Chambournier G, Gawley R E
Department of Chemistry, University of Miami, Coral Gables, Florida 33124, USA.
Org Lett. 2000 Jun 1;2(11):1561-4. doi: 10.1021/ol005770u.
[equation--see text] 2-Tributylstannyl-N-methylpiperidines that are conformationally locked by a 4-tert-butyl substituent were evaluated in transmetalations (Sn-Li exchange) and reactions with electrophiles. When the tin is equatorial, transmetalation occurs smoothly as does reaction with carbonyl electrophiles. Alkyl halides seem to undergo single electron transfer reactions, affording nonselective alkylation products, along with products of radical disproportionation. In a surprise, an axially oriented tin failed to transmetalate, suggesting that a synclinal relationship between the nitrogen lone pair and the carbon-tin bond is a requirement for transmetalation.
[方程式 - 见正文] 被4-叔丁基取代基构象锁定的2-三丁基锡基-N-甲基哌啶在金属转移反应(锡-锂交换)以及与亲电试剂的反应中进行了评估。当锡处于平伏键时,金属转移反应以及与羰基亲电试剂的反应都能顺利发生。卤代烃似乎会发生单电子转移反应,生成非选择性的烷基化产物以及自由基歧化产物。令人惊讶的是,轴向取向的锡无法进行金属转移反应,这表明氮孤对与碳 - 锡键之间的顺错关系是金属转移反应的一个必要条件。