Caso Carolina, Altmann Karl-Heinz
Department of Chemistry and Applied Biosciences, Institute of Pharmaceutical Sciences, ETH Zürich, HCI H429, Vladimir-Prelog-Weg 1-5/10, 8093, Zürich, Switzerland.
Chemistry. 2025 Jan 2;31(1):e202402664. doi: 10.1002/chem.202402664. Epub 2024 Nov 14.
Ring systems of all sizes are frequent core or substructures in natural products and they are important elements of many drug molecules, as they often confer high binding affinity to and selectivity for disease-relevant biological targets. A uniform key transformation in the synthesis of such structures is the cyclization step. Among the various approaches that have been developed for ring closure, the intramolecular Suzuki-Miyaura reaction has emerged as a powerful option for the construction of normal- and medium-sized rings as well as macrocycles, due to its stereospecificity, the mild reaction conditions, and the non-toxic nature of the boron by-products. In this review, we summarize the state-of-the-art of the application of intramolecular Suzuki-Miyaura cross-coupling reactions in the construction of (macro)cyclic frameworks of natural products and bioactive molecules of synthetic origin, covering (mostly) examples that have been reported since 2015. Target molecules prepared via intramolecular Suzuki-Miyaura cross-coupling as a key step range from natural products/natural product analogs to synthetic drug candidates, featuring ring sizes from 4 to ≫12. We highlight the utility, scope, and limitations of the reaction for different ring sizes and arrays of functional groups. Where possible, comparisons with other methods of cyclization are provided.
各种大小的环系在天然产物中常常是核心或子结构,并且它们是许多药物分子的重要组成部分,因为它们通常对与疾病相关的生物靶点具有高结合亲和力和选择性。此类结构合成中的一个统一关键转化步骤是环化反应。在已开发的各种闭环方法中,分子内铃木-宫浦反应已成为构建普通大小环、中环以及大环的有力选择,这归因于其立体专一性、温和的反应条件以及硼副产物的无毒性质。在本综述中,我们总结了分子内铃木-宫浦交叉偶联反应在构建天然产物和合成来源的生物活性分子的(大)环骨架中的应用现状,涵盖(主要)自2015年以来报道的实例。通过分子内铃木-宫浦交叉偶联作为关键步骤制备的目标分子范围从天然产物/天然产物类似物到合成药物候选物,其环大小从4到远大于12。我们强调了该反应对于不同环大小和官能团阵列的实用性、适用范围和局限性。在可能的情况下,还提供了与其他环化方法的比较。