Cascade synthesis of a gold nanoparticle–network polymer composite
Abstract
In this paper, the multi-step, cascade synthesis of a self-supporting, hierarchically-structured gold nanoparticle hydrogel composite is described. The composite is spontaneously prepared from a non-covalent, lamellar lyotropic mesophase composed of amphiphiles that support the reactive constituents, a mixture of hydroxyl- and acrylate-end-derivatized PEO117-PPO47-PEO117 and [AuCl4]-. The reaction sequence begins with the auto-reduction of aqueous [AuCl4]- by PEO117-PPO47-PEO117 which leads to both the production of Au NPs and the free radical initiated polymerization and crosslinking of the acrylate endderivatized PEO117-PPO47-PEO117 to yield a network polymer. Optical spectroscopy and TEM monitored the reduction of [AuCl4]-, formation of large aggregated Au NPs and oxidative etching into a final state of dispersed, spherical Au NPs. ATR/FT-IR spectroscopy and thermal analysis confirms acrylate crosslinking to yield the polymer network. X-ray scattering (SAXS and WAXS) monitored the evolution of the multilamellar structured mesophase and revealed the presence of semi-crystalline PEO confined within the water layers. The hydrogel could be reversibly swollen without loss of the well-entrained Au NPs with full recovery of composite structure. Finally, optical spectroscopy shows a notable red shift (Δλ~ 45 nm) in the surface plasmon resonance between swollen and contracted states, demonstrating solvent-mediated modulation of the internal NP packing arrangement.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1347351
- Alternate Identifier(s):
- OSTI ID: 1335623; OSTI ID: 1352655
- Report Number(s):
- SAND2015-2522J; LA-UR-15-28768
Journal ID: ISSN 2040-3364; 579846
- Grant/Contract Number:
- AC04-94AL85000; AC52-06NA25396; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 5; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Material Science
Citation Formats
Grubjesic, Simonida, Ringstrand, Bryan Scott, Jungjohann, Katherine L., Brombosz, Scott M., Seifert, Sönke, and Firestone, Millicent Anne. Cascade synthesis of a gold nanoparticle–network polymer composite. United States: N. p., 2015.
Web. doi:10.1039/c5nr06594a.
Grubjesic, Simonida, Ringstrand, Bryan Scott, Jungjohann, Katherine L., Brombosz, Scott M., Seifert, Sönke, & Firestone, Millicent Anne. Cascade synthesis of a gold nanoparticle–network polymer composite. United States. https://doi.org/10.1039/c5nr06594a
Grubjesic, Simonida, Ringstrand, Bryan Scott, Jungjohann, Katherine L., Brombosz, Scott M., Seifert, Sönke, and Firestone, Millicent Anne. Mon .
"Cascade synthesis of a gold nanoparticle–network polymer composite". United States. https://doi.org/10.1039/c5nr06594a. https://www.osti.gov/servlets/purl/1347351.
@article{osti_1347351,
title = {Cascade synthesis of a gold nanoparticle–network polymer composite},
author = {Grubjesic, Simonida and Ringstrand, Bryan Scott and Jungjohann, Katherine L. and Brombosz, Scott M. and Seifert, Sönke and Firestone, Millicent Anne},
abstractNote = {In this paper, the multi-step, cascade synthesis of a self-supporting, hierarchically-structured gold nanoparticle hydrogel composite is described. The composite is spontaneously prepared from a non-covalent, lamellar lyotropic mesophase composed of amphiphiles that support the reactive constituents, a mixture of hydroxyl- and acrylate-end-derivatized PEO117-PPO47-PEO117 and [AuCl4]-. The reaction sequence begins with the auto-reduction of aqueous [AuCl4]- by PEO117-PPO47-PEO117 which leads to both the production of Au NPs and the free radical initiated polymerization and crosslinking of the acrylate endderivatized PEO117-PPO47-PEO117 to yield a network polymer. Optical spectroscopy and TEM monitored the reduction of [AuCl4]-, formation of large aggregated Au NPs and oxidative etching into a final state of dispersed, spherical Au NPs. ATR/FT-IR spectroscopy and thermal analysis confirms acrylate crosslinking to yield the polymer network. X-ray scattering (SAXS and WAXS) monitored the evolution of the multilamellar structured mesophase and revealed the presence of semi-crystalline PEO confined within the water layers. The hydrogel could be reversibly swollen without loss of the well-entrained Au NPs with full recovery of composite structure. Finally, optical spectroscopy shows a notable red shift (Δλ~ 45 nm) in the surface plasmon resonance between swollen and contracted states, demonstrating solvent-mediated modulation of the internal NP packing arrangement.},
doi = {10.1039/c5nr06594a},
journal = {Nanoscale},
number = 5,
volume = 8,
place = {United States},
year = {Mon Nov 02 00:00:00 EST 2015},
month = {Mon Nov 02 00:00:00 EST 2015}
}
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