化工学报 ›› 2022, Vol. 73 ›› Issue (8): 3511-3517.DOI: 10.11949/0438-1157.20220262

• 热力学 • 上一篇    下一篇

基体(TDI-TMP-T313)与氧化剂(AP)相互作用的第一性原理研究

俞夏琪1(), 冯格1, 赵金燕1, 李嘉远1, 邓声威1, 郑靖楠1, 李雯雯1, 王亚秋1, 沈榄1, 刘旭1, 徐威威1, 王建国1, 王式彬1, 姚子豪1(), 毛成立2()   

  1. 1.浙江工业大学化学工程学院,浙江 杭州 310014
    2.上海新力动力设备研究所,上海 201100
  • 收稿日期:2022-03-01 修回日期:2022-04-26 出版日期:2022-08-05 发布日期:2022-09-06
  • 通讯作者: 姚子豪,毛成立
  • 作者简介:俞夏琪(1997—),女,硕士研究生,yuxq4561@163.com

A first-principles study of the interaction between TDI-TMP-T313 and AP

Xiaqi YU1(), Ge FENG1, Jinyan ZHAO1, Jiayuan LI1, Shengwei DENG1, Jingnan ZHENG1, Wenwen LI1, Yaqiu WANG1, Lan SHEN1, Xu LIU1, Weiwei XU1, Jianguo WANG1, Shibin WANG1, Zihao YAO1(), Chengli MAO2()   

  1. 1.College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China
    2.Shanghai Xinli Power Equipment Research Institute, Shanghai 201100, China
  • Received:2022-03-01 Revised:2022-04-26 Online:2022-08-05 Published:2022-09-06
  • Contact: Zihao YAO, Chengli MAO

摘要:

采用密度泛函理论(DFT)研究了氧化剂高氯酸铵(001)、(210)、(011)、(201)四种晶面的表面能并对其进行从头算分子动力学(AIMD)模拟,测试其稳定性。基体组分甲苯二异氰酸酯(TDI)、三羟基甲基丙烷(TMP)、三氟化硼三乙醇胺络合物(T313)在氧化剂晶面的吸附能同样由DFT进行计算。针对基体和氧化剂之间的相互作用进行了化学理论分析,最后选取吸附物和晶面相互作用最强的T313-AP(201)体系,模拟其分子电子结构并观察原子间的电荷转移情况。通过多种理论方法在分子尺度上揭示键合剂(T313)与氧化剂(AP)的作用机制,证实老化过程中产生的关键产物来源。

关键词: 基体, 氧化剂, 键合剂, 叠氮推进剂, 密度泛函理论, 燃料, 计算化学, 表面

Abstract:

Density functional theory (DFT) is used to study the surface energies of four crystal planes of oxidant-ammonium perchlorate (001), (210), (011), (201), and the surfaces' stability is tested by ab initio molecular dynamics (AIMD) simulation. The adsorption energies of the matrix components-toluene diisocyanate (TDI), trihydroxymethyl propane (TMP) and boron trifluoride tritylamine complex (T313) on the crystal planes of oxidizing agent are also calculated by DFT. The interaction between matrix and oxidizing agent is analyzed theoretically. Eventually, the T313-AP (201) system with the strongest interaction between adsorbent and crystal plane is selected for bader charge analysis to simulate its molecular electronic structure and observe the charge transfer between atoms. The mechanism of interaction between bonding agent (T313) and oxidizing agent (AP) is revealed on a molecular scale by various theoretical methods. The sources of critical products produced in the ageing process are confirmed.

Key words: matrix, oxidizing agent, bonding agent, azide propellant, density functional theory, fuel, computational chemistry, surface

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