Department of Chemistry, The City College of New York, 160 Convent Avenue, New York, New York 10031, USA.
Nat Chem. 2013 Jul;5(7):607-12. doi: 10.1038/nchem.1652. Epub 2013 May 19.
The development of transition metal-catalysed cross-coupling reactions has greatly influenced the manner in which the synthesis of complex organic molecules is approached. A wide variety of methods are now available for the formation of C(sp(2))-C(sp(2)) bonds, and more recent work has focused on the use of C(sp(3)) electrophiles and nucleophiles. The use of secondary and tertiary alkyl nucleophiles in cross-coupling reactions remains a challenge because of the propensity of these alkyl groups to isomerize under the reaction conditions. Here, we report the development of a general Pd-catalysed process for the stereoretentive cross-coupling of secondary alkyl azastannatrane nucleophiles with aryl chlorides, bromides, iodides and triflates. Coupling partners with a wide range of electronic characteristics are well tolerated. The reaction occurs with minimal isomerization of the secondary alkyltin nucleophile, and with retention of absolute configuration. This process constitutes the first general method to use secondary alkyltin reagents in cross-coupling reactions.
过渡金属催化的交叉偶联反应的发展极大地影响了复杂有机分子合成的方式。现在有各种各样的方法可用于形成 C(sp(2))-C(sp(2))键,最近的工作重点是使用 C(sp(3))亲电试剂和亲核试剂。由于这些烷基在反应条件下容易异构化,因此在交叉偶联反应中使用仲烷基和叔烷基亲核试剂仍然是一个挑战。在这里,我们报告了一种通用的 Pd 催化方法的发展,用于立体保留性的仲烷基氮杂锡烷亲核试剂与芳基氯化物、溴化物、碘化物和三氟甲磺酸酯的交叉偶联。具有广泛电子特性的偶联伙伴可以很好地耐受。反应中仲烷基锡亲核试剂的异构化最小,并且保留了绝对构型。该过程构成了首次在交叉偶联反应中使用仲烷基锡试剂的通用方法。