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Title: Self-assembling hydrogel scaffolds for photocatalytic hydrogen production

Journal Article · · Nature Chemistry
DOI:https://doi.org/10.1038/nchem.2075· OSTI ID:1162321
 [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

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.

Research Organization:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Health (NIH); National Science Foundation (NSF)
Grant/Contract Number:
SC0001059; AC02-06CH11357; 5P41RR007707; 8P41GM103543; CHE-9871268
OSTI ID:
1162321
Alternate ID(s):
OSTI ID: 1820340
Journal Information:
Nature Chemistry, Vol. 6, Issue 11; ISSN 1755-4330
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
ENGLISH
Citation Metrics:
Cited by: 338 works
Citation information provided by
Web of Science

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  • Boettcher, Shannon W.; Warren, Emily L.; Putnam, Morgan C.
  • Journal of the American Chemical Society, Vol. 133, Issue 5, p. 1216-1219 https://doi.org/10.1021/ja108801m
journal January 2011
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Challenges and opportunities for hydrogen production from microalgae journal January 2016
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Development of a framework catalyst for photocatalytic hydrogen evolution journal January 2018
Beyond Covalent Crosslinks: Applications of Supramolecular Gels journal May 2018
Multi-component supramolecular gels induce protonation of a porphyrin exciplex to achieve improved collective optical properties for effective photocatalytic hydrogen generation journal January 2020
Covalent Attachment of the Water-insoluble Ni(P Cy 2 N Phe 2 ) 2 Electrocatalyst to Electrodes Showing Reversible Catalysis in Aqueous Solution journal October 2016
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Supramolecular fluorescent hydrogelators as bio-imaging probes journal January 2019
Tuning the polarity and surface activity of hydroxythiazoles – extending the applicability of highly fluorescent self-assembling chromophores to supra-molecular photonic structures journal January 2016
Photoswitchable phthalocyanine-assembled nanoparticles for controlled “double-lock” photodynamic therapy journal January 2019
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A squaraine-linked metalloporphyrin two-dimensional polymer photocatalyst for hydrogen and oxygen evolution reactions journal January 2019
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