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Optically pure monosubstituted [n]paracyclophanes are promising candidates for material synthesis, asymmetric catalysis, and drug discovery. Thus far, only a few catalytic asymmetric synthesis processes have been reported for assessing these strained atropisomers. In this study, we describe a highly enantioselective synthesis of monosubstituted [n]paracyclophanes by combining desymmetrization and kinetic resolution. The proposed protocol involves Pd-catalyzed atroposelective C-H bond olefination enabled by a monoprotected amino acid ligand, which affords a variety of monosubstituted [n]paracyclophanes with excellent enantioselectivity (≥99 %ee). Thermodynamic experiments are conducted to investigate the racemization barrier. The synthesized monosubstituted [n]paracyclophanes exhibit vivid fluorescence and impressive circularly polarized luminescence. Further, the emission color and dissymmetry factor can be tuned and controlled by switching the substituent on the benzene ring of the cyclophanes.
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http://dx.doi.org/10.1002/chem.202404610 | DOI Listing |
Chemistry
February 2025
Key Laboratory of Radiopharmaceuticals, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing, 100875, China.
Optically pure monosubstituted [n]paracyclophanes are promising candidates for material synthesis, asymmetric catalysis, and drug discovery. Thus far, only a few catalytic asymmetric synthesis processes have been reported for assessing these strained atropisomers. In this study, we describe a highly enantioselective synthesis of monosubstituted [n]paracyclophanes by combining desymmetrization and kinetic resolution.
View Article and Find Full Text PDFACS Catal
May 2024
Department of Chemistry, Emory University, 1515 Dickey Drive, Atlanta, Georgia 30322, United States.
Chiral [2.2]paracyclophane derivatives are of considerable interest because of their potential in asymmetric catalysis and the development of chiral materials. This study describes the scope of rhodium-catalyzed reactions of aryldiazoacetates with [2.
View Article and Find Full Text PDFOrg Biomol Chem
January 2012
Department of Chemistry, University of Florida, Gainesville, FL 32611-7200, USA.
The product of S(N)Ar addition of the enolate of ethyl acetoacetate to perfluoro[2.2]para-cyclophane exists entirely as its enol tautomer 5. This enol exhibits two NMR signals for its enolic proton, and these signals were shown to derive from the presence of two, equal energy conformations that were observable as distinct, stable conformations at room temperature, but which when heated, interconverted with an energy barrier of 23.
View Article and Find Full Text PDFMagn Reson Chem
March 2011
Chemistry Department, University of Florida, Gainesville, 32611-7200, USA.
In the process of studying the chemistry of perfluoro[2.2]paracyclophanes (PFPCs), a novel class of compounds, it became necessary to identify some disubstituted products. To achieve this goal, we characterize in this work some monosubstituted PFPCs, identifying their (19)F-(19) F coupling patterns, and establishing a methodology for the assignment of their (19)F chemical shifts.
View Article and Find Full Text PDFJ Org Chem
September 2009
Department of Chemistry, P.O. Box 117200, University of Florida, Gainesville, Florida 32611-7200, USA.
The aromatic rings of perfluoro[2.2]paracyclophane are extremely reactive with respect to nucleophilic substitution reactions. This paper emphasizes products of monosubstitution by hydroxide, alkoxide, thiolate, enolate, and amine nucleophiles.
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