Kinetic Monte Carlo simulation of the synthesis of periodic mesoporous silicas SBA-2 and STAC-1

generation of realistic atomistic models

Carlos A. Ferreiro-Rangel, Magdalena M. Lozinska, Paul Wright, Nigel A. Seaton, Tina Düren*

*Corresponding author for this work

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

SBA-2 and STAC-1 are two related periodic mesoporous silicas (PMSs) that have regular networks of spherical, interconnected pores; the pores are similar in the two materials but the networks differ in their symmetry. The nature of the interconnected network of pores in these materials gives rise to interesting properties related to their potential use in separation processes. In this work, we extend a kinetic Monte Carlo (kMC) technique, originally derived for MCM-41, a simpler PMS, and apply it to mimic the condensation, aggregation, deformation, and calcination stages of the synthesis of SBA-2 and STAC-1. Our simulated synthesis results suggest that the pores are connected through windows formed during micelle aggregation because of the close packing of the spherical micelles and the presence of water molecules at the silica-micelle interface. The simulated materials were validated by comparing properties such as unit cell size, pore size, pore shape, and wall density to results from experimental X-ray diffraction (XRD), transmission electron microscopy (TEM), density measurements, and 29Si NMR. Quantitative agreement between simulated and experimental nitrogen isotherms was achieved demonstrating the realism of the pore models obtained by the kMC simulations. Our results highlight the importance of a realistic, rough pore surface for the prediction of adsorption at low pressures in these materials.

Original languageEnglish
Pages (from-to)20966-20974
Number of pages9
JournalJournal of Physical Chemistry C
Volume116
Issue number39
Early online date29 Aug 2012
DOIs
Publication statusPublished - 4 Oct 2012
Externally publishedYes

Fingerprint

Silicon Dioxide
Micelles
Silica
silicon dioxide
porosity
Kinetics
kinetics
synthesis
Agglomeration
simulation
micelles
Multicarrier modulation
Density (specific gravity)
Calcination
Pore size
Isotherms
Condensation
Nitrogen
Nuclear magnetic resonance
Transmission electron microscopy

Cite this

Ferreiro-Rangel, Carlos A. ; Lozinska, Magdalena M. ; Wright, Paul ; Seaton, Nigel A. ; Düren, Tina. / Kinetic Monte Carlo simulation of the synthesis of periodic mesoporous silicas SBA-2 and STAC-1 : generation of realistic atomistic models. In: Journal of Physical Chemistry C. 2012 ; Vol. 116, No. 39. pp. 20966-20974.
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Kinetic Monte Carlo simulation of the synthesis of periodic mesoporous silicas SBA-2 and STAC-1 : generation of realistic atomistic models. / Ferreiro-Rangel, Carlos A.; Lozinska, Magdalena M. ; Wright, Paul; Seaton, Nigel A.; Düren, Tina.

In: Journal of Physical Chemistry C, Vol. 116, No. 39, 04.10.2012, p. 20966-20974.

Research output: Contribution to journalArticle

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AB - SBA-2 and STAC-1 are two related periodic mesoporous silicas (PMSs) that have regular networks of spherical, interconnected pores; the pores are similar in the two materials but the networks differ in their symmetry. The nature of the interconnected network of pores in these materials gives rise to interesting properties related to their potential use in separation processes. In this work, we extend a kinetic Monte Carlo (kMC) technique, originally derived for MCM-41, a simpler PMS, and apply it to mimic the condensation, aggregation, deformation, and calcination stages of the synthesis of SBA-2 and STAC-1. Our simulated synthesis results suggest that the pores are connected through windows formed during micelle aggregation because of the close packing of the spherical micelles and the presence of water molecules at the silica-micelle interface. The simulated materials were validated by comparing properties such as unit cell size, pore size, pore shape, and wall density to results from experimental X-ray diffraction (XRD), transmission electron microscopy (TEM), density measurements, and 29Si NMR. Quantitative agreement between simulated and experimental nitrogen isotherms was achieved demonstrating the realism of the pore models obtained by the kMC simulations. Our results highlight the importance of a realistic, rough pore surface for the prediction of adsorption at low pressures in these materials.

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