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催化二氟卡宾插入反应可用于制备含氟氧杂环丁烷电子等排体。

Catalytic difluorocarbene insertion enables access to fluorinated oxetane isosteres.

作者信息

Tan Tong-De, Zhou Fang, Quirion Kevin P, Wang Yu-Qi, Ng Daniel Zhi Wei, Luo Xiaohua, Chan Eric Chun Yong, Liu Peng, Koh Ming Joo

机构信息

Department of Chemistry, National University of Singapore, Singapore, Singapore.

Department of Chemistry, University of Pittsburgh, Pittsburgh, PA, USA.

出版信息

Nat Chem. 2025 May;17(5):719-726. doi: 10.1038/s41557-024-01730-7. Epub 2025 Feb 20.

Abstract

Skeletal editing of heterocyclic building blocks offers an appealing way to expand the accessible chemical space by diversifying molecular scaffolds for drug discovery. Despite the recent boom in this area, catalytic strategies that directly introduce fluorine into the backbone of small-ring heterocycles remain rare owing to the challenges of strain-induced ring cleavage and defluorination. Here we describe a copper-catalysed approach for skeletal expansion of oxygen heterocycles by reaction with a difluorocarbene species generated in situ to induce carbon atom insertion. The α,α-difluoro-oxetane products are potential surrogates of oxetane, β-lactone and carbonyl pharmacophores on the basis of their computed molecular properties and electrostatic potential maps. The utility of this approach is highlighted by synthesis of various drug-like molecules and fluorinated isosteres of biologically active compounds. Experimental and computational investigations provide insight into the mechanism and the unique role of the copper catalyst in promoting both ring-opening and cyclization steps of the reaction.

摘要

对杂环结构单元进行骨架编辑,为药物发现提供了一种通过多样化分子支架来扩展可及化学空间的诱人方法。尽管该领域近来发展迅速,但由于应变诱导的环开裂和脱氟的挑战,直接将氟引入小环杂环骨架的催化策略仍然很少见。在此,我们描述了一种铜催化的方法,通过与原位生成的二氟卡宾物种反应以诱导碳原子插入,实现氧杂环的骨架扩展。基于计算得到的分子性质和静电势图,α,α-二氟氧杂环丁烷产物是氧杂环丁烷、β-内酯和羰基药效团的潜在替代物。各种类药物分子和生物活性化合物的氟化电子等排体的合成突出了该方法的实用性。实验和计算研究深入了解了反应机理以及铜催化剂在促进反应的开环和环化步骤中的独特作用。

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