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基于酸和氨基基基的易斯对化学

Adrien T Normand^1,2, Constantin G Daniliuc¹, Birgit Wibbeling¹

¹Organisch-Chemisches Institut, Westfälische Wilhelms-Universität Münster , Corrensstraße 40, 48149 Münster, Germany.

Journal of the American Chemical Society

|July 22, 2015

概括

合成了含有和联体的新复合物. 这些复合物催化了油脂化,并与二氧化碳和碳基反应,在有机金属化学中表现出多样性的反应性.

科学领域:

有机金属化学
催化剂
协调化学

背景情况:

从中性复合物中提取甲基是产生催化活性物种的关键步骤.
对于设计新的催化剂来说,了解复合物的电子和硬质效应至关重要.
化学中的氨基和联体的反应性是一个活跃的研究领域.

研究的目的:

通过甲基抽象用和联体合成新的复合物.
研究这些新复合物的结构性质,包括Zr/N-π相互作用.
探索合成的复合物的催化活性和反应性与各种基质.

主要方法:

使用基易斯酸合成中性[Cp2ZrMe(ERR') 复合物 (1),然后进行甲基提取.
用X射线结晶学来确定胺复合物的结构[Cp2Zr(NPh2) ][MeB(C6F5) ] (2d) 和[Cp2Zr(N(t) BuAr]][B(C6F5) ] (2e').
素和素的催化化,二氧化碳结合研究以及与甲和乙烯的反应.

主要成果:

通过甲基抽象形成阴离子复合物[Cp2Zr(ERR') ][X] (2).
结构分析揭示了体依赖的Zr/N-π相互作用.
复合物2在化中表现出催化活性,并与二氧化碳,甲和基发生反应,形成包括易斯对在内的新产物.

结论:

甲基抽象策略提供了具有和联体的多功能阴离子复合物.
合成的复合物具有显著的催化潜力和与小分子和不和基质的独特反应模式.
这项工作扩大了介导转换的范围,并突出了连接体设计在催化中的重要性.

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