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Simulations on the Thermal Decomposition of a Poly(dimethylsiloxane) Polymer Using the ReaxFF Reactive Force Field
Abstract
To investigate the failure of the poly(dimethylsiloxane) polymer (PDMS) at high temperatures and pressures and in the presence of various additives, we have expanded the ReaxFF reactive force field to describe carbon-silicon systems. From molecular dynamics (MD) simulations using ReaxFF we find initial thermal decomposition products of PDMS to be CH(3) radical and the associated polymer radical, indicating that decomposition and subsequent cross-linking of the polymer is initiated by Si-C bond cleavage, in agreement with experimental observations. Secondary reactions involving these CH(3) radicals lead primarily to formation of methane. We studied temperature and pressure dependence of PDMS decomposition by following the rate of production of methane in the ReaxFF MD simulations. We tracked the temperature dependency of the methane production to extract Arrhenius parameters for the failure modes of PDMS. Furthermore, we found that at increased pressures the rate of PDMS decomposition drops considerably, leading to the formation of fewer CH(3) radicals and methane molecules. Finally, we studied the influence of various additives on PDMS stability. We found that the addition of water or a SiO(2) slab has no direct effect on the short-term stability of PDMS, but addition of reactive species such as ozone leads to significantly lower PDMS decomposition temperature. The addition of nitrogen monoxide does not significantly alter the degradation temperature but does retard the initial production of methane and C(2) hydrocarbons until the nitrogen monoxide is depleted. These results, and their good agreement with available experimental data, demonstrate that ReaxFF provides a useful computational tool for studying the chemical stability of polymers.
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Cites
Generalized Gradient Approximation Made Simple
Perdew, J. P., Burke, K., & Ernzerhof, M. (1996) · Physical Review Letters · doi:10.1103/physrevlett.77.3865 · Cited by 215,824
Density-functional thermochemistry. III. The role of exact exchange
Becke, A. D. (1993) · The Journal of Chemical Physics · doi:10.1063/1.464913 · Cited by 103,767
Lee, C., Yang, W., & Parr, R. G. (1988) · Physical Review B · doi:10.1103/physrevb.37.785 · Cited by 100,874
Special points for Brillouin-zone integrations
Monkhorst, H. J., & Pack, J. D. (1976) · Physical Review B · doi:10.1103/physrevb.13.5188 · Cited by 71,721
Perdew, J. P., Chevary, J. A., Vosko, S. H., Jackson, K. A., Pederson, M. R., Singh, D. J., & Fiolhais, C. (1992) · Physical Review B · doi:10.1103/physrevb.46.6671 · Cited by 22,269
Self-consistent molecular orbital methods. XX. A basis set for correlated wave functions
Krishnan, R., Binkley, J. S., Seeger, R., & Pople, J. A. (1980) · The Journal of Chemical Physics · doi:10.1063/1.438955 · Cited by 17,772
Perdew, J. P., Chevary, J. A., Vosko, S. H., Jackson, K. A., Pederson, M. R., Singh, D. J., & Fiolhais, C. (1993) · Physical Review B · doi:10.1103/physrevb.48.4978.2 · Cited by 17,144
The influence of polarization functions on molecular orbital hydrogenation energies
Hariharan, P. C., & Pople, J. A. (1973) · Theoretica Chimica Acta · doi:10.1007/bf00533485 · Cited by 15,816
Payne, M. C., Teter, M. P., Allan, D. C., Arias, T. A., & Joannopoulos, J. D. (1992) · Reviews of Modern Physics · doi:10.1103/revmodphys.64.1045 · Cited by 9,728
Francl, M. M., Pietro, W. J., Hehre, W. J., Binkley, J. S., Gordon, M. S., DeFrees, D. J., & Pople, J. A. (1982) · The Journal of Chemical Physics · doi:10.1063/1.444267 · Cited by 8,187
Clark, T., Chandrasekhar, J., Spitznagel, G. W., & Schleyer, P. V. R. (1983) · Journal of Computational Chemistry · doi:10.1002/jcc.540040303 · Cited by 7,224
ReaxFF: A Reactive Force Field for Hydrocarbons
van Duin, A. C. T., Dasgupta, S., Lorant, F., & Goddard, W. A. (2001) · The Journal of Physical Chemistry A · doi:10.1021/jp004368u · Cited by 6,402
Self-citationEncyclopedia of polymer science and technology
(2003) · Choice Reviews Online · doi:10.5860/choice.41-0674 · Cited by 5,095
Brenner, D. W. (1990) · Physical Review B · doi:10.1103/physrevb.42.9458 · Cited by 4,030
New empirical approach for the structure and energy of covalent systems
Tersoff, J. (1988) · Physical Review B · doi:10.1103/physrevb.37.6991 · Cited by 3,529
Physical properties of polymers handbook
(1996) · Choice Reviews Online · doi:10.5860/choice.34-2186 · Cited by 1,047
ReaxFFSiO Reactive Force Field for Silicon and Silicon Oxide Systems
van Duin, A. C. T., Strachan, A., Stewman, S., Zhang, Q., Xu, X., & Goddard, W. A. (2003) · The Journal of Physical Chemistry A · doi:10.1021/jp0276303 · Cited by 1,011
Self-citationPolydimethylsiloxane thermal degradation Part 1. Kinetic aspects
Camino, G., Lomakin, S. M., & Lazzari, M. (2001) · Polymer · doi:10.1016/s0032-3861(00)00652-2 · Cited by 795
Shock Waves in High-Energy Materials: The Initial Chemical Events in Nitramine RDX
Strachan, A., van Duin, A. C. T., Chakraborty, D., Dasgupta, S., & Goddard, W. A. (2003) · Physical Review Letters · doi:10.1103/physrevlett.91.098301 · Cited by 606
Self-citationThermal polydimethylsiloxane degradation. Part 2. The degradation mechanisms
Camino, G., Lomakin, S. M., & Lageard, M. (2002) · Polymer · doi:10.1016/s0032-3861(01)00785-6 · Cited by 566
Thermal analysis of polydimethylsiloxanes. I. Thermal degradation in controlled atmospheres
Thomas, T. H., & Kendrick, T. C. (1969) · Journal of Polymer Science Part A-2: Polymer Physics · doi:10.1002/pol.1969.160070308 · Cited by 320
Adhesion and nonwetting-wetting transition in theAl/α−Al2O3interface
Zhang, Q., Çaǧın, T., van Duin, A., Goddard, W. A., Qi, Y., & Hector, L. G. (2004) · Physical Review B · doi:10.1103/physrevb.69.045423 · Cited by 224
Self-citationMechanism of the Acid-Catalyzed Si−O Bond Cleavage in Siloxanes and Siloxanols. A Theoretical Study
Cypryk, M., & Apeloig, Y. (2002) · Organometallics · doi:10.1021/om011055s · Cited by 219
Deshpande, G., & Rezac, M. E. (2002) · Polymer Degradation and Stability · doi:10.1016/s0141-3910(01)00261-0 · Cited by 161
Landis, C., Cleveland, T., & Firman, T. (1998) · Journal of the American Chemical Society · doi:10.1021/ja9734859 · Cited by 108
The conformation of poly(dimethylsiloxane) in the crystalline state
Albouy, P. (2000) · Polymer · doi:10.1016/s0032-3861(99)00664-3 · Cited by 54
Cited by
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Chenoweth, K., van Duin, A. C. T., & Goddard, W. A. (2008) · The Journal of Physical Chemistry A · doi:10.1021/jp709896w · Cited by 2,697
Self-citationParallel reactive molecular dynamics: Numerical methods and algorithmic techniques
Aktulga, H. M., Fogarty, J. C., Pandit, S. A., & Grama, A. Y. (2012) · Parallel Computing · doi:10.1016/j.parco.2011.08.005 · Cited by 1,070
Additive manufacturing of structural materials
Liu, G., Zhang, X., Chen, X., He, Y., Cheng, L., Huo, M., Yin, J., Hao, F., Chen, S., Wang, P., et al. (2021) · Materials Science and Engineering: R: Reports · doi:10.1016/j.mser.2020.100596 · Cited by 707
Liu, L., Liu, Y., Zybin, S. V., Sun, H., & Goddard, W. A. (2011) · The Journal of Physical Chemistry A · doi:10.1021/jp201599t · Cited by 566
Self-citationNanoscale heat transfer – from computation to experiment
Luo, T., & Chen, G. (2013) · Physical Chemistry Chemical Physics · doi:10.1039/c2cp43771f · Cited by 273
Metadata
- Authors
- Chenoweth, K., Cheung, S., van Duin, A. C. T., Goddard, W. A., & Kober, E. M.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2005-04-20
- Volume
- 127
- Issue
- 19
- Pages
- 7192-7202
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2059344540
- Cited by
- 498
- References
- 26
- FWCI
- 5.64
- Type
- journal article
- Language
- en
- Open access
- closed
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