Dirhodium tetracarboxylates as catalysts for selective intermolecular C-H functionalization.
Dirhodium tetracarboxylates as catalysts for selective intermolecular C-H functionalization.
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DOI：
10.1038/s41570-019-0099-x
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发表时间：
2019-06
期刊：
影响因子：
--
通讯作者：
Liao K
中科院分区：
文献类型：
--
作者：
Davies HML;Liao K
C-H官能化已成为人们公认的合成复杂分子靶标的一种激动人心的新策略。它没有依赖官能团作为分子组装的控制元素，而是为有机合成提供了一种完全不同的逻辑。为了这类策略的成功，需要开发产生中间体的试剂和催化剂，这些中间体足以使C-H键官能化，但仍然能够区分分子中存在的不同C-H键和其他官能团。最成熟的方法倾向于使用具有固有的C-H官能化有利位置的底物，或者依赖分子内反应来控制反应发生的位置。一种具有挑战性但可能更具通用性的方法是使用催化剂来控制位置选择性，而不需要任何导向基团的影响。能够实现这种转化的一个例子是瞬时金属卡宾的C-H插入化学。对于这些反应，四羧酸氢二钠已被证明是特别有效的催化剂。本综述将重点介绍这类催化剂的发展，并说明它们在控制多种底物的位置选择性和立体选择性C-H官能化方面的有效性。
C–H Functionalization has become widely recognized as an exciting new strategy for the synthesis of complex molecular targets. Instead of relying on functional groups as the controlling elements of how molecules are assembled, it offers a totally different logic for organic synthesis. For this type of strategy to be successful, reagents and catalysts need to be developed that generate intermediates that are sufficiently reactive to functionalize C–H bonds but still capable of distinguishing between the different C–H bonds and other functional groups present in a molecule. The most well-established approaches have tended to use substrates that have inherently a favored site for C–H functionalization or rely on intramolecular reactions to control where the reaction will occur. A challenging but potentially more versatile approach would be to use catalysts to control the site-selectivity without requiring the influence of any directing group. One example that is capable of achieving such transformations is the C–H insertion chemistry of transient metal carbenes. Dirhodium tetracarboxylates have been shown to be especially effective catalysts for these reactions. This review will highlight the development of these dirhodium catalysts and illustrate their effectiveness to control both site-selective and stereoselective C–H functionalization of a wide variety of substrates.
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影响因子：
15
作者：
Ammann, Stephen E.;Rice, Grant T.;White, M. Christina
通讯作者：
White, M. Christina
固有的和引导的 C-H 功能化逻辑。
影响因子：
18.3
作者：
Brueckl, Tobias;Baxter, Ryan D.;Ishihara, Yoshihiro;Baran, Phil S.
通讯作者：
Baran, Phil S.
影响因子：
56.9
作者：
Cook, Amanda K.;Schimler, Sydonie D.;Sanford, Melanie S.
通讯作者：
Sanford, Melanie S.
影响因子：
2.3
作者：
Davies, HML;Yang, J;Nikolai, J
通讯作者：
Nikolai, J
影响因子：
15
作者：
Davies, HML;Ren, PD
通讯作者：
Ren, PD