Design of catalytic metal-organic assemblies via shape complementarity and conformational constraints in dual curvature ligands

Autor: Michael L. Singleton, Cuilian Liu, Koen Robeyns, Yann Garcia, Eduard O. Bobylev, Brice Kauffmann, Joost N. H. Reek
Rok vydání: 2021
Předmět:
Popis: Non-covalent interactions play an essential role in the folding and self-assembly of large biological assemblies. These interactions are not only a driving force for the formation of large structures but also control conformation and com-plementary shapes of subcomponents that promote the diversity of structures and functions of the resulting assemblies. Understanding how non-covalent interactions direct self-assembly and the effect of conformation and complementary shapes on self-assembled structures will help design artificial supramolecular systems with extended components and functions. Herein, we develop a strategy for controlling more complex self-assembly with lower symmetry and flexible building blocks that combine endohedral non-covalent interactions with a dual curvature in the ligand backbone to give additional shape complementarity. A Diels-Alder reaction was used to break the symmetry of the diazaanthracene units of the ligands to give dual curvature ligands with different shapes and endohedral groups (L1-L3). The self-assembly studies of these ligands demonstrated that non-covalent interactions and shape complementary effectively control the self-assembly and enable the design of cages for supramolecular catalysis.
Databáze: OpenAIRE