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Synthesis of Information-bearing Peptoids and their Sequence-directed Dynamic Covalent Self-assembly
Published on: February 6, 2020
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Dynamic self-assembly of supramolecular catalysts from precision macromolecules
Qian Qin1, Jie Li1, David Dellemme2
1Institute of Condensed Matter and Nanosciences, Université catholique de Louvain Croix du Sud 1 L7.04.02, Louvain-la-Neuve Belgium alain.jonas@uclouvain.be.
Chemical Science
|September 15, 2023
Summary
Dynamic libraries of sequence-defined oligomers show strong catalytic activity. Self-assembled macrocycles exhibit significantly higher catalytic turnover than linear chains, offering design guidelines for functional supramolecular systems.
Area of Science:
- Supramolecular Chemistry
- Catalysis
- Polymer Science
Background:
- Dynamic combinatorial libraries offer a versatile platform for discovering novel molecular functions.
- Sequence-defined oligomers with functional groups can self-assemble into complex architectures.
- Catalytic activity in supramolecular systems is often dependent on specific structural arrangements.
Purpose of the Study:
- To investigate the catalytic activity of dynamic libraries composed of sequence-defined oligomeric chains.
- To compare the catalytic efficiency of self-assembled supramolecular macrocycles versus linear oligomers.
- To develop a mathematical model for predicting catalytic properties in these dynamic systems.
Main Methods:
- Synthesis of sequence-defined oligomeric chains with pendant catalytic groups and terminal recognition units.
- Formation of dynamic constitutional libraries in solution, including free oligomers, macrocycles, and linear polymers.
- Experimental evaluation of catalytic turnover frequency for different supramolecular assemblies.
- Molecular dynamics simulations and network analysis to understand self-assembly stabilization.
- Mathematical modeling of catalytic properties based on physical parameters.
Main Results:
- Emergence of strong catalytic activity at low concentrations within dynamic oligomer libraries.
- Supramolecular di(oligomeric) macrocycles demonstrated a catalytic turnover frequency approximately 20 times greater than linear poly(oligomers) and free chains.
- Identification of stabilizing interactions, including chain end pairing, within the self-assembled macrocycles.
- Development of a mathematical model correlating library composition and catalytic performance.
Conclusions:
- Self-assembled supramolecular macrocycles derived from dynamic libraries exhibit significantly enhanced catalytic activity.
- The study provides a framework for designing sequence-defined oligomers for targeted supramolecular catalysis.
- Mathematical modeling offers predictive power for optimizing the synthesis of functional macrocyclic systems.
