Self-assembling hydrogel scaffolds for photocatalytic hydrogen production
Abstract
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:
-
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. Argonne-Northwestern Solar Energy Research (ANSER) Center
- 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
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering
- Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- 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:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Health (NIH); National Science Foundation (NSF)
- OSTI Identifier:
- 1162321
- Alternate Identifier(s):
- OSTI ID: 1820340
- Grant/Contract Number:
- SC0001059; AC02-06CH11357; 5P41RR007707; 8P41GM103543; CHE-9871268
- Resource 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
- Country of Publication:
- United States
- Language:
- ENGLISH
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Self-assembly
Citation Formats
Weingarten, Adam S., Kazantsev, Roman V., Palmer, Liam C., McClendon, Mark, Koltonow, Andrew R., Samuel, Amanda P. S., Kiebala, Derek J., Wasielewski, Michael R., and Stupp, Samuel I. Self-assembling hydrogel scaffolds for photocatalytic hydrogen production. United States: N. p., 2014.
Web. doi:10.1038/nchem.2075.
Weingarten, Adam S., Kazantsev, Roman V., Palmer, Liam C., McClendon, Mark, Koltonow, Andrew R., Samuel, Amanda P. S., Kiebala, Derek J., Wasielewski, Michael R., & Stupp, Samuel I. Self-assembling hydrogel scaffolds for photocatalytic hydrogen production. United States. https://doi.org/10.1038/nchem.2075
Weingarten, Adam S., Kazantsev, Roman V., Palmer, Liam C., McClendon, Mark, Koltonow, Andrew R., Samuel, Amanda P. S., Kiebala, Derek J., Wasielewski, Michael R., and Stupp, Samuel I. Sun .
"Self-assembling hydrogel scaffolds for photocatalytic hydrogen production". United States. https://doi.org/10.1038/nchem.2075. https://www.osti.gov/servlets/purl/1162321.
@article{osti_1162321,
title = {Self-assembling hydrogel scaffolds for photocatalytic hydrogen production},
author = {Weingarten, Adam S. and Kazantsev, Roman V. and Palmer, Liam C. and McClendon, Mark and Koltonow, Andrew R. and Samuel, Amanda P. S. and Kiebala, Derek J. and Wasielewski, Michael R. and Stupp, Samuel I.},
abstractNote = {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.},
doi = {10.1038/nchem.2075},
journal = {Nature Chemistry},
number = 11,
volume = 6,
place = {United States},
year = {Sun Oct 05 00:00:00 EDT 2014},
month = {Sun Oct 05 00:00:00 EDT 2014}
}
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- Nandi, Sujay Kumar; Maji, Krishnendu; Haldar, Debasish
- ACS Omega, Vol. 3, Issue 4
Supramolecular Packing Controls H 2 Photocatalysis in Chromophore Amphiphile Hydrogels
journal, November 2015
- Weingarten, Adam S.; Kazantsev, Roman V.; Palmer, Liam C.
- Journal of the American Chemical Society, Vol. 137, Issue 48
Crystal-Phase Transitions and Photocatalysis in Supramolecular Scaffolds
journal, April 2017
- Kazantsev, Roman V.; Dannenhoffer, Adam J.; Weingarten, Adam S.
- Journal of the American Chemical Society, Vol. 139, Issue 17
Supramolecular Packing and Macroscopic Alignment Controls Actuation Speed in Macroscopic Strings of Molecular Motor Amphiphiles
journal, November 2018
- Leung, Franco King-Chi; van den Enk, Tobias; Kajitani, Takashi
- Journal of the American Chemical Society, Vol. 140, Issue 50
Energy landscapes and functions of supramolecular systems
journal, January 2016
- Tantakitti, Faifan; Boekhoven, Job; Wang, Xin
- Nature Materials, Vol. 15, Issue 4
A broadband and strong visible-light-absorbing photosensitizer boosts hydrogen evolution
journal, July 2019
- Wang, Ping; Guo, Song; Wang, Hong-Juan
- Nature Communications, Vol. 10, Issue 1
Biocompatible fluorescent supramolecular nanofibrous hydrogel for long-term cell tracking and tumor imaging applications
journal, November 2015
- Wang, Huaimin; Mao, Duo; Wang, Youzhi
- Scientific Reports, Vol. 5, Issue 1
Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy
journal, January 2018
- Hayes, Dugan; Kohler, Lars; Hadt, Ryan G.
- Chemical Science, Vol. 9, Issue 4
Challenges and opportunities for hydrogen production from microalgae
journal, January 2016
- Oey, Melanie; Sawyer, Anne Linda; Ross, Ian Lawrence
- Plant Biotechnology Journal, Vol. 14, Issue 7