Computational Tools to Rationalize and Predict the Self-Assembly Behavior of Supramolecular Gels

Abstract

Supramolecular gels form a class of soft materials that has been heavily explored by the chemical community in the past 20 years. While a multitude of experimental techniques has demonstrated its usefulness when characterizing these materials, the potential value of computational techniques has received much less attention. This review aims to provide a complete overview of studies that employ computational tools to obtain a better fundamental understanding of the self-assembly behavior of supramolecular gels or to accelerate their development by means of prediction. As such, we hope to stimulate researchers to consider using computational tools when investigating these intriguing materials. In the concluding remarks, we address future challenges faced by the field and formulate our vision on how computational methods could help overcoming them.

Dynamic protein and polypeptide hydrogels based on Schiff base co-assembly for biomedicine

“…235 For example, the chemical space available for hydrogel design using peptides is practically infinite, and structurally similar molecules within this space often do not gelate. 236 Several approaches to illuminate principles for hydrogel design have been explored, such as structure-based design, enumeration of chemical libraries, and quantitative structure-property relationships (QSPR). However, structurebased design and chemical libraries heavily depend on experimental methods and may require synthesising hundreds or This journal is © The Royal Society of Chemistry 2022 thousands of compounds.…”

Advanced Methods for the Characterization of Supramolecular Hydrogels

“…A promising approach to complement the experimental rheological characterization of hydrogels is the use of modeling simulations, which can help to reduce the time and costs associated with the experiments. This approach is feasible because the molecular structure of the hydrogel network influences its rheological properties, and increasingly sophisticated computational models of supramolecular materials are being developed, as reviewed by Van Lommel et al [118]. That review provides further detail regarding computational modeling techniques, including DFT, molecular dynamics calculations, and crystal structure prediction, which have been applied to understand many aspects of supramolecular gels [118].…”

“…This approach is feasible because the molecular structure of the hydrogel network influences its rheological properties, and increasingly sophisticated computational models of supramolecular materials are being developed, as reviewed by Van Lommel et al [118]. That review provides further detail regarding computational modeling techniques, including DFT, molecular dynamics calculations, and crystal structure prediction, which have been applied to understand many aspects of supramolecular gels [118]. These computational methods can assist in determining rheological properties of supramolecular hydrogels.…”

Donor–acceptor organogels and xerogels fromC3-symmetric pyrene and naphthalene-diimide components

“…Over the last few decades, much effort has been dedicated to the rationalisation of gelling properties. 5,[14][15][16] Though scientists can still discover exotic supramolecular behaviours, noncovalent design principles have been proposed and accepted to build supramolecular polymers 17,18 eventually behaving as gelators. 19,20 The role of the solvent also has to be emphasized, since this component appears critical with regard to the gelling ability, the structure of the corresponding xerogel materials and their physicochemical properties.…”