Solubility-Driven Design of Multicomponent Self-Assembled Hydrogels.
- 1Institute of Advanced Materials (INAM), Universitat Jaume I, 12071, Castelló, Spain.
- 2Institute of Physical Chemistry, University of Stuttgart, Pfaffenwaldring 55, 70569, Stuttgart, Germany.
- 3Research & Open Innovation-Material Science, Henkel AG & Co. KGaA, 40589, Dusseldorf, Germany.
Abstract
Nature has skillfully harnessed molecular social behavior, such as "co-assembly" and "self-sorting", to achieve functional intricacy from simple building blocks. However, the rational control of such "social diversity" in synthetic supramolecular systems remains an unresolved problem. The entropy-enthalpy balance in hydrogelator self-assembly is a crucial thermodynamic parameter to control whether low molecular weight gelators (LMWGs) interact or act autonomously in multicomponent hydrogels. Here we propose that a simple inspection of the hydrogelator solubility vs temperature profile, as measured by 1H NMR, allows us to classify and select single-component hydrogelators in order to combine them at will. Thus, we demonstrate our hypothesis through an investigation of three individual LMWGs, with different solubility profiles, and their pairwise combinations to assess their assembly behavior over molecular, mesoscopic, and macroscopic length scales using a range of techniques. Our data show that one binary mixture exhibits co-assembly to form a unified network hydrogel material, whereas the other combinations display self-sorting, whereby each hydrogelator maintains its own structural integrity and intrinsic material properties. Crucially, temperature is used as an external stimulus to control these systems, providing direct and predictable control over material architecture. Our work highlights how simple NMR solubility measurements manifest the entropy-enthalpy balance as a rational approach to design multicomponent supramolecular materials with multifunctionality from simple and accessible molecular building blocks.
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BibTeX
@article{singh2026solubilitydriven,
title = {{Solubility-Driven Design of Multicomponent Self-Assembled Hydrogels.}},
author = {Misthi Singh and Florian Trummer and Peter Schmiedel and Thomas Sottmann and Beatriu Escuder},
journal = {Langmuir : the ACS journal of surfaces and colloids},
year = {2026},
month = sep,
doi = {10.1021/acs.langmuir.6c03536},
url = {https://europepmc.org/article/MED/42916831},
note = {CC BY},
}
RIS
TY - JOUR
TI - Solubility-Driven Design of Multicomponent Self-Assembled Hydrogels.
AU - Misthi Singh
AU - Florian Trummer
AU - Peter Schmiedel
AU - Thomas Sottmann
AU - Beatriu Escuder
PY - 2026
DA - 2026/09/01
JO - Langmuir : the ACS journal of surfaces and colloids
DO - 10.1021/acs.langmuir.6c03536
UR - https://europepmc.org/article/MED/42916831
AB - Nature has skillfully harnessed molecular social behavior, such as "co-assembly" and "self-sorting", to achieve functional intricacy from simple building blocks. However, the rational control of such "social diversity" in synthetic supramolecular systems remains an unresolved problem. The entropy-enthalpy balance in hydrogelator self-assembly is a crucial thermodynamic parameter to control whether low molecular weight gelators (LMWGs) interact or act autonomously in multicomponent hydrogels. Here we propose that a simple inspection of the hydrogelator solubility vs temperature profile, as measured by 1H NMR, allows us to classify and select single-component hydrogelators in order to combine them at will. Thus, we demonstrate our hypothesis through an investigation of three individual LMWGs, with different solubility profiles, and their pairwise combinations to assess their assembly behavior over molecular, mesoscopic, and macroscopic length scales using a range of techniques. Our data show that one binary mixture exhibits co-assembly to form a unified network hydrogel material, whereas the other combinations display self-sorting, whereby each hydrogelator maintains its own structural integrity and intrinsic material properties. Crucially, temperature is used as an external stimulus to control these systems, providing direct and predictable control over material architecture. Our work highlights how simple NMR solubility measurements manifest the entropy-enthalpy balance as a rational approach to design multicomponent supramolecular materials with multifunctionality from simple and accessible molecular building blocks.
SN - 0743-7463
SN - 1520-5827
ER -