Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics

Ponomarev, Ilia; van Duin, Adri C.  T.; Kroll, Peter

doi:10.1021/acs.jpcc.9b03810

Title: Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics

Journal Article · 10 June 2019 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.9b03810 · OSTI ID:1542912

^[1];

^[2];

^[1]

Univ. of Texas, Arlington, TX (United States)
Pennsylvania State Univ., University Park, PA (United States)

We provide a new reactive force field (ReaxFF) for simulations of silicon oxycarbide (SiCO) ceramics and of their syntheses from inorganic polymer precursors. The validity of the force field is extensively tested against experimental and computational thermochemical data. Its performance in simulation at elevated temperatures is gauged by the results of comprehensive ab initio molecular dynamics simulations. We apply the force field to the formation of amorphous SiCO in a simulated polymer pyrolysis. Modeling results are in good agreement with experimental observations and allow new insights into the formation of graphene segregations embedded in an amorphous oxycarbide matrix. The new ReaxFF for Si-C-O-H compounds enables large- scale and long-time atomistic simulations with unprecedented fidelity.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Univ. of Virginia, Charlottesville, VA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008195

OSTI ID:: 1542912

Journal Information:: Journal of Physical Chemistry. C, Vol. 123, Issue 27; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 17 works

Citation information provided by
Web of Science

References (58)

Chemical Durability of Silicon Oxycarbide Glasses Sorarù, Gian Domenico; Modena, Stefano; Guadagnino, Emanuel Journal of the American Ceramic Society, Vol. 85, Issue 6 https://doi.org/10.1111/j.1151-2916.2002.tb00308.x	journal	June 2002
Microstructural and mechanical characterization of sol gel-derived Si–O–C glasses Walter, S.; Soraru, G. D.; Bréquel, H. Journal of the European Ceramic Society, Vol. 22, Issue 13 https://doi.org/10.1016/s0955-2219(01)00537-4	journal	December 2002
Influence of free carbon on the Young's modulus and hardness of polymer‐derived silicon oxycarbide glasses Sorarù, Gian Domenico; Kundanati, Lakshminath; Santhosh, Balanand Journal of the American Ceramic Society https://doi.org/10.1111/jace.16131	journal	October 2018
A Hydrogen-Permselective Silicon Oxycarbide Membrane Derived from Polydimethylsilane Lee, Lang-Luen; Tsai, Dah-Shyang Journal of the American Ceramic Society, Vol. 82, Issue 10 https://doi.org/10.1111/j.1151-2916.1999.tb02158.x	journal	October 1999
Physical and Barrier Properties of Amorphous Silicon-Oxycarbide Deposited by PECVD from Octamethylcyclotetrasiloxane Chiang, Chiu-Chih; Chen, Mao-Chieh; Li, Lain-Jong Journal of The Electrochemical Society, Vol. 151, Issue 9 https://doi.org/10.1149/1.1778169	journal	January 2004
Hydrogen enhances the radiation resistance of amorphous silicon oxycarbides Ding, Hepeng; Demkowicz, Michael J. Acta Materialia, Vol. 136 https://doi.org/10.1016/j.actamat.2017.07.017	journal	September 2017
Superior radiation tolerant materials: Amorphous silicon oxycarbide Nastasi, Michael; Su, Qing; Price, Lloyd Journal of Nuclear Materials, Vol. 461 https://doi.org/10.1016/j.jnucmat.2015.02.039	journal	June 2015
Chemical oxidation of silicon oxycarbide ceramics for advanced drug delivery systems Tamayo, Aitana; Ruiz-Caro, Roberto; Mazo, Alejandra Journal of Materials Science, Vol. 51, Issue 3 https://doi.org/10.1007/s10853-015-9457-3	journal	September 2015
Silicon oxycarbide glass-graphene composite paper electrode for long-cycle lithium-ion batteries David, Lamuel; Bhandavat, Romil; Barrera, Uriel Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms10998	journal	March 2016
Polymer-Derived Ceramics: 40 Years of Research and Innovation in Advanced Ceramics: Polymer-Derived Ceramics Colombo, Paolo; Mera, Gabriela; Riedel, Ralf Journal of the American Ceramic Society https://doi.org/10.1111/j.1551-2916.2010.03876.x	journal	June 2010
Comparative study of the effects of thermal treatment on the optical properties of hydrogenated amorphous silicon-oxycarbide Gallis, Spyros; Nikas, Vasileios; Huang, Mengbing Journal of Applied Physics, Vol. 102, Issue 2 https://doi.org/10.1063/1.2753572	journal	July 2007
Precursor chemistry for ULK CVD Rouessac, V.; Favennec, L.; Rémiat, B. Microelectronic Engineering, Vol. 82, Issue 3-4 https://doi.org/10.1016/j.mee.2005.07.071	journal	December 2005
Synthesis and characterization of inorganic silicon oxycarbide glass thin films by reactive rf-magnetron sputtering Ryan, Joseph V.; Pantano, C. G. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 25, Issue 1 https://doi.org/10.1116/1.2404688	journal	January 2007
Systematic Structural Characterization of the High-Temperature Behavior of Nearly Stoichiometric Silicon Oxycarbide Glasses Bréquel, H.; Parmentier, J.; Walter, S. Chemistry of Materials, Vol. 16, Issue 13 https://doi.org/10.1021/cm049847a	journal	June 2004
Microstructural Evolution of Thermally Treated Low-Dielectric Constant SiOC:H Films Prepared by PECVD Das, G.; Mariotto, G.; Quaranta, A. Journal of The Electrochemical Society, Vol. 153, Issue 3 https://doi.org/10.1149/1.2165781	journal	January 2006
Structural Characterization of Sol-Gel Derived Oxycarbide Glasses. 1. Study of the Pyrolysis Process Bois, Laurence; Maquet, Jocelyne; Babonneau, Florence Chemistry of Materials, Vol. 6, Issue 6 https://doi.org/10.1021/cm00042a016	journal	June 1994
First-Principles Calculations and Analysis of ²⁹ Si Nuclear Magnetic Resonance Chemical Shifts in Silicon Oxycarbide Ceramics Nimmo, John P.; Kroll, Peter The Journal of Physical Chemistry C, Vol. 118, Issue 51 https://doi.org/10.1021/jp510021z	journal	December 2014
Polymer-derived SiCN and SiOC ceramics – structure and energetics at the nanoscale Mera, Gabriela; Navrotsky, Alexandra; Sen, Sabyasachi Journal of Materials Chemistry A, Vol. 1, Issue 12 https://doi.org/10.1039/c2ta00727d	journal	January 2013
Ceramic Nanocomposites from Tailor-Made Preceramic Polymers Mera, Gabriela; Gallei, Markus; Bernard, Samuel Nanomaterials, Vol. 5, Issue 2 https://doi.org/10.3390/nano5020468	journal	April 2015
Silicon oxycarbide glasses and glass-ceramics: “All-Rounder” materials for advanced structural and functional applications Stabler, Christina; Ionescu, Emanuel; Graczyk-Zajac, Magdalena Journal of the American Ceramic Society, Vol. 101, Issue 11 https://doi.org/10.1111/jace.15932	journal	August 2018
Modelling and simulation of amorphous silicon oxycarbide Kroll, Peter Journal of Materials Chemistry, Vol. 13, Issue 7 https://doi.org/10.1039/b301389h	journal	January 2003
Searching insight into the atomistic structure of SiCO ceramics Kroll, Peter Journal of Materials Chemistry, Vol. 20, Issue 46 https://doi.org/10.1039/c0jm01583k	journal	January 2010
ReaxFF: A Reactive Force Field for Hydrocarbons van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois The Journal of Physical Chemistry A, Vol. 105, Issue 41 https://doi.org/10.1021/jp004368u	journal	October 2001
Thermal Stability of Organic Monolayers Grafted to Si(111): Insights from ReaxFF Reactive Molecular Dynamics Simulations Soria, Federico A.; Zhang, Weiwei; van Duin, Adri C. T. ACS Applied Materials & Interfaces, Vol. 9, Issue 36 https://doi.org/10.1021/acsami.7b05444	journal	August 2017
Si/C/H ReaxFF Reactive Potential for Silicon Surfaces Grafted with Organic Molecules Soria, Federico A.; Zhang, Weiwei; Paredes-Olivera, Patricia A. The Journal of Physical Chemistry C, Vol. 122, Issue 41 https://doi.org/10.1021/acs.jpcc.8b07075	journal	June 2018
Oxidation of Silicon Carbide by O ₂ and H ₂ O: A ReaxFF Reactive Molecular Dynamics Study, Part I Newsome, David A.; Sengupta, Debasis; Foroutan, Hosein The Journal of Physical Chemistry C, Vol. 116, Issue 30 https://doi.org/10.1021/jp306391p	journal	July 2012
Hydrogen reverses the clustering tendency of carbon in amorphous silicon oxycarbide Ding, Hepeng; Demkowicz, Michael J. Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep13051	journal	August 2015
Reactive Dynamics Simulation Study on the Pyrolysis of Polymer Precursors To Generate Amorphous Silicon Oxycarbide Structures Gao, Hongfei; Wang, Hongjie; Zhao, Zihao The Journal of Physical Chemistry C, Vol. 122, Issue 10 https://doi.org/10.1021/acs.jpcc.7b12287	journal	February 2018
Development of a ReaxFF Potential for Carbon Condensed Phases and Its Application to the Thermal Fragmentation of a Large Fullerene Srinivasan, Sriram Goverapet; van Duin, Adri C. T.; Ganesh, P. The Journal of Physical Chemistry A, Vol. 119, Issue 4 https://doi.org/10.1021/jp510274e	journal	January 2015
Structure and reactivity of amorphous silicon nitride investigated with density-functional methods Kroll, Peter Journal of Non-Crystalline Solids, Vol. 293-295 https://doi.org/10.1016/s0022-3093(01)00676-7	journal	November 2001
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Parallel reactive molecular dynamics: Numerical methods and algorithmic techniques Aktulga, H. M.; Fogarty, J. C.; Pandit, S. A. Parallel Computing, Vol. 38, Issue 4-5 https://doi.org/10.1016/j.parco.2011.08.005	journal	April 2012
Canonical sampling through velocity rescaling Bussi, Giovanni; Donadio, Davide; Parrinello, Michele The Journal of Chemical Physics, Vol. 126, Issue 1 https://doi.org/10.1063/1.2408420	journal	January 2007
ARXPS studies of SiO ₂ -SiC interfaces and oxidation of 6H SiC single crystal Si-(001) and C-(00 1 ) surfaces Hornetz, B.; Michel, H-J.; Halbritter, J. Journal of Materials Research, Vol. 9, Issue 12 https://doi.org/10.1557/jmr.1994.3088	journal	December 1994
Silicon oxycarbide formation on SiC surfaces and at the SiC/SiO2 interface Önneby, C.; Pantano, C. G. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 15, Issue 3 https://doi.org/10.1116/1.580951	journal	May 1997
Influence of the polymer architecture on the high temperature behavior of SiCO glasses: A comparison between linear- and cyclic-derived precursors Dibandjo, P.; Diré, S.; Babonneau, F. Journal of Non-Crystalline Solids, Vol. 356, Issue 3 https://doi.org/10.1016/j.jnoncrysol.2009.10.006	journal	February 2010
Elucidation of the atomic-scale mechanism of the anisotropic oxidation rate of 4H-SiC between the (0001) Si-face and ( 000 1 ¯) C-face by using a new Si-O-C interatomic potential Takamoto, So; Yamasaki, Takahiro; Ohno, Takahisa Journal of Applied Physics, Vol. 123, Issue 18 https://doi.org/10.1063/1.5028273	journal	May 2018
Creep Viscosity and Stress Relaxation of Gel-Derived Silicon Oxycarbide Glasses Rouxel, Tanguy; Soraru, Gian-Domenico; Vicens, Jean Journal of the American Ceramic Society, Vol. 84, Issue 5 https://doi.org/10.1111/j.1151-2916.2001.tb00789.x	journal	May 2001
Notes - Thermal Rearrangement of Hexamethyldisilane to Trimethyl(dimethylsilylmethyl)silane Shiina, Kyo; Kumada, Makoto The Journal of Organic Chemistry, Vol. 23, Issue 1 https://doi.org/10.1021/jo01095a635	journal	January 1958
Revisiting silica with ReaxFF: Towards improved predictions of glass structure and properties via reactive molecular dynamics Yu, Yingtian; Wang, Bu; Wang, Mengyi Journal of Non-Crystalline Solids, Vol. 443 https://doi.org/10.1016/j.jnoncrysol.2016.03.026	journal	July 2016
Dynamics of Confined Reactive Water in Smectite Clay–Zeolite Composites Pitman, Michael C.; van Duin, Adri C. T. Journal of the American Chemical Society, Vol. 134, Issue 6 https://doi.org/10.1021/ja208894m	journal	February 2012
Interatomic potential for Si–O systems using Tersoff parameterization Munetoh, Shinji; Motooka, Teruaki; Moriguchi, Koji Computational Materials Science, Vol. 39, Issue 2 https://doi.org/10.1016/j.commatsci.2006.06.010	journal	April 2007
Structural and Chemical Properties of Silyl Radicals Chatgilialoglu, Chryssostomos. Chemical Reviews, Vol. 95, Issue 5 https://doi.org/10.1021/cr00037a005	journal	July 1995
Molecular dynamics investigation of structure and high-temperature mechanical properties of SiBCO ceramics Liao, Ningbo; Xue, Wei; Zhou, Hongming Journal of Alloys and Compounds, Vol. 610 https://doi.org/10.1016/j.jallcom.2014.04.189	journal	October 2014
Synthesis and characterization of carbon-enriched silicon oxycarbides Blum, Yigal D.; MacQueen, D. Brent; Kleebe, Hans-Joachim Journal of the European Ceramic Society, Vol. 25, Issue 2-3 https://doi.org/10.1016/j.jeurceramsoc.2004.07.019	journal	January 2005
Porous and high surface area silicon oxycarbide-based materials—A review Lu, Kathy Materials Science and Engineering: R: Reports, Vol. 97 https://doi.org/10.1016/j.mser.2015.09.001	journal	November 2015
SiOC ceramic with high excess free carbon Kleebe, Hans-Joachim; Blum, Yigal D. Journal of the European Ceramic Society, Vol. 28, Issue 5 https://doi.org/10.1016/j.jeurceramsoc.2007.09.024	journal	January 2008
Structural Design of Polymer-Derived SiOC Ceramic Aerogels for High-Rate Li Ion Storage Applications Vallachira Warriam Sasikumar, Pradeep; Zera, Emanuele; Graczyk-Zajac, Magdalena Journal of the American Ceramic Society, Vol. 99, Issue 9 https://doi.org/10.1111/jace.14323	journal	June 2016
The Li-storage capacity of SiOC glasses with and without mixed silicon oxycarbide bonds Graczyk-Zajac, Magdalena; Vrankovic, Dragoljub; Waleska, Philipp Journal of Materials Chemistry A, Vol. 6, Issue 1 https://doi.org/10.1039/c7ta09236a	journal	January 2018
Silicon Oxycarbide-Derived Carbon as Potential NO ₂ Gas Sensor: A First Principles’ Study Liao, Ningbo; Zhou, Hongming; Zheng, Beirong IEEE Electron Device Letters, Vol. 39, Issue 11 https://doi.org/10.1109/led.2018.2869158	journal	November 2018
New insights into the sol–gel condensation of silica by reactive molecular dynamics simulations Du, Tao; Li, Hui; Sant, Gaurav The Journal of Chemical Physics, Vol. 148, Issue 23 https://doi.org/10.1063/1.5027583	journal	June 2018
Pyrolysis Kinetics for the Conversion of a Polymer into an Amorphous Silicon Oxycarbide Ceramic Sorarù, Gian Domenico; Pederiva, Luca; Latournerie, Jérôme Journal of the American Ceramic Society, Vol. 85, Issue 9 https://doi.org/10.1111/j.1151-2916.2002.tb00432.x	journal	September 2002
Pyrolytic conversion of organopolysiloxanes Hourlier, Djamila; Venkatachalam, Srisaran; Ammar, Mohamed-Ramzi Journal of Analytical and Applied Pyrolysis, Vol. 123 https://doi.org/10.1016/j.jaap.2016.11.016	journal	January 2017
Heat capacities, entropies, and Gibbs free energies of formation of low-k amorphous Si(O)CH dielectric films and implications for stability during processing Chen, Jiewei; Calvin, Jason; Asplund, Megan The Journal of Chemical Thermodynamics, Vol. 128 https://doi.org/10.1016/j.jct.2018.08.026	journal	January 2019
Thermal conductivity of plasma deposited amorphous hydrogenated boron and carbon rich thin films Harikrishna, Hari; Lanford, William A.; King, Sean W. Journal of Nuclear Materials, Vol. 514 https://doi.org/10.1016/j.jnucmat.2018.11.031	journal	February 2019
Influence of topological constraints on ion damage resistance of amorphous hydrogenated silicon carbide Su, Qing; Wang, Tianyao; Gigax, Jonathan Acta Materialia, Vol. 165 https://doi.org/10.1016/j.actamat.2018.12.016	journal	February 2019

Cited By (1)

Metal-catalyst-free access to multiwalled carbon nanotubes/silica nanocomposites (MWCNT/SiO ₂ ) from a single-source precursor Mera, Gabriela; Kroll, Peter; Ponomarev, Ilia Dalton Transactions, Vol. 48, Issue 29 https://doi.org/10.1039/c9dt01783f	journal	January 2019

Similar Records

Atomistic Scale Analysis of the Carbonization Process for C/H/O/N-Based Polymers with the ReaxFF Reactive Force Field

Journal Article · 2019 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry · OSTI ID:1542911

Kowalik, Malgorzata; Ashraf, Chowdhury; Damirchi, Behzad; +3 more

Simulating the Initial Stage of Phenolic-resin Carbonization via the Reactive Force Field

Journal Article · 2009 · Journal of Physical Chemistry A · OSTI ID:967125

Jiang, Deen; GoddardIII, William A; Dai, Sheng

Reactive molecular dynamics simulation and chemical kinetic modeling of pyrolysis and combustion of n-dodecane

Journal Article · 2011 · Combustion and Flame · OSTI ID:21401353

Wang, Quan-De; Wang, Jing-Bo; Li, Juan-Qin; +2 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics

Citation Formats

References (58)

Cited By (1)

Similar Records

Related Subjects