Trost Barry M, Xu Jiayi
Department of Chemistry, Stanford University, Stanford, California 94305-5080, USA.
J Am Chem Soc. 2005 Mar 9;127(9):2846-7. doi: 10.1021/ja043472c.
The Pd-catalyzed reorganization of enol allyl carbonates to allylated ketones occurs asymmetrically in the presence of chiral ligands previously developed in this group. With 2-methylcyclohexanone, asymmetric regioselective alkylation occurs at the more substituted carbon without complications of polyalkylation. Alkylation to create quaternary centers in indanones and benzonabenone occurs in much higher ee than using tin or lithium enolates. The sense of enantioinduction in tetralones is opposite from the tin and lithium enolate examples. For the first time, asymmetric creation of tertiary centers occurs with high ee (78-99%). The different results between this reaction and the use of lithium or tin enolates suggest different mechanisms may be involved.
在该研究组之前开发的手性配体存在下,钯催化的烯醇烯丙基碳酸酯重排为烯丙基化酮的反应以不对称方式进行。对于2-甲基环己酮,在取代较多的碳上发生不对称区域选择性烷基化,而没有多烷基化的复杂情况。在茚满酮和苯并萘醌中生成季碳中心的烷基化反应,其对映体过量值(ee)比使用锡或锂烯醇盐时高得多。在四氢萘酮中对映体诱导的方向与锡和锂烯醇盐的例子相反。首次以高对映体过量值(78 - 99%)实现了叔碳中心的不对称构建。该反应与使用锂或锡烯醇盐的不同结果表明可能涉及不同的机制。