期刊
ACS NANO
卷 14, 期 5, 页码 5491-5505出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b09610
关键词
supramolecular chemistry; bioinspired materials; hydrogels; nonequilibrium self-assembly; hierarchical materials; gelation kinetics
类别
资金
- 3MNon-Tenured Faculty Award (3M Company)
- University of Notre Dame Advancing our Vision initiative
- Berry Family Foundation Graduate Fellowship through Notre Dame Advanced Diagnostics Therapeutics
Natural proteins traverse complex free energy landscapes to assemble into hierarchically organized structures, often through stimuli-directed kinetic pathways in response to relevant biological cues. Bioinspired strategies have sought to emulate the complexity, dynamicity, and modularity exhibited in these natural processes with synthetic analogues. However, these efforts are limited by many factors that complicate the rational design and predictable assembly of synthetic constructs, especially in aqueous environments. Herein, a model discotic amphiphile gelator is described that undergoes pathway-dependent structural maturation when exposed to varying application rates of a pH stimulus, investigated by electron microscopy, spectroscopy, and X-ray scattering techniques. Under the direction of a slowly changing pH stimulus, complex hierarchical assemblies result, characterized by mesoscale elongated superstructure bundles embedded in a percolated mesh of narrow nanofibers. In contrast, the assembly under a rapidly applied pH stimulus is characterized by homogeneous structures that are reminiscent of the superstructures arising from the more deliberate path, except with significantly reduced scale and concomitantly large increases in bulk rheological properties. This synthetic system bears resemblance to the pathway complexity and hierarchical ordering observed for native structures, such as collagen, and points to fundamental design principles that might be applied toward enhanced control of the properties of supramolecular self-assembly across length scales.
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