Molecular simulation of silica/surfactant self-assembly in the synthesis of periodic mesoporous silicas

Miguel Jorge, Jose R. B. Gomes, M. Natalia D. S. Cordeiro, Nigel A. Seaton

Research output: Contribution to journalArticle

30 Citations (Scopus)

Abstract

Understanding the synthesis of periodic mesoporous silica (PMS) is crucial for a more efficient use of these materials and is a necessary first step toward a rational design strategy for the templated synthesis of porous solids. In this paper, the early stages of the synthesis process of PMS materials are simulated directly by molecular dynamics, using realistic atomistic models. It is the first time that such computationally demanding calculations have been attempted. By comparing the self-assembly of cationic surfactants in the presence and absence of silicates, we are able to show that silica promotes the formation of larger aggregates than in a simple surfactant/water solution. The formation of these larger micelles is explained by a strong interaction of the silicate molecules with the surfactant head groups. This strong interaction increases the local concentration of silica at the surface of the micelles, which induces the formation of more condensed silicate species. The surfactant/silica structures observed here are potentially important intermediates in PMS synthesis.

LanguageEnglish
Pages15414-15415
Number of pages2
JournalJournal of the American Chemical Society
Volume129
Issue number50
Early online date23 Nov 2007
DOIs
Publication statusPublished - 19 Dec 2007

Fingerprint

Surface-Active Agents
Silicon Dioxide
Self assembly
Surface active agents
Silica
Silicates
Micelles
Cationic surfactants
Molecular Dynamics Simulation
Molecular dynamics
Molecules
Water

Keywords

  • molecular simulation
  • silica/surfactant
  • self-assembly
  • synthesis
  • periodic mesoporous silicas
  • PMS
  • rational design strategy

Cite this

Jorge, Miguel ; Gomes, Jose R. B. ; D. S. Cordeiro, M. Natalia ; Seaton, Nigel A. / Molecular simulation of silica/surfactant self-assembly in the synthesis of periodic mesoporous silicas. In: Journal of the American Chemical Society. 2007 ; Vol. 129, No. 50. pp. 15414-15415.
@article{8ee3cf0f39f34327a8365844c6a46ff2,
title = "Molecular simulation of silica/surfactant self-assembly in the synthesis of periodic mesoporous silicas",
abstract = "Understanding the synthesis of periodic mesoporous silica (PMS) is crucial for a more efficient use of these materials and is a necessary first step toward a rational design strategy for the templated synthesis of porous solids. In this paper, the early stages of the synthesis process of PMS materials are simulated directly by molecular dynamics, using realistic atomistic models. It is the first time that such computationally demanding calculations have been attempted. By comparing the self-assembly of cationic surfactants in the presence and absence of silicates, we are able to show that silica promotes the formation of larger aggregates than in a simple surfactant/water solution. The formation of these larger micelles is explained by a strong interaction of the silicate molecules with the surfactant head groups. This strong interaction increases the local concentration of silica at the surface of the micelles, which induces the formation of more condensed silicate species. The surfactant/silica structures observed here are potentially important intermediates in PMS synthesis.",
keywords = "molecular simulation , silica/surfactant , self-assembly, synthesis, periodic mesoporous silicas, PMS, rational design strategy",
author = "Miguel Jorge and Gomes, {Jose R. B.} and {D. S. Cordeiro}, {M. Natalia} and Seaton, {Nigel A.}",
note = "This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of the American Chemical Society, copyright {\circledC} American Chemical Society after peer review. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/ja075070l.",
year = "2007",
month = "12",
day = "19",
doi = "10.1021/ja075070l",
language = "English",
volume = "129",
pages = "15414--15415",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "American Chemical Society",
number = "50",

}

Molecular simulation of silica/surfactant self-assembly in the synthesis of periodic mesoporous silicas. / Jorge, Miguel; Gomes, Jose R. B.; D. S. Cordeiro, M. Natalia; Seaton, Nigel A.

In: Journal of the American Chemical Society, Vol. 129, No. 50, 19.12.2007, p. 15414-15415.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Molecular simulation of silica/surfactant self-assembly in the synthesis of periodic mesoporous silicas

AU - Jorge, Miguel

AU - Gomes, Jose R. B.

AU - D. S. Cordeiro, M. Natalia

AU - Seaton, Nigel A.

N1 - This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of the American Chemical Society, copyright © American Chemical Society after peer review. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/ja075070l.

PY - 2007/12/19

Y1 - 2007/12/19

N2 - Understanding the synthesis of periodic mesoporous silica (PMS) is crucial for a more efficient use of these materials and is a necessary first step toward a rational design strategy for the templated synthesis of porous solids. In this paper, the early stages of the synthesis process of PMS materials are simulated directly by molecular dynamics, using realistic atomistic models. It is the first time that such computationally demanding calculations have been attempted. By comparing the self-assembly of cationic surfactants in the presence and absence of silicates, we are able to show that silica promotes the formation of larger aggregates than in a simple surfactant/water solution. The formation of these larger micelles is explained by a strong interaction of the silicate molecules with the surfactant head groups. This strong interaction increases the local concentration of silica at the surface of the micelles, which induces the formation of more condensed silicate species. The surfactant/silica structures observed here are potentially important intermediates in PMS synthesis.

AB - Understanding the synthesis of periodic mesoporous silica (PMS) is crucial for a more efficient use of these materials and is a necessary first step toward a rational design strategy for the templated synthesis of porous solids. In this paper, the early stages of the synthesis process of PMS materials are simulated directly by molecular dynamics, using realistic atomistic models. It is the first time that such computationally demanding calculations have been attempted. By comparing the self-assembly of cationic surfactants in the presence and absence of silicates, we are able to show that silica promotes the formation of larger aggregates than in a simple surfactant/water solution. The formation of these larger micelles is explained by a strong interaction of the silicate molecules with the surfactant head groups. This strong interaction increases the local concentration of silica at the surface of the micelles, which induces the formation of more condensed silicate species. The surfactant/silica structures observed here are potentially important intermediates in PMS synthesis.

KW - molecular simulation

KW - silica/surfactant

KW - self-assembly

KW - synthesis

KW - periodic mesoporous silicas

KW - PMS

KW - rational design strategy

UR - http://pubs.acs.org/journal/jacsat

U2 - 10.1021/ja075070l

DO - 10.1021/ja075070l

M3 - Article

VL - 129

SP - 15414

EP - 15415

JO - Journal of the American Chemical Society

T2 - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 50

ER -