Molecular dynamics-quantum model simulation of pyrolysis reactivity of kerogen in oil shale from Fushun
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摘要: 采用MS(Materials Studio 2017)软件中Forcite模块,对自主构建的抚顺油页岩干酪根二维结构模型进行能量最小化分子动力学模拟,通过能量最优化过程得到干酪根初始优化结构。在此基础上进行分子动力学退火模拟,获得全局能量最优化构型,即油页岩干酪根分子三维结构模型。基于密度泛函理论的量子力学模拟方法,计算分析干酪根三维结构模型的动力学、键能、键级、电荷密度等参数,分析化学活性位点,探讨了干酪根热解微观化学演化机理,进而预测了反应性。Abstract: Using the Forcite module in MS (Materials Studio 2017) software, the energy minimization molecular dynamics simulation was performed on the self-constructed two-dimensional structural model of Fushun oil shale kerogen, and the initial optimized structure of kerogen was obtained through the energy optimization process. Then, molecular dynamics annealing simulations were performed to obtain a global energy optimization configuration, ie a three-dimensional structural model of oil shale kerogen molecules. Based on the density functional theory of quantum mechanics simulation method, a three-dimensional structural model of kerogen dynamics, bond energy, bond level, charge density and other parameters were calculated, and the chemical active sites were analyzed. The microchemical evolution mechanism of kerogen pyrolysis was discussed. And then, the reactivity was predicted.
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Key words:
- oil shale /
- kerogen /
- molecular simulation /
- structural model
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表 1 抚顺结构模型结构优化前后的势能变化
Table 1 Changes of potential energy before and after optimization of Fushun structural model
Structure Total energy/ (kcal·mol-1) Valence electron energy/(kcal·mol-1) Non-bond energy/(kcal·mol-1) bond energy angle energy torsion energy inversion energy van der Waals energy electrostatic energy hydrogen bond energy Initial structure 13441.84 2802.15 197.48 130.84 7.33 10286.74 17.31 0.00 Optimized structure 652.29 89.184 219.50 51.43 0.82 352.87 -56.27 -5.25 表 2 抚顺干酪根化学键键级
Table 2 Chemical bond level of Fushun kerogen
Chemical bond Bond order Chemical bond Bond order Chemical bond Bond order C118-S119 0.6185 C265-O266 0.9054 C150-C151 0.9140 S119-C120 0.6319 C74-C200 0.9058 C85-C172 0.9146 S177-C178 0.7123 C97-C196 0.9062 C169-C260 0.9146 C176-S177 0.7638 C75-C76 0.9063 C255-C256 0.9156 C263-O264 0.8726 C223-O270 0.9064 C209-C210 0.9159 C144-C145 0.8743 C82-C183 0.9066 C126-C127 0.9161 C267-O268 0.8774 C253-C254 0.9070 C87-C153 0.9163 C116-C117 0.8876 C175-C176 0.9091 C105-C242 0.9164 C164-C165 0.8923 C214-C215 0.9093 C131-C189 0.9166 C140-C260 0.8963 C113-C114 0.9107 C86-C87 0.9170 C82-C137 0.9027 C159-C160 0.9120 C144-C211 0.9172 C82-C161 0.9027 C144-C261 0.9127 C83-C188 0.9180 C131-C132 0.9030 C197-C198 0.9130 C148-C149 0.9186 C105-C106 0.9053 C164-C263 0.9137 C196-C250 0.9187 -
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