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.
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http://dx.doi.org/10.1038/s41557-024-01730-7 | DOI Listing |
Nat Chem
February 2025
Department of Chemistry, National University of Singapore, Singapore, Singapore.
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.
View Article and Find Full Text PDFJ Org Chem
December 2024
Department of Chemistry & Biochemistry, University of California, Santa Barbara, California 93106, United States.
Environmentally respectful methods for generating and utilizing difluorocarbene (:CF) in the synthesis of a wide array of valuable difluoromethylated compounds are disclosed. In particular, the insertion of the CF moiety into aromatic/heteroaromatic alcohols, thiols, olefins, and alkynes under neat or aqueous micellar catalysis conditions is demonstrated. These methods yield both satisfactory results and significantly lower E-Factors compared to traditional synthetic approaches.
View Article and Find Full Text PDFACS Catal
July 2024
Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
Fluoroalkyl fragments have played a critical role in the design of pharmaceutical and agrochemical molecules in recent years due to the enhanced biological properties of fluorinated molecules compared to their non-fluorinated analogues. Despite the potential advantages conferred by incorporating a difluoromethyl group in organic compounds, industrial adoption of difluoromethylation methods lags behind fluorination and trifluoromethylation. This is due in part to challenges in applying common difluoromethyl sources towards industrial applications.
View Article and Find Full Text PDFJ Am Chem Soc
June 2024
Key Laboratory of Fluorine and Nitrogen Chemistry and Advanced Materials (Chinese Academy of Sciences), Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, Chinese Academy of Sciences, 345 Lingling Road, Shanghai 200032, China.
Angew Chem Int Ed Engl
July 2024
Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science, Westlake University, Hangzhou, 310024, China.
Microenvironment regulation of M-N single-atom catalysts (SACs) is a promising way to tune their catalytic properties toward the electrochemical CO reduction reaction. However, strategies that can effectively introduce functional groups around the M-N sites through strong covalent bonding and under mild reaction conditions are highly desired. Taking the hydrophilic Ni-N SAC as a representative, we report herein a [2+1] cycloaddition reaction between Ni-N and in situ generated difluorocarbene (FC:), and enable the surface fluorocarbonation of Ni-N, resulting in the formation of a super-hydrophobic Ni-N-CF catalyst.
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