Guimarães Ricardo L, Lima Dimas J P, Barros Maria Ester S B, Cavalcanti Lívia N, Hallwass Fernando, Navarro Marcelo, Bieber Lothar W, Malvestiti Ivani
Instituto de Ciências Ambientais e Desenvolvimento Sustentável, Universidade Federal da Bahia -Campus Universitário Reitor Edgar Santos, Rua Professor José Seabra S/N - Barreiras - BA - 47805-100, Brazil.
Molecules. 2007 Aug 29;12(9):2089-105. doi: 10.3390/12092089.
The aqueous tin-mediated Barbier reaction affords good to excellent yields and moderate syn diastereoselectivity under basic and acidic conditions. The high yields and stereoselectivity observed in the case of o-substituted aldehydes suggest a cyclic organotin intermediate or transition state in K2HPO4 solution. A practical and efficient aqueous tin allylation of methoxy- and hydroxybenzaldehydes can be carried out in HCl solution in 15 minutes to afford the corresponding homoallylic alcohols in high yields. Aliphatic aldehydes give moderate to excellent yields with reaction times ranging from 30 to 60 minutes. Under these conditions, crotylation gives exclusively the gamma-product and the syn isomer is formed preferentially. For 2-methoxybenzaldehyde, an equilibration of the isomers to a syn/anti ratio of 1:1 can be observed after several hours. Control experiments with radical sources or scavengers give no support for radical intermediates. NMR studies suggest a mechanism involving an organotin intermediate. The major organotin species formed depends on the reaction medium and the reaction time. The use of acidic solution reduces the reaction times, due to the acceleration of the formation of the allyltin(IV) species.
水相锡介导的巴比耶反应在碱性和酸性条件下能提供良好至优异的产率以及适度的顺式非对映选择性。在邻位取代醛的情况下观察到的高产率和立体选择性表明在磷酸氢二钾溶液中存在环状有机锡中间体或过渡态。甲氧基苯甲醛和羟基苯甲醛的实用且高效的水相锡烯丙基化反应可在盐酸溶液中于15分钟内完成,以高产率得到相应的高烯丙醇。脂肪醛的产率适中至优异,反应时间为30至60分钟。在这些条件下,巴豆酰化反应仅生成γ-产物,且优先形成顺式异构体。对于2-甲氧基苯甲醛,数小时后可观察到异构体平衡为顺式/反式比例为1:1。使用自由基源或清除剂进行的对照实验不支持自由基中间体的存在。核磁共振研究表明其机理涉及有机锡中间体。形成的主要有机锡物种取决于反应介质和反应时间。由于烯丙基锡(IV)物种形成的加速,使用酸性溶液可缩短反应时间。