-substituted alkenes is rarely explored and those catalyzed by earth-abundant metals are yet to be reported. Herein, we report a cobalt-catalyzed asymmetric hydroboration of ketone-derived silyl enol ethers and provide a convenient approach to access valuable enantiopure β-hydroxy boronic esters. This protocol features mild reaction conditions, a broad substrate scope, and excellent enantioselectivities (up to 99 % ee). This approach was applied in the successful synthesis of salmeterol and albuterol, demonstrating its potential to streamline complex molecule synthesis.
烯烃的催化不对称硼氢化反应是通过手性烷基硼酸酯的多功能转化来合成天然产物、农用化学品和药物的有力工具。然而,可用的烯烃范围仅限于苯乙烯、活化烯烃和带有导向基团的化合物。对于杂原子取代的烯烃的催化对映选择性硼氢化反应很少被探索,而由丰富的地球金属催化的反应尚未被报道。在此,我们报告了钴催化的酮衍生的硅基烯醇醚的不对称硼氢化反应,并提供了一种方便的方法来获得有价值的对映纯β-羟基硼酸酯。该方案具有温和的反应条件、广泛的底物范围和优异的对映选择性(高达 99%ee)。该方法成功应用于沙美特罗和沙丁胺醇的合成,证明了其在简化复杂分子合成方面的潜力。