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Title: Effect of molecular properties of block copolymers and nanoparticles on the morphology of self-assembled bulk nanocomposites.

Abstract

Self-assembly of thiol-terminated polystyrene-tethered Au nanoparticles in microphase-separated diblock copolymers composed of poly(styrene-b-2vinylpyridine) (PS-PVP) as a function of particle concentration and composition of block copolymers was investigated using anomalous small-angle X-ray scattering (ASAXS) and transmission electron microscopy (TEM). Results reveal that the self-assembly of nanoparticles in the PS domain causes swelling and increases the interfacial curvature that, in turn, induces order-order transitions. At intermediate loading, the presence of nanoparticles amplifies the local compositional fluctuations, hence the roughness at the PS and PVP interface, which creates conditions to induce disorder in the polymer morphology. The system thus undergoes an order-disorder transition. At high particle loading, packing constraints prevent all particles from assembling in the PS domain, and the excess nanoparticles undergo macrophase separation. The present systematic study augments experimental data to the scarce literature on the phase behavior of bulk nanocomposites. We present a generalized phase map for the bulk composites as a function of effective volume fraction of PS (F{sub PS}) for a given nanoparticle size. We believe that the results from this study will enable comparison of the phase maps from various studies and will serve to validate the simulation studies of inorganic particle/block copolymer composites.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
939325
Report Number(s):
ANL/IPNS/JA-59980
TRN: US200823%%12
DOE Contract Number:  
DE-AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 40; Journal Issue: 23 ; Nov. 13, 2007
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; COPOLYMERS; COMPOSITE MATERIALS; NANOSTRUCTURES; THIOLS; POLYSTYRENE; GOLD; PYRIDINES; MORPHOLOGY; SWELLING; INTERFACES; ORDER-DISORDER TRANSFORMATIONS; PHASE STUDIES

Citation Formats

Lo, C -T, Lee, B, Dietz Rago, N L, Seifert, S, Winans, R E, and Thiyagarajan, P. Effect of molecular properties of block copolymers and nanoparticles on the morphology of self-assembled bulk nanocomposites.. United States: N. p., 2007. Web. doi:10.1021/ma070835v.
Lo, C -T, Lee, B, Dietz Rago, N L, Seifert, S, Winans, R E, & Thiyagarajan, P. Effect of molecular properties of block copolymers and nanoparticles on the morphology of self-assembled bulk nanocomposites.. United States. doi:10.1021/ma070835v.
Lo, C -T, Lee, B, Dietz Rago, N L, Seifert, S, Winans, R E, and Thiyagarajan, P. Tue . "Effect of molecular properties of block copolymers and nanoparticles on the morphology of self-assembled bulk nanocomposites.". United States. doi:10.1021/ma070835v.
@article{osti_939325,
title = {Effect of molecular properties of block copolymers and nanoparticles on the morphology of self-assembled bulk nanocomposites.},
author = {Lo, C -T and Lee, B and Dietz Rago, N L and Seifert, S and Winans, R E and Thiyagarajan, P},
abstractNote = {Self-assembly of thiol-terminated polystyrene-tethered Au nanoparticles in microphase-separated diblock copolymers composed of poly(styrene-b-2vinylpyridine) (PS-PVP) as a function of particle concentration and composition of block copolymers was investigated using anomalous small-angle X-ray scattering (ASAXS) and transmission electron microscopy (TEM). Results reveal that the self-assembly of nanoparticles in the PS domain causes swelling and increases the interfacial curvature that, in turn, induces order-order transitions. At intermediate loading, the presence of nanoparticles amplifies the local compositional fluctuations, hence the roughness at the PS and PVP interface, which creates conditions to induce disorder in the polymer morphology. The system thus undergoes an order-disorder transition. At high particle loading, packing constraints prevent all particles from assembling in the PS domain, and the excess nanoparticles undergo macrophase separation. The present systematic study augments experimental data to the scarce literature on the phase behavior of bulk nanocomposites. We present a generalized phase map for the bulk composites as a function of effective volume fraction of PS (F{sub PS}) for a given nanoparticle size. We believe that the results from this study will enable comparison of the phase maps from various studies and will serve to validate the simulation studies of inorganic particle/block copolymer composites.},
doi = {10.1021/ma070835v},
journal = {Macromolecules},
number = 23 ; Nov. 13, 2007,
volume = 40,
place = {United States},
year = {2007},
month = {11}
}