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Structural evolution of surfactant - Silica film-forming solutions, investigated using small-angle neutron scattering

Brennan, Tessa ; Roser, Stephen J. ; Mann, Stephen and Edler, Karen J. LU orcid (2002) In Chemistry of Materials 14(10). p.4292-4299
Abstract

Time-resolved small-angle neutron scattering has been used to investigate the evolution of micelles in the subphase of surfactant-templated silica film-forming solutions. Two samples have been prepared using cetyltrimethylammonium bromide (CTABr), as the structure-directing agent, and different amounts of tetramethoxysilane (TMOS) (CTABr/TMOS molar ratio 0.093, 0.139). The solutions have been reproduced at three different H2O/D2O contrasts and allowed to develop until a precipitate formed in the bulk. The surfactant initially forms micelles in solution while the hydrolyzed TMOS is dispersed uniformly through the aqueous phase. The micelles appear to have an ellipsoidal structure immediately after mixing, composed... (More)

Time-resolved small-angle neutron scattering has been used to investigate the evolution of micelles in the subphase of surfactant-templated silica film-forming solutions. Two samples have been prepared using cetyltrimethylammonium bromide (CTABr), as the structure-directing agent, and different amounts of tetramethoxysilane (TMOS) (CTABr/TMOS molar ratio 0.093, 0.139). The solutions have been reproduced at three different H2O/D2O contrasts and allowed to develop until a precipitate formed in the bulk. The surfactant initially forms micelles in solution while the hydrolyzed TMOS is dispersed uniformly through the aqueous phase. The micelles appear to have an ellipsoidal structure immediately after mixing, composed of a surfactant core surrounded by a thin, low-density silica film. The ellipsoidal micelles are typically 32 Å in length and with time elongate and become "rodlike" silica-coated cylinders with length in excess of 150 Å. This value is significantly larger in the composition containing more TMOS (≈1100 Å). In contrast, the radius of the core exhibits limited growth, swelling from 15.6 to ≈19 Å during the induction period. At long times the CTABr/TMOS = 0.139 sample exhibits a first-order diffraction peak at Q = 0.133 Å-1, corresponding to cooperative scattering from an ordered mesostructure. An analogous peak is not observed in the CTABr/TMOS = 0.093 solution. This is discussed in terms of different film formation mechanisms and compared with previous data measured by X-ray reflection techniques at the air/water interface.

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author
; ; and
publishing date
type
Contribution to journal
publication status
published
in
Chemistry of Materials
volume
14
issue
10
pages
8 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:0036797327
ISSN
0897-4756
DOI
10.1021/cm020399l
language
English
LU publication?
no
id
a4165877-20cc-4dd1-af6b-e4074999a53b
date added to LUP
2023-05-04 18:29:14
date last changed
2023-06-13 12:37:32
@article{a4165877-20cc-4dd1-af6b-e4074999a53b,
  abstract     = {{<p>Time-resolved small-angle neutron scattering has been used to investigate the evolution of micelles in the subphase of surfactant-templated silica film-forming solutions. Two samples have been prepared using cetyltrimethylammonium bromide (CTABr), as the structure-directing agent, and different amounts of tetramethoxysilane (TMOS) (CTABr/TMOS molar ratio 0.093, 0.139). The solutions have been reproduced at three different H<sub>2</sub>O/D<sub>2</sub>O contrasts and allowed to develop until a precipitate formed in the bulk. The surfactant initially forms micelles in solution while the hydrolyzed TMOS is dispersed uniformly through the aqueous phase. The micelles appear to have an ellipsoidal structure immediately after mixing, composed of a surfactant core surrounded by a thin, low-density silica film. The ellipsoidal micelles are typically 32 Å in length and with time elongate and become "rodlike" silica-coated cylinders with length in excess of 150 Å. This value is significantly larger in the composition containing more TMOS (≈1100 Å). In contrast, the radius of the core exhibits limited growth, swelling from 15.6 to ≈19 Å during the induction period. At long times the CTABr/TMOS = 0.139 sample exhibits a first-order diffraction peak at Q = 0.133 Å<sup>-1</sup>, corresponding to cooperative scattering from an ordered mesostructure. An analogous peak is not observed in the CTABr/TMOS = 0.093 solution. This is discussed in terms of different film formation mechanisms and compared with previous data measured by X-ray reflection techniques at the air/water interface.</p>}},
  author       = {{Brennan, Tessa and Roser, Stephen J. and Mann, Stephen and Edler, Karen J.}},
  issn         = {{0897-4756}},
  language     = {{eng}},
  month        = {{10}},
  number       = {{10}},
  pages        = {{4292--4299}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Chemistry of Materials}},
  title        = {{Structural evolution of surfactant - Silica film-forming solutions, investigated using small-angle neutron scattering}},
  url          = {{http://dx.doi.org/10.1021/cm020399l}},
  doi          = {{10.1021/cm020399l}},
  volume       = {{14}},
  year         = {{2002}},
}