CL20/BTF共晶高温热分解ReaxFF/lg分子动力学模拟

用ReaxFF/lg反应力场模拟CL20/BTF共晶在2000~3000 K高温条件下的热分解过程,获得了势能和物种数的演化、初始反应路径及热分解产物等详细信息。通过指数函数对势能的演化曲线进行拟合得到反映特征时间等参数,采用经典的Arrhenius反应速率方程描述总包反应,获得CL20/BTF共晶的活化能E_a=60.8 kcal/mol。研究得到CL20/BTF共晶热分解的初始路径,CL20分子中N-NO₂首先断裂,在热分解起始阶段占主导作用。在不同温度条件下,CL20分子均在BTF分子前完全分解。CL20/BTF共晶的主要产物为NO₂、NO、NO₃、HNO、N₂、H₂O、CO₂、O₂、N₂O、HONO 等。温度对产物均产生一定程度的影响.     

基于ReaxFF反应分子动力学模拟的正十二烷醇的热裂解特性研究

醇类添加剂是提高碳氢燃料再生冷却效率的有效途径之一。特别是多碳醇由于自身高热值成为了潜在的主动冷却介质,而其裂解机理尚未完善。本研究基于反应分子动力学模拟的方法,分别探究了正十二烷、正十二烷醇的热解过程,从分子尺度揭示其反应动力学微观机理,并分析温度等敏感因素对反应速率、产物分布的影响。结果表明,温度的提高会极大地提升热解的反应速率,并且反应物倾向于分解成分子量更小的气体产物。相比于正十二烷,正十二烷醇的起始裂解温度以及活化能更低,其展现了作为主动冷却介质的潜力。     

BaTiO3晶体结构及弹性的分子动力学模拟

有效的势函数是分子动力学模拟的关键. 引入了一种势函数,该势函数的特点是运用参数r_eff计算原子间的静电作用. 通过分子动力学方法模拟得到了BaTiO₃晶体立方相、四方相结构的对关联函数和X射线衍射谱,计算得出了它们的晶格常数及弹性常数. 模拟结果与实验结果符合较好.该势函数可以有效地模拟BaTiO₃晶体的热学和力学性能. 关键词： 分子动力学模拟 势函数 3铁电晶体')" href="#">BaTiO₃铁电晶体     

六硝基六氮杂异伍兹烷/2, 4, 6-三硝基甲苯共晶冲击起爆过程的分子动力学模拟

多尺度冲击技术可以准确的再现含能材料冲击起爆过程中冲击波阵面及反应区内的热力学和化学反应路径. 文本利用反应力场分子动力学(ReaxFF-MD)对六硝基六氮杂异伍兹烷/2, 4, 6-三硝基甲苯(CL20/TNT)1:1共晶沿<110>方向以6–10 km·s^-1的冲击速度进行冲击压缩模拟. 产物识别分析显示当冲击速度≥7 km·s^-1时, 冲击激发化学反应发生, 并且利用Rankine-Hugoniot守恒关系求得冲击起爆压力为24.56 GPa. 再者, 比较了冲击速度与粒子速度, 冲击速度与冲击诱发形变的关系, 当冲击速度为7–8 km·s^-1时, 冲击起爆发生, 系统经历弹- 塑性相变, 初级化学反应及次级化学反应, 并且相变与化学反应同时进行, 对于较高的冲击波速度(≥9 km·s^-1), 共晶系统内为过驱响应, 热力学参数均出现陡峭的梯度变化, 冲击波压缩材料直接阶跃至塑性变形阶段, 并且此阶段出现大量的碳原子.     

ε-CL-20/F2311 PBXs力学性能和结合能的分子动力学模拟

本文应用分子动力学(MD)模拟方法, 研究高能量密度化合物六硝基六氮杂异伍兹烷(ε-CL-20)与常用高聚物粘结剂F2311所构成的CL-20/F2311高聚物粘结炸药(PBXs)的力学性能和结合能随温度和高聚物浓度而变化的规律. 结果表明, 添加高聚物于主体炸药中, 使其弹性模量减小, 表明刚性减小, 弹性增大, 机械力学性能大为改善; 在一定范围内, 随高聚物F2311在PBXs中浓度的增加,体系结合能从正值变为负值, 而随温度升高,体系的结合能变化不是很明显.     

界面结构对Cu/Ni多层膜纳米压痕特性影响的分子动力学模拟

金属多层膜调制周期下降到纳米级时,其力学性质会发生显著改变. Cu-Ni晶格失配度约为2.7%,可以形成共格界面和半共格界面,实验中实现沿[111]方向生长的调制周期为几纳米且具有异孪晶界面结构的Cu/Ni多层膜,其力学性质发生显著改变.本文采用分子动力学方法对共格界面、共格孪晶界面、半共格界面、半共格孪晶界面等四种不同界面结构的Cu/Ni多层膜进行纳米压痕模拟,研究压痕过程中不同界面结构类型的形变演化规律以及位错与界面的相互作用,获取Cu/Ni多层膜不同界面结构对其力学性能的影响特征.计算结果表明,不同界面结构的样品在不同压痕深度时表现出的强化或软化作用机理不同,软化机制主要是由于形成了平行于界面的分位错以及孪晶界面的迁移,强化机制主要是由于界面对位错的限定作用以及失配位错网状结构与孪晶界面迁移时所形成的弓形位错之间的相互作用.     

ε-CL-20/F_(2311) PBXs力学性能和结合能的分子动力学模拟

本文应用分子动力学(MD)模拟方法,研究高能量密度化合物六硝基六氮杂异伍兹烷(ε-CL-20)与常用高聚物粘结剂F2311所构成的CL-20/F2311高聚物粘结炸药(PBXs)的力学性能和结合能随温度和高聚物浓度而变化的规律.结果表明,添加高聚物于主体炸药中,使其弹性模量减小,表明刚性减小,弹性增大,机械力学性能大为改善;在一定范围内,随高聚物F2311在PBXs中浓度的增加,体系结合能从正值变为负值,而随温度升高,体系的结合能变化不是很明显.     

TiO2/ZnO纳米薄膜界面热导率的分子动力学模拟

采用平衡分子动力学方法及Buckingham势研究了金红石型TiO₂薄膜与闪锌矿型ZnO薄膜构筑的纳米薄膜界面沿晶面[0001](z轴方向)的热导率.通过优化分子模拟初始条件中的截断半径r_c和时间步后,计算并分析了平衡温度、薄膜厚度、薄膜截面大小对热导率的影响.研究表明,薄膜热导率受薄膜温度和厚度的影响很大,当温度由300 K升高600 K时,薄膜的热导率逐渐减小;当薄膜厚度由1.8 nm增大到5 nm时,热导率会逐渐增大;并在此基础 关键词： 热导率 分子动力学 2/ZnO纳米薄膜界面')" href="#">TiO₂/ZnO纳米薄膜界面 数值模拟     

Ti75Al25合金微观结构演变的分子动力学模拟

本文利用分子动力学模拟方法,研究了液态Ti₇₅Al₂₅合金在不同冷却条件下形成晶体及非晶的过程(Q1:1.0×10¹³K Ks^-1,Q2:1.0×10¹¹Ks^-1).利用平均原子体积、双体分布函数、键角分布函数、键对分析和Voronoi多面体方法研究了微观局域结构随温度的变化关系.研究发现:在Q1冷却过程中,液态Ti₇₅A1₂₅合金在1000 K发生玻璃化转变,形成非晶结构;而在Q2冷却过程中,液态Ti₇₅Al₂₅合金发生结晶,并最终形成hcp晶体结构.     

水对无定形SiO2拉伸特性影响的反应分子动力学模拟

潮湿对SiO₂的强度有重要影响. 采用反应场分子动力学模拟方法,研究液态水对无定形SiO₂ （a-SiO₂）准静态拉伸特性的影响. 准静态拉伸模拟的结果表明,在干燥条件下,a-SiO₂的拉伸强度为9.4 GPa,而在含液态水时则下降为4.7 GPa,表明液态水使得a-SiO₂拉伸强度发生显著下降. 根据应力-应变曲线分析可知,干燥条件下a-SiO₂结构的刚度随着拉伸应变的增加保持稳定,而含液态水的a-SiO₂刚度随着拉伸应变的增加而逐步降低,并且应变为16%–20%时的应力-应变曲线类似于金属的屈服现象. 通过对拉伸过程的原子图像分析可知,含液态水a-SiO₂的拉伸过程并没有发生塑性变形,而是因为应力增大加速了水解反应,使得应力-应变曲线表现出上述塑性现象. 关键词： 2')" href="#">无定形SiO₂ 机械强度 水 分子动力学模拟     

Diffusion and thermite reaction process of film-honeycomb Al/NiO nanothermite:Molecular dynamics simulations using ReaxFF reactive force field

The diffusion and thermite reaction process of Al/NiO nanothermite composed of Al nanofilm and NiO nano honeycomb are investigated by molecular dynamics simulations in combination with the Reax FF. The diffusion and thermite reaction are characterized by measuring energy release, adiabatic reaction temperature, and activation energy. Based on time evolution of atomic configuration and mean square displacement, the initialization of the thermite reaction process of Al/NiO nanothermite results from the diffusion of Al atoms. Under the microcanonical ensemble, it is found that the adiabatic reaction temperature of the thermite reaction process of Al/NiO nanothermite reaches over 5500 K, and activation energy is 8.43 k J/mol. The release energy of the thermite reaction process of Al/NiO nanothermite is 2.2 k J/g, which is in accordance with the available experimental value. With the same initial temperature, the adiabatic reaction temperature of the thermite reaction process of Al/NiO nanothermite has a tendency to decrease dramatically as the equivalence ratio increases. On the basis of chemical bond analysis, the initial temperature and equivalence ratio have great effects on the thermite reaction process, but do not significantly affect the average length of Al–Ni nor Al–O bond. Overall, the thermite reaction of film-honeycomb Al/NiO nanothermite is a complicated process instead of a theoretical equation.     

HMX不同晶型热膨胀特性及相变的ReaxFF分子动力学模拟

HMX（octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine）晶体不同晶型对温度的响应对于深入认识含能材料在外加载荷下的感度、稳定性、相变等具有重要意义．采用ReaxFF—lg势函数和等温等压分子动力学（NPT-MD）方法,研究了β-,δ-和α-HMX三种固态晶型在T=303—503K内的晶体结构和分子结构．结果表明,ReaxFF—lg势函数能够合理地描述HMX晶体的热膨胀行为,计算得到的晶体结构和热膨胀系数与实验数据比较符合．三种晶型的线膨胀系数表明,β-HMX晶体具有明显的热膨胀各向异性;δ-HMX晶体C轴的热膨胀特性与a,b轴略有不同;α-HMX晶体三个方向的热膨胀特性基本相同．三种晶型的体膨胀系数为8-HMX〉α-HMX〉β-HMX,表明δ-HMX晶体对温度最敏感,这可能是δ-HMX晶体具有更高感度的原因．在T=443K时,β-HMX晶体的晶胞参数突变,且部分分子构型由“椅式”转变为“船式-椅式”．采用两相热力学模型（2PT）得到的亥姆赫兹自由能表明,β—HMX晶体在T=423—443K时发生相变．β-,δ-和α-HMX晶体分别在T=303—423K,T=443—503K和T=363-423K内稳定存在．     

Theoretical insight into the influence of molecular ratio on the binding energy and mechanical property of HMX/2-picoline-N-oxide cocrystal,cooperativity effect and surface electrostatic potential

Molecular dynamics method was employed to study the binding energies and mechanical properties of the selected crystal planes of the energetic/nonenergetic 1,3,5,7-tetranitro-1,3,5,7-tetrazacyclooctane (HMX)/2-picoline-N-oxide cocrystal in different molecular ratios. The solvent effect in HMX:2-picoline-N-oxide (1:1) was calculated, and the cooperativity effect was discussed in HMX···HF/CH₄···2-picoline-N-oxide by using the M06-2X and MP2(full) methods at the 6-311++G^** basis set. The density, oxygen balance and detonation velocity were calculated. The results indicate that HMX/2-picoline-N-oxide prefers cocrystalising in the 1:1, 2:1 and 3:1 molar ratios, in which the cocrystals own the highest binding energy and best ductility. The cooperativity effect is present in the cyclic complex with CH₄, while the anti-cooperativity effect is found in the HF complex. Thus, in order to obtain stable HMX/2-picoline-N-oxide cocrystal, the solvent with low dielectric constant should be chosen, as is in accordance with the result from solvent effect. The reduced density gradient (RDG) and surface electrostatic potential analysis confirms the cooperativity effect and reveals the nature of decreased sensitivity in complex (or cocrystal). The cocrystals in the molar ratios of 5:1–10:1 could be satisfactory in view of explosive properties.     

Energy flow in thermostatted non-equilibrium molecular dynamics simulations

Energy transfers between internal kinetic and potential energy reservoirs in a simple liquid are studied by setting the temperature of one energy reservoir to a different value from that of the others and computing the resultant energy flows. In the first set of simulations, the x-directional kinetic temperature was artificially raised above the other five, and in the second, the x-directional configurational temperature was artificially raised above the other five. In both cases, external energy flows balanced, but unexpected energy flows between different directional components of the potential energy were observed. Additional simulations showed that these energy flows occurred regardless of the arrangement of thermostats imposed on the six degrees of freedom and the addition of shear. Heat flow between degrees of freedom that were ostensibly at the same temperature was anomalously observed. It was concluded that a different breakdown of the contributions to the configurational energy that is consistent with the definition of the directional configurational temperatures is required.     

Monte Carlo molecular dynamics simulations for two-dimensional magnets

A combined Monte Carlo molecular dynamics simulation technique is used to study thedynamic structure factor on a square lattice for isotropic Heisenberg and planar classical ferromagnetic spin Hamiltonians.     

Investigation of the structural and dynamic basis of kinesin dissociation from microtubule by atomistic molecular dynamics simulations

Kinesin is a molecular motor that can step processively on microtubules via the hydrolysis of ATP molecules. An important factor characterizing the processivity of the kinesin motor is its dissociation from the microtubule. Here, using all-atom molecular dynamics simulations, we studied the dissociation process of the kinesin head in weak-microtubule-binding or ADP state from tubulin on the basis of the available high-resolution structural data for the head and tubulin. By analyzing the simulated snapshots of the structure of the head-tubulin complex we provided detailed structural and dynamic information for the dissociation process. We found that the dissociation of the head along different directions relative to the tubulin exhibits very different dynamic behaviors. Moreover, the potential forms or energy landscapes of the interaction between the head and tubulin along different directions were determined. The studies have important implications for the detailed molecular mechanism of the dissociation of the kinesin motor and thus are critical to the mechanism of its processivity.     

氦热力学性质的分子动力学研究

 利用经典分子动力学和第一性原理分子动力学,研究了氦在高压下的熔化曲线、状态方程和非金属-金属转变。得到了氦在温度小于4.5 eV、 密度0.3~5.0 g/cm³范围内的状态方程,并把氦的熔化曲线的压强范围拓展到了50 GPa。氦的能隙宽度曲线表明,温度大大降低了氦的金属化密度。     

Influence of water on HFO-1234yf oxidation pyrolysis via ReaxFF molecular dynamics simulation

ABSTRACT

The effect of water molecules on HFO-1234yf oxidation pyrolysis was investigated by ReaxFF-molecular dynamics simulation from 1900 to 4200?K. The initial pyrolysis of HFO-1234yf starts around 2500?K and the water molecules participate in chemical reactions at 2800?K when the reactants pyrolysis reached the highest reaction rate. The primary products including HF, COF₂ and CO₂ are observed at 2600, 2700 and 2900?K, respectively. The influence of water molecules on products is mainly reflected in the promotion activity on the conversion from COF₂ to CO₂ and the generation of HF molecules. Four formation pathways are observed and calculated to further elucidate the procedure of pyrolysis. The main conversion process from H₂O to HF is the ?F?+?H₂O?=?HF+?OH reaction, and the paths from H₂O to ?OH radical and COF₂ to ?CFO radical which are promoted by ?F and ?H radical, respectively, have relatively low energy barriers of 10.44 and 40.29?kJ/mol, and both reaction processes released HF molecules.