General access to furan-substituted gem-difluoroalkenes enabled by PFTB-promoted cross-coupling of ene-yne-ketones and difluorocarbene

Chem Sci. 2024 Dec 23. doi: 10.1039/d4sc08247h. Online ahead of print.

Abstract

Replacement of a carbonyl group with fluorinated bioisostere (e.g., CF2[double bond, length as m-dash]C) has been adopted as a key tactical strategy in drug design and development, which typically improves potency and modulates lipophilicity while maintaining biological activity. Consequently, new gem-difluoroalkenation reactions have undoubtedly accelerated this shift, and conceptually innovative practices would be of great benefit to medicinal chemists. Here we describe an expeditous protocol for the direct assembly of furan-substituted gem-difluoroalkenes via PFTB-promoted cross-coupling of ene-yne-ketones and difluorocarbene. In this multi-step tandem reaction process, the furan ring and the gem-difluorovinyl group are constructed simultaneously in an efficient manner. These products can serve as bioisosteres of the α-carbonyl furan core, which is an important scaffold present in natural products and drug candidates. The broad generality and practicality of this method for late-stage modification of bioactive molecules, gram-scale synthesis and versatile derivatisation of products has been described. Biological activity evaluation showed that the gem-difluoroalkene skeleton exhibited dramatic antitumor activity.