Wu Kai, Tessarolo Jacopo, Baksi Ananya, Clever Guido H
Department of Chemistry and Chemical Biology, TU Dortmund University, Otto Hahn Str. 6, 44227, Dortmund, Germany.
Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK.
Angew Chem Int Ed Engl. 2022 Aug 26;61(35):e202205725. doi: 10.1002/anie.202205725. Epub 2022 Jul 4.
Multicomponent metallo-supramolecular assembly allows the rational combination of different building blocks. Discrete multifunctional hosts with an accessible cavity can be prepared in a non-statistical fashion. We employ our shape-complementary assembly (SCA) method to achieve for the first time integrative self-sorting of heteroleptic Pd cages showing guest-tunable circularly polarized luminescence (CPL). An enantiopure helicene-based ligand (M or P configuration) is coupled with a non-chiral emissive fluorenone-based ligand (A or B) to form a series of Pd L L' assemblies. The modular strategy allows to impart the chiral information of the helicenes to the overall supramolecular system, resulting in CPL from the non-chiral component. Guest binding results in a 4-fold increase of CPL intensity. The principle offers potential to generate libraries of multifunctional materials with applications in molecular recognition, enantioselective photo-redox catalysis and information processing.
多组分金属超分子组装能够实现不同结构单元的合理组合。可以以非统计方式制备具有可及空腔的离散多功能主体。我们采用形状互补组装（SCA）方法，首次实现了具有客体可调圆偏振发光（CPL）的杂配体钯笼的整合自分类。一种对映体纯的基于螺旋烯的配体（M或P构型）与一种非手性发光芴酮基配体（A或B）偶联，形成一系列钯L L'组装体。这种模块化策略能够将螺旋烯的手性信息赋予整个超分子体系，从而使非手性组分产生CPL。客体结合导致CPL强度增加4倍。该原理为生成多功能材料库提供了潜力，这些材料可应用于分子识别、对映选择性光氧化还原催化和信息处理。
