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Access to Metastable Gel States Using Seeded Self‐Assembly of Low‐Molecular‐Weight Gelators
Author(s) -
Wang Yiming,
de Kruijff Robin M.,
Lovrak Matija,
Guo Xuhong,
Eelkema Rienk,
van Esch Jan H.
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201812412
Subject(s) - supramolecular chemistry , metastability , self assembly , homogeneous , ionic bonding , chemical engineering , chemistry , materials science , chemical physics , nanotechnology , organic chemistry , molecule , ion , thermodynamics , physics , engineering
Here we report on how metastable supramolecular gels can be formed through seeded self‐assembly of multicomponent gelators. Hydrazone‐based gelators decorated with non‐ionic and anionic groups are formed in situ from hydrazide and aldehyde building blocks, and lead through multiple self‐sorting processes to the formation of heterogeneous gels approaching thermodynamic equilibrium. Interestingly, the addition of seeds composing of oligomers of gelators bypasses the self‐sorting processes and accelerates the self‐assembly along a kinetically favored pathway, resulting in homogeneous gels of which the network morphologies and gel stiffness are markedly different from the thermodynamically more stable gel products. Importantly, over time, these metastable homogeneous gel networks are capable of converting into the thermodynamically more stable state. This seeding‐driven formation of out‐of‐equilibrium supramolecular structures is expected to serve as a simple approach towards functional materials with pathway‐dependent properties.