摘要
运用从头算分子动力学(AIMD)方法对均四嗪分子的热分解轨迹进行了模拟,用密度泛涵理论在B3LYP/6-311G(d,p)水平下计算了极小点和过渡态的几何结构和能量性质。然后在多种理论水平下(包括B3LYP/6-311+G(2df,2p)、G3MP2B3、G3B3、CCSD(T)/6-311G(d,p)、CCSD(T)/6-311+G(2df,2p))计算了反应物、产物和过渡态的单点能,并运用微正则变分过渡态理论(μVT)计算了均四嗪的热分解反应速率常数,得到较为准确可靠的反应信息。研究结果表明:均四嗪分子的热分解机理为协同的三键断裂,生成1个N2和2个HCN,此机理与均四嗪的光分解机理一致。
By combining the ab initio molecular dynamics （AIMD） method and density functional theory （DFT）, the thermal decomposition mechanism of s-tetrazine was studied. The dissociation channel was first simulated in a number of trajectories using the VASP package based on ab initio MD method, then further examined by Ganssian 98 at the B3LYP/6-311G（d,p） level to locate the minimum points and the transition structure. The high accuracy single point calculations were performed by B3LYP/6-311 ＋G（2df,2p）, G3MP2B3, G3B3, CCSD（T）/6-311G（d,p）, CCSD（T）/6-311 ＋G（2df,2p） and the rate constants were calculated by the microcanonical variational transition state theory （pNT）. The studies suggest that s-tetrazine undergo concerted triple dissociation to form one N2 and two HCN.
出处
《含能材料》
EI
CAS
CSCD
2006年第6期421-424,共4页
Chinese Journal of Energetic Materials
基金
国家自然科学基金-中物院NSAF联合基金(No.10576030)
