Cascade synthesis of a gold nanoparticle-network polymer composite

Grubjesic, Simonida; Ringstrand, Bryan Scott; Jungjohann, Katherine L.; Brombosz, Scott M.; Seifert, Sonke; Firestone, Millicent Anne

doi:10.1039/c5nr06594a

Cascade synthesis of a gold nanoparticle-network polymer composite

Journal Article · Sun Nov 01 23:00:00 EST 2015 · Nanoscale

DOI:https://doi.org/10.1039/c5nr06594a· OSTI ID:1335623

Grubjesic, Simonida ^[1]; Ringstrand, Bryan Scott ^[2]; Jungjohann, Katherine L. ^[3]; Brombosz, Scott M. ^[1]; Seifert, Sonke ^[1]; Firestone, Millicent Anne ^[2]

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396; AC04-94AL85000

OSTI ID:: 1335623

Alternate ID(s):: OSTI ID: 1347351
OSTI ID: 1352655

Report Number(s):: LA-UR--15-28768

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 5 Vol. 8; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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