A Promising Strategy for Searching High Energy Density Materials Based on 2,4,5‐Trinitro‐Imidazole Functional Backbone

Abstract A series of high energy density compounds are designed by altering the triazole, tetrazine, oxadiazole rings and energetic groups (such as −CN, −N 3 , −NH 2 , −NHNH 2 , −NO 2 , −NHNO 2 , −C(NO 2 ) 3 , −CH(NO 2 ) 2 ) into 2,4,5‐trinitro‐imidazole skeleton. Their structures are optimized by density functional theory (DFT) methods at B3LYP/6‐311G (d,p) method. Based on the optimized structures, the impact of different rings and energetic groups on their energy gaps, heats of formation, detonation performance and sensitivities are investigated. The results show that compound F4 possesses the highest values of heats of formation due to their high nitrogen content. However, compound F2 possesses the highest values of detonation pressure and detonation velocity which indicates that the detonation performance are determined by values of density rather than those of heats of formation. Taking both detonation performance and impact sensitivities into consideration, compounds B4, C4, F4, I4, J4 and J8 are screened as high energy density compounds due to their excellent detonation performance and acceptable sensitivities compared to those of RDX. Finally, the distribution of frontier molecular orbital, the electrostatic potential area distribution, thermodynamic properties and weak interactions of the screened compounds are fully investigated.