Angewandte Chemie International Edition · 2023 · 26 citations · 42 references
PharmacyChemistryMedicinal ChemistryDrug DiscoveryPsychopharmacologySynthetic Medicinal ChemistryLate-stage FunctionalizationRetrosynthetic AnalysisAcid-catalyzed ReactionsAmine FunctionalizationArene FunctionalizationBrønsted Acid CatalysisC-h ActivationControl ExperimentsFunctional Group ToleranceHeterocycle Functionalization
Reversing the conventional site-selectivity of C-H activation provides efficient retrosynthetic disconnections to otherwise unreactive bonds. Described herein is the Brønsted acid-catalyzed reaction that selectively performs meta-amination of anisidines with aliphatic-, heterocyclic- and aromatic amines in a one-pot procedure. In addition to dramatically simplifying the synthesis of meta-substituted anilines, our approach has the advantage of the scalability and remarkable functional group tolerance, including late-stage functionalization of pharmaceutical compounds and natural products. The control experiments and detailed computational analysis provide insight into the reaction mechanism and the origin of meta-selectivity. The protocol extended to the synthesis of challenging tri-aminated arenes and successfully applied for the efficient synthesis of 5-HT6 receptor antagonists, the anti-psychotic drugs viz.. SB-214111, SB-258510, and specifically, anti-schizophrenic drug SB-271046.
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A Meta-Selective Copper-Catalyzed C–H Bond Arylation
Robert J. Phipps, Matthew J. Gaunt · Science · 2009 · 988 citations
Activation of remote meta-C–H bonds assisted by an end-on template
Dasheng Leow, Gang Li, Tian‐Sheng Mei et al. · Nature · 2012 · 914 citations · Full text