![]() Coarse-grained molecular dynamics simulations revealed that the chromophore amphiphile assembly is guided by the polyelectrolyte network via ionic interactions. ![]() Furthermore, this allows optimization of the hydrogel mechanical properties, retention of the chromophore amphiphile assemblies, and the photocatalytic reaction efficiency. By varying the monomer and crosslinker composition in the feed, we can tune the porosity of the network as well as the chemical environment in which supramolecular crystallization of the chromophore amphiphiles takes place. However, molecular components necessary for catalysis, byproducts from photocatalysis, and the hydrogen produced are able to diffuse in or out of the covalent network to create a reusable robust host for photocatalysis. Opposite charges in the covalent polyelectrolyte and the chromophore amphiphiles and sterics entrap the supramolecular assemblies within the mechanically more » stable network. ![]() Chromophore amphiphiles were introduced into non-aqueous solvent swollen polymer matrices and self-assembly of the chromophore amphiphiles into crystalline nanostructures was triggered in the confined environment of the covalent network upon solvent exchange for water. We report here on the synthesis of functional hybrid hydrogels containing self-assembling chromophore amphiphiles and polyelectrolytes. Hybrid systems based on covalent polymers and supramolecular assemblies offer unique opportunities for functional materials based on the pathway-dependent dynamic structures of supramolecular assemblies and the mechanical stability of covalent polymers. Center for Bio-Inspired Energy Science (CBES) Sponsoring Org.: USDOE Office of Science (SC), Basic Energy Sciences (BES) OSTI Identifier: 1798323 Alternate Identifier(s): OSTI ID: 1822878 OSTI ID: 1846639 Grant/Contract Number: SC0000989 Resource Type: Journal Article: Accepted Manuscript Journal Name: Journal of the American Chemical Society Additional Journal Information: Journal Volume: 142 Journal Issue: 18 Journal ID: ISSN 0002-7863 Publisher: American Chemical Society (ACS) Country of Publication: United States Language: English Subject: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Molecules Light Hydrogels Polymers Irradiation 99 GENERAL AND MISCELLANEOUS Molecules, Light, Hydrogels, Polymers, = , Publication Date: Fri Apr 24 00:00: Research Org.: Northwestern Univ., Evanston, IL (United States) Energy Frontier Research Centers (EFRC) (United States).
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