title: General Enantioselective C-H Activation with Efficiently Tunable Cyclopentadienyl Ligands.
abstract: Cyclopentadienyl (Cp) ligands enable efficient steering of various transition-metal-catalyzed transformations, in particular enantioselective C-H activation. Currently only few chiral Cp ligands are available. Therefore, a conceptually general approach to chiral Cp ligand discovery would be invaluable as it would enable the discovery of applicable Cp ligands and to efficiently and rapidly vary and tune their structures. Herein, we describe the three-step gram-scale synthesis of a structurally diverse and widely applicable chiral Cp ligand collection (JasCp ligands) with highly variable and adjustable structures. Their modular nature and their amenability to rapid structure variation enabled the efficient discovery of ligands for three enantioselective RhIII-catalyzed C-H activation reactions, including one unprecedented transformation. This novel approach should enable the discovery of efficient chiral Cp ligands for various further enantioselective transformations.
authors.affiliation: Max-Planck-Institut für Molekulare Physiologie, Abteilung Chemische Biologie, Otto-Hahn-Strasse 11, 44227, Dortmund, Germany.|Technische Universität Dortmund, Fakultät Chemie und Chemische Biologie, Chemische Biologie, Otto-Hahn-Strasse 4a, 44227, Dortmund, Germany.
authors.forename: Zhi-Jun
authors.identifier: 0000-0002-5143-4875
authors.initials: ZJ
authors.lastname: Jia
authors.affiliation: Ruhr-Universität Bochum, Lehrstuhl für Organische Chemie II, Universitätsstrasse 150, 44801, Bochum, Germany.
authors.forename: Christian
authors.identifier: 0000-0002-4106-1905
authors.initials: C
authors.lastname: Merten
authors.affiliation: Max-Planck-Institut für Molekulare Physiologie, Abteilung Chemische Biologie, Otto-Hahn-Strasse 11, 44227, Dortmund, Germany.
authors.forename: Rajesh
authors.identifier: 0000-0001-5918-7568
authors.initials: R
authors.lastname: Gontla
authors.affiliation: Westfälische Wilhelms-Universität Münster, Organisch-Chemisches Institut, Corrensstrasse 40, 48149, Münster, Germany.
authors.forename: Constantin G
authors.identifier: 0000-0002-6709-3673
authors.initials: CG
authors.lastname: Daniliuc
authors.affiliation: Max-Planck-Institut für Molekulare Physiologie, Abteilung Chemische Biologie, Otto-Hahn-Strasse 11, 44227, Dortmund, Germany.|Technische Universität Dortmund, Fakultät Chemie und Chemische Biologie, Chemische Biologie, Otto-Hahn-Strasse 4a, 44227, Dortmund, Germany.
authors.forename: Andrey P
authors.identifier: 0000-0003-0435-9443
authors.initials: AP
authors.lastname: Antonchick
authors.affiliation: Max-Planck-Institut für Molekulare Physiologie, Abteilung Chemische Biologie, Otto-Hahn-Strasse 11, 44227, Dortmund, Germany.|Technische Universität Dortmund, Fakultät Chemie und Chemische Biologie, Chemische Biologie, Otto-Hahn-Strasse 4a, 44227, Dortmund, Germany.
authors.forename: Herbert
authors.initials: H
authors.lastname: Waldmann
keywords: C−H activation; asymmetric synthesis; cycloadditions; cyclopentadienyl ligands; rhodium