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Toward a Process-Based Molecular Model of SiC Membranes. 1. Development of a Reactive Force Field

Naserifar, Saber and Liu, Lianchi and Goddard, William A., III and Tsotsis, Theodore T. and Sahimi, Muhammad (2013) Toward a Process-Based Molecular Model of SiC Membranes. 1. Development of a Reactive Force Field. Journal of Physical Chemistry C, 117 (7). pp. 3308-3319. ISSN 1932-7447.

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A broad class of important materials, such as carbon molecular sieves, silicon carbide (SiC), and silicon nitride, are fabricated by temperature-controlled pyrolysis of preceramic polymers. In particular, the fabrication of SiC membranes by pyrolysis of a polymer precursor that contains Si is quite attractive for separation of hydrogen from other gases. It has been quite difficult to extract atomistic-scale information about such SiC membranes since they are amorphous. In principle, ab initio quantum mechanics (QM) can provide information about the structure of the amorphous systems. However, to determine the structure of the SiC membrane layer one should capture in the simulations the various reactive processes involved in forming the layer. This requires QM simulations on systems with about 3000 atoms per cell at temperature of 1200 K for microseconds, which are far beyond the current QM capabilities. Instead, this paper extends the ReaxFF reactive force field, validated for high temperature reactions of other materials, to describe the processes involved in the thermal decomposition of hydridopolycarbosilane (HPCS) to form SiC nanoporous membranes. First, we carry out QM calculations on models meant to capture important reaction steps and structures. Then, we develop a model of the HPCS polymer and utilize ReaxFF to describe the thermal degradation and decomposition of the polymer as the system is heated in the molecular dynamics (MD) simulations. Analysis of the pyrolysis studies and their results leads to various quantities that can be compared with experimental data. Good agreement is found between the data and the results of the MD simulations.

Item Type:Article
Related URLs:
URLURL TypeDescription DOIArticle
Naserifar, Saber0000-0002-1069-9789
Goddard, William A., III0000-0003-0097-5716
Sahimi, Muhammad0000-0002-8009-542X
Additional Information:© 2013 American Chemical Society. Received: August 6, 2012; Revised: January 23, 2013; Published: January 28, 2013. The support of the Office of Energy Sciences, Chemical Sciences, Geosciences & Biosciences Division of the Department of Energy is gratefully acknowledged. T.T.T. also acknowledges the support of the National Science Foundation. W.A.G. received support from the Department of Transportation.
Funding AgencyGrant Number
Department of Energy (DOE)UNSPECIFIED
Department of TransportationUNSPECIFIED
Issue or Number:7
Record Number:CaltechAUTHORS:20130404-093840964
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Official Citation:Toward a Process-Based Molecular Model of SiC Membranes. 1. Development of a Reactive Force Field Saber Naserifar, Lianchi Liu, William A. Goddard, III, Theodore T. Tsotsis, and Muhammad Sahimi The Journal of Physical Chemistry C2013117 (7), 3308-3319
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:37759
Deposited By: Tony Diaz
Deposited On:08 Apr 2013 21:59
Last Modified:03 Oct 2019 04:50

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