In situ Synthesis of Supramolecular Polymers:Finding the Right Conditions when Combining Covalent and Non-Covalent Synthesis

摘要

The combination of covalent and non-covalent synthesis is omnipresent in nature and potentially enables access to new materials.Yet,the fundamental principles that govern such a synthesis are barely understood.Here,we demonstrate how even simple reaction mixtures behave surprisingly complex when covalent reactions are coupled to self-assembly processes.Specifically,we study the reaction behavior of a system in which the in situ formation of disco tic benzene-1,3,5-tricarboxamide(BTA)monomers is linked to an intertwined non-covalent reaction network including self-assembly into helical BTA polymers.This system shows an unexpected phase-separation behavior in which an interplay of reactant/product concentrations,side-products and solvent purity determines the system composition.We envision that these insights can bring us one step closer to how to design the synthesis of systems in a combined covalent/non-covalent fashion.