高级搜索

您是今天第:5020位访问者

您是第:7243081位访问者

FOX-7团簇中分子间相互作用对其裂解影响的量子化学研究
Quantum Chemical Study on Effects of Intermolecular Interactions in FOX-7 Clusters on the Dissociation of FOX-7
  • 摘要
  •  
  • 参考文献
  •  
  • 引证文献
  •  
  • 相似文献
中文摘要:
      采用色散校正密度泛函理论的RI-B2PLYP-D3和PW6B95-D3方法得到了1,1-二氨基-2,2-二硝基乙烯(FOX-7)的四种气相团簇,以此模拟FOX-7分子在晶体结构中的存在状态。绘制了团簇形成过程中各分子相邻处的电子密度差图,从电子密度变化的角度解释了分子间相互作用的形成及来源,研究了凝聚相FOX-7分子间相互作用对FOX-7裂解机理的影响。结果表明,FOX-7团簇中分子间相互作用源于电子偏移形成的部分分子间共享电子,分子间相互作用形成的同时也使部分分子内的化学键被弱化,致使FOX-7的裂解通道发生改变。采用PW6B95-D3理论时,分子间相互作用使各团簇中FOX-7的C—NO2键裂解活化能比单分子状态时普遍降低。不同团簇中分子间相互作用力角度不同,硝基异构反应的过程有所变化,与单分子FOX-7相比, 团簇Ⅱ硝基异构通道的活化能下降了210.9 kJ·mol-1,而团簇Ⅳ硝基异构通道的活化能升高了39.4 kJ·mol-1
中文关键词: 1,1-二氨基-2,2-二硝基乙烯(FOX-7)  裂解  团簇  分子间相互作用  电子密度差
英文摘要:
      Four kinds of gas clusters of 1,1-diamino-2,2-dinitroethene (FOX-7) were obtained by using RI-B2PLYP-D3 and PW6B95-D3 methods with dispersion correction density functional theory. On this account, the existing state of FOX-7 molecules in the crystal structures was simulated. The electron density difference of the neighboring molecules in the process of cluster formation was plotted, and the formation and origin of intermolecular interactions were explained from the point of view of electron density change. The effect of intermolecular interaction of condensed phase FOX-7 on the dissociation mechanism of FOX-7 was investigated. Results show that the intermolecular interactions are due to the partial intermolecular sharing of electrons formed by electron offsets in the FOX-7 clusters. The formation of intermolecular interactions also weakens the chemical bonds in some molecules, resulting in a change in the cleavage channel of FOX-7. Compared with the unimolecule state, the intermolecular interaction makes the cleavage activation energy of C—NO2 bond in FOX-7 clusters reduce generally when PW6B95-D3 theory is used. Because of different angles of molecular interaction in different clusters, the process of nitro isomer has changed, compared with the unimolecule, the activation energy of nitro isomer channels of cluster Ⅱ decreases by 210.9 kJ·mol-1, and the activation energy of nitro nitro isomer channel of cluster Ⅳ increases by 39.4 kJ·mol-1.
英文关键词: 1,1-diamino-2,2-dinitroethene(FOX-7)  dissociation  clusters  intermolecular interaction  electron density differences
DOI:10.11943/j.issn.1006-9941.2018.03.003
投稿日期:2017-04-19
最后修改日期:2017-06-15
网络出版日期:2018-03-13
书版出版日期:2018-03-21
基金项目:武器装备预先研究项目(41419120201)
引用文献:李小东,徐哲,燕翔,刘磊,王恒,王晶禹,等.FOX-7团簇中分子间相互作用对其裂解影响的量子化学研究[J].含能材料,2018,26(3):218~222
作者单位E-mail
李小东 中北大学化工与环境学院, 山西 太原 030051 lixd78@126.com 
徐哲 中北大学化工与环境学院, 山西 太原 030051  
燕翔 中北大学化工与环境学院, 山西 太原 030051  
刘磊 中北大学化工与环境学院, 山西 太原 030051  
王恒 中北大学化工与环境学院, 山西 太原 030051  
王晶禹 中北大学化工与环境学院, 山西 太原 030051  
摘要点击次数: 691
全文下载次数: 416
HTML 查看全文   查看/发表评论   下载PDF阅读器

更多>>

更多>>

分享按钮