Chen Yiding, Murray Philip R D, Davies Alyn T, Willis Michael C
Department of Chemistry, Chemistry Research Laboratory , University of Oxford , Mansfield Road , Oxford OX1 3TA , United Kingdom.
J Am Chem Soc. 2018 Jul 18;140(28):8781-8787. doi: 10.1021/jacs.8b04532. Epub 2018 Jul 2.
First introduced into medicines in the 1930s, the sulfonamide functional group continues to be present in a wide range of contemporary pharmaceuticals and agrochemicals. Despite their popularity in the design of modern bioactive molecules, the underpinning methods for sulfonamide synthesis are essentially unchanged since their introduction, and rely on the use of starting materials with preinstalled sulfur-functionality. Herein we report a direct single-step synthesis of sulfonamides that combines two of the largest monomer sets available in discovery chemistry, (hetero)aryl boronic acids and amines, along with sulfur dioxide, using a Cu(II) catalyst, to deliver a broad range of sulfonamides. Sulfur dioxide is provided by the surrogate reagent DABSO. The reaction tolerates broad variation in both coupling partners, including aryl, heteroaryl and alkenyl boronic acids, as well as cyclic and acyclic alkyl secondary amines, and primary anilines. We validate the method by showing that a variety of drugs, and drug-fragments, can be incorporated into the process.
磺胺官能团于20世纪30年代首次被引入药物领域,至今仍存在于众多现代药品和农用化学品中。尽管它们在现代生物活性分子设计中很受欢迎,但自引入以来,磺胺合成的基本方法基本未变,且依赖于使用预先安装了硫官能团的起始原料。在此,我们报告了一种磺胺的直接一步合成法,该方法将发现化学中可用的两个最大单体集,即(杂)芳基硼酸和胺,与二氧化硫结合,使用铜(II)催化剂,以制备多种磺胺。二氧化硫由替代试剂DABSO提供。该反应对两种偶联伙伴的广泛变化都具有耐受性,包括芳基、杂芳基和烯基硼酸,以及环状和非环状烷基仲胺和伯苯胺。我们通过证明多种药物和药物片段可纳入该过程来验证该方法。