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一种灵活的应变夹心化合物方法:桥位为硼、镓、硅和锡的手性[1]二茂铁。

A flexible approach to strained sandwich compounds: chiral [1]ferrocenophanes with boron, gallium, silicon, and tin in bridging positions.

机构信息

Department of Chemistry, University of Saskatchewan, 110 Science Place, Saskatoon, Saskatchewan S7N 5C9 (Canada).

出版信息

Chemistry. 2013 Sep 27;19(40):13408-17. doi: 10.1002/chem.201301991. Epub 2013 Aug 14.

Abstract

The enantiomerically pure dibromoferrocene 3 [(Sp,Sp )-1,1'-dibromo-2,2'-di(isopropyl)ferrocene], equipped with two iPr groups in α positions, was prepared using known "Ugi amine" chemistry. Species 3 was targeted in order to gain access to new [1]ferrocenophanes ([1]FCPs) to be used as monomers for ring-opening polymerization. The iPr groups on the sandwich unit were introduced to stabilize bridging moieties, as well as to increase solubilities of targeted metallopolymers. The planar chiral dibromide 3 can quantitatively be lithiated at 0°C [2 equiv nBuLi, hexanes/thf (9:1), 30 min]. Salt-metathesis reactions with respective element dichloride species gave chiral [1]FCPs with a variety of bridging moieties [ERx =Ga[2-(Me2NCH2)C6H4] (4 a), SiMe2 (4 b), SntBu2 (4 c), BNiPr2 (4 d)]. The new [1]FCPs were fully characterized including single-crystal X-ray analysis. The stabilizing iPr groups on the Cp rings increase the thermal stabilities of 4 b-d compared to known [1]FCPs, equipped with the same bridging moieties. All three compounds 4 b-d are volatile and could be isolated by vacuum sublimation. Our new approach to [1]FCPs has the potential to overcome many of the existing difficulties in ferrocenophane chemistry, such as limited stability of starting monomers and low solubilities of resulting polyferrocenes.

摘要

对映体纯二溴二茂铁 3 [(Sp,Sp)-1,1'-二溴-2,2'-二(异丙基)二茂铁],在α位带有两个 iPr 基团,使用已知的“Ugi 胺”化学方法制备。选择 3 是为了获得新的[1]茂铁并环([1]FCPs),用作开环聚合的单体。夹心单元上的 iPr 基团用于稳定桥接基团,并增加目标金属聚合物的溶解度。平面手性二溴化物 3 可以在 0°C 定量锂化[2 当量 nBuLi,己烷/THF(9:1),30 分钟]。与各自元素二氯化物的盐-复分解反应得到具有各种桥接基团的手性[1]FCPs [ERx = Ga[2-(Me2NCH2)C6H4](4 a),SiMe2(4 b),SntBu2(4 c),BNiPr2(4 d)]。新的[1]FCPs 经过全面表征,包括单晶 X 射线分析。Cp 环上的稳定 iPr 基团增加了 4 b-d 与具有相同桥接基团的已知[1]FCPs 的热稳定性。所有三种化合物 4 b-d 都是挥发性的,可以通过真空升华分离。我们的新方法[1]FCPs 有可能克服茂铁并环化学中存在的许多困难,例如起始单体的稳定性有限和所得聚二茂铁的溶解度低。

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