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Title: Self-assembling hydrogel scaffolds for photocatalytic hydrogen production

Integration into a soft material of all the molecular components necessary to generate storable fuels is an interesting target in supramolecular chemistry. The concept is inspired by the internal structure of photosynthetic organelles, such as plant chloroplasts, which colocalize molecules involved in light absorption, charge transport and catalysis to create chemical bonds using light energy. We report in this paper on the light-driven production of hydrogen inside a hydrogel scaffold built by the supramolecular self-assembly of a perylene monoimide amphiphile. The charged ribbons formed can electrostatically attract a nickel-based catalyst, and electrolyte screening promotes gelation. We found the emergent phenomenon that screening by the catalyst or the electrolytes led to two-dimensional crystallization of the chromophore assemblies and enhanced the electronic coupling among the molecules. Finally, photocatalytic production of hydrogen is observed in the three-dimensional environment of the hydrogel scaffold and the material is easily placed on surfaces or in the pores of solid supports.
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [5] ;  [1] ;  [6]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. Argonne-Northwestern Solar Energy Research (ANSER) Center
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. Argonne-Northwestern Solar Energy Research (ANSER) Center; Northwestern Univ., Chicago, IL (United States). Simpson Querrey Inst. for BioNanotechnology
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  6. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. Argonne-Northwestern Solar Energy Research (ANSER) Center; Northwestern Univ., Chicago, IL (United States). Simpson Querrey Inst. for BioNanotechnology. Dept. of Materials Science and Engineering. Dept. of Medicine
Publication Date:
OSTI Identifier:
1162321
Grant/Contract Number:
SC0001059; AC02-06CH11357; 5P41RR007707; 8P41GM103543; CHE-9871268
Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 6; Journal Issue: 11; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Research Org:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Inst. of Health (NIH) (United States); National Science Foundation (NSF)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Self-assembly