基于反应力场(reactive force field,ReaxFF)的反应分子动力学模拟的结果分析具有挑战性。国际首个ReaxFF MD化学反应分析及可视化工具VARxMD(visulization and analysis of ReaxFF molecular dynamics)可自动生成不同时刻之间完整的化...基于反应力场(reactive force field,ReaxFF)的反应分子动力学模拟的结果分析具有挑战性。国际首个ReaxFF MD化学反应分析及可视化工具VARxMD(visulization and analysis of ReaxFF molecular dynamics)可自动生成不同时刻之间完整的化学反应列表,通过物种检索进一步对反应路径进行分类。但VARxMD目前的反应分析针对的是某一确定条件下单一的ReaxFF MD模拟轨迹,利用VARxMD分析获得一次模拟的完整反应列表需要消耗大量计算资源和时间。本文提出基于数据库来储存VARxMD反应分析结果数据,基于数据库检索进一步分析反应的思路,并采用MVVM(model-view-view model)的系统设计模式、结合渐进式框架Vue.js建立了ReaxFF MD模拟的化学反应数据系统ReaxMDDB(reaction database of ReaxFF MD simulation)。系统应用于多个RP-3模型热解和氧化模拟反应数据的结果表明:该系统不仅实现了多个ReaxFF MD模拟的详细反应的统一分析和化学反应的2D分子结构显示,而且可永久保存模拟获得的反应数据集以备后续进一步分析反应机理。ReaxMDDB具有很好的通用性,为认识不同反应模拟所揭示的共性化学反应机理提供了方便的平台。展开更多
Cyclotriphosphazene derivatives can effectively improve the flame retardancy and fire safety of epoxy resins(EPs)via their influence on the pyrolysis process.In this work,the effects of hexa(5-methyl-2-pyridinoxyl)cyc...Cyclotriphosphazene derivatives can effectively improve the flame retardancy and fire safety of epoxy resins(EPs)via their influence on the pyrolysis process.In this work,the effects of hexa(5-methyl-2-pyridinoxyl)cyclotriphosphazene(HMPOP)incorporation on the initial pyrolysis of an EP at 500–3500 K were studied using the ReaxFF method.The pyrolysis fragments,initial reaction pathways,and main products were identified for the EP and EP/HMPOP composites.The activation energies were derived by fitting the weight percentage curves for solid species during the pyrolysis reactions and the obtained values were in good agreement with experimental data.The initial EP pyrolysis reactions included four major decomposition modes,which primarily involved the cleavage of C–O and C–N bonds.The main pyrolysis products were H_(2)O,CO,C_(2)H_(4),and CH_(2)O.HMPOP bonded with the oxygen-containing fragments to form larger molecular fragments and reduced the amounts of C_(0)–C_(4) products,especially that of the harmful gas CH_(2)O.Thus,HMPOP promoted the formation of carbon clusters and reduced the generation of combustible gases,ultimately decreasing the capacity for fire propagation.展开更多
To obtain detailed information on the potential energy, the evolution of species, the initial reaction paths, and thermal decomposition products, we conducted simulations on pyrolysis process of CL20/BTF co-crystal us...To obtain detailed information on the potential energy, the evolution of species, the initial reaction paths, and thermal decomposition products, we conducted simulations on pyrolysis process of CL20/BTF co-crystal using the ReaxFF/lg reaction force field, with temperature set at 2000 K to 3000 K. With the analysis of evolution curves of potential energy based on exponential function, we obtain the overall characteristic time. Via a description of the total package reaction with classical Arrhenius law, we obtain the activation energy of CL20/BTF co-crystal： Ea=60.8 kcal/mol. Based on the initial path of CL20/BTF co-crystal thermal decomposition we studied, we conclude that N-NO2 bond of CL20 molecules breaks first, working as a dominant role in the initial stage of thermal decomposition under the condition of different temperatures, and that all CL20 molecules completely decompose before BTF molecular regardless of different temperatures. We also find that the main products of CL20/BTF co-crystal are NO2, NO, NO3, HNO, O2, N2, H2O, CO2, N2O, and HONO, etc., on which the temperature forms certain influence.展开更多
文摘基于反应力场(reactive force field,ReaxFF)的反应分子动力学模拟的结果分析具有挑战性。国际首个ReaxFF MD化学反应分析及可视化工具VARxMD(visulization and analysis of ReaxFF molecular dynamics)可自动生成不同时刻之间完整的化学反应列表,通过物种检索进一步对反应路径进行分类。但VARxMD目前的反应分析针对的是某一确定条件下单一的ReaxFF MD模拟轨迹,利用VARxMD分析获得一次模拟的完整反应列表需要消耗大量计算资源和时间。本文提出基于数据库来储存VARxMD反应分析结果数据,基于数据库检索进一步分析反应的思路,并采用MVVM(model-view-view model)的系统设计模式、结合渐进式框架Vue.js建立了ReaxFF MD模拟的化学反应数据系统ReaxMDDB(reaction database of ReaxFF MD simulation)。系统应用于多个RP-3模型热解和氧化模拟反应数据的结果表明:该系统不仅实现了多个ReaxFF MD模拟的详细反应的统一分析和化学反应的2D分子结构显示,而且可永久保存模拟获得的反应数据集以备后续进一步分析反应机理。ReaxMDDB具有很好的通用性,为认识不同反应模拟所揭示的共性化学反应机理提供了方便的平台。
基金the National Natural Science Foundation of China(51901209).
文摘Cyclotriphosphazene derivatives can effectively improve the flame retardancy and fire safety of epoxy resins(EPs)via their influence on the pyrolysis process.In this work,the effects of hexa(5-methyl-2-pyridinoxyl)cyclotriphosphazene(HMPOP)incorporation on the initial pyrolysis of an EP at 500–3500 K were studied using the ReaxFF method.The pyrolysis fragments,initial reaction pathways,and main products were identified for the EP and EP/HMPOP composites.The activation energies were derived by fitting the weight percentage curves for solid species during the pyrolysis reactions and the obtained values were in good agreement with experimental data.The initial EP pyrolysis reactions included four major decomposition modes,which primarily involved the cleavage of C–O and C–N bonds.The main pyrolysis products were H_(2)O,CO,C_(2)H_(4),and CH_(2)O.HMPOP bonded with the oxygen-containing fragments to form larger molecular fragments and reduced the amounts of C_(0)–C_(4) products,especially that of the harmful gas CH_(2)O.Thus,HMPOP promoted the formation of carbon clusters and reduced the generation of combustible gases,ultimately decreasing the capacity for fire propagation.
文摘To obtain detailed information on the potential energy, the evolution of species, the initial reaction paths, and thermal decomposition products, we conducted simulations on pyrolysis process of CL20/BTF co-crystal using the ReaxFF/lg reaction force field, with temperature set at 2000 K to 3000 K. With the analysis of evolution curves of potential energy based on exponential function, we obtain the overall characteristic time. Via a description of the total package reaction with classical Arrhenius law, we obtain the activation energy of CL20/BTF co-crystal： Ea=60.8 kcal/mol. Based on the initial path of CL20/BTF co-crystal thermal decomposition we studied, we conclude that N-NO2 bond of CL20 molecules breaks first, working as a dominant role in the initial stage of thermal decomposition under the condition of different temperatures, and that all CL20 molecules completely decompose before BTF molecular regardless of different temperatures. We also find that the main products of CL20/BTF co-crystal are NO2, NO, NO3, HNO, O2, N2, H2O, CO2, N2O, and HONO, etc., on which the temperature forms certain influence.
