Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics
Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics
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DOI：
10.1021/acs.jpcc.9b03810
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发表时间：
2019-06
期刊：
影响因子：
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通讯作者：
I. Ponomarev;A. V. van Duin;P. Kroll
中科院分区：
文献类型：
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作者：
I. Ponomarev;A. V. van Duin;P. Kroll
我们提供了一种新的反作用力场 (ReaxFF)，用于模拟碳氧化硅 (SiCO) 陶瓷及其由无机聚合物前体的合成。力场的有效性根据实验和计算热化学数据进行了广泛的测试。其在高温模拟中的性能是通过全面的从头算分子动力学模拟的结果来衡量的。我们将力场应用于模拟聚合物热解中无定形 SiCO 的形成。建模结果与实验观察结果非常吻合，并为嵌入无定形碳氧化物基质中的石墨烯偏析的形成提供了新的见解。用于 Si-C-O-H 化合物的新型 ReaxFF 能够以前所未有的保真度实现大规模、长时间的原子模拟。
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.