诱导期法研究过饱和度对LLM-105成核的影响  

Effect of Supersaturation on Nucleation of LLM⁃105 Based on Induction Period Measurement Method

作　　者：单军辉 周小清[2] 李洪珍[2] 刘天生 SHAN Jun-hui;ZHOU Xiao-qing;LI Hong-zhen;LIU Tian-sheng(School of Environment and Safety Engineering,North University of China,Taiyuan 030051,China;Institute of Chemical Materials,China Academy of Engineering Physics,Mianyang 621999,China)

机构地区：[1]中北大学环境与安全工程学院,山西太原030051 [2]中国工程物理研究院化工材料研究所,四川绵阳621999

出　　处：《含能材料》2020年第9期841-847,I0005,共8页Chinese Journal of Energetic Materials

基　　金：国家自然科学基金资助(11672273)。

摘　　要：为了研究2,6-二氨基-3,5-二硝基吡嗪-1-氧化物(LLM-105)的结晶成核过程,利用CrystlScan多通道结晶仪测量了不同过饱和度比下LLM-105反溶剂结晶成核诱导期。采用诱导期测量法研究了过饱和度对LLM-105成核的影响并结合经典成核理论计算了成核的重要参数。结果表明,LLM-105反溶剂结晶的诱导期随过饱和度的增大而降低。当过饱和度比S<2.53时,主要发生异相成核,界面张力γ值为6.67717×10^-23 J·m^-2,表面熵因子f值为1.49;当S>2.53时,主要发生均相成核,界面张力γ值9.98942×10^-23 J·m^-2表面熵因子f值为2.23。表面熵因子值均小于3,表明LLM-105在乙酸乙酯为反溶剂结晶中的生长方式为连续生长机制。另外,当LLM-105反溶剂结晶为发生均相成核时,成核速率随着过饱和比的增加而增加,临界晶核半径和临界成核数量均随着过饱和比的增加而减小。In order to study the crystal nucleation process of 2,6-diamino-3,5-dinitropyrazine-1-oxide(LLM-105),the CrystlScan multi-channel crystallizer was used to measure the crystallization nucleation induction period of LLM-105 in antisolvent system.The influence of supersaturation on the nucleation of LLM-105 was studied by using the induction period measurement method,and the important nucleation parameters were calculated by the classic nucleation theory.The results show that the induction period of anti-solvent crystallization of LLM-105 decreases with increasing supersaturation.When the supersaturation ratio S<2.53,heterogeneous nucleation was mainly observed,the interfacial tensionγvalue is 6.67717×10^-23 J·m^-2,and the surface entropy factor f value is 1.49;when S>2.53,the homogeneous nucleation was mainly achieved,the interfacial tensionγvalue is 9.89842×10^-23 J·m^-2 and the surface entropy factor f value is 2.23.The surface entropy factor values were all less than 3,indicating that the growth mode of LLM-105 in ethyl acetate as an anti-solvent crystal is a continuous growth mechanism,the nucleation rate increases as the supersaturation ratio increases,and the critical nucleus radius and the number of critical nucleation decrease as the supersaturation ratio increases.

关 键 词：2 6-二氨基-3 5-二硝基吡嗪-1-氧化物(LLM-105) 反溶剂结晶 诱导期 过饱和度 成核 

分 类 号：TJ55[兵器科学与技术—军事化学与烟火技术] O64[理学—物理化学]