New Efficient High-Energy Materials Based on 4,6-Dinitrobenzimidazol-2-One Core: Simulations of Properties

In this study, the impact of incorporating energetic substituents such as -NO₂, -NH₂, -NH₃, -N₂ (both with perchlorate anion), and -N₃ into 4,6-dinitrobenzimidazol-2-one on its detonation performance and stability was investigated. The DFT B3LYP/cc-pVTZ method was employed to evaluate key molecular properties: the HOMO–LUMO gap, cohesive energy, chemical hardness, and electronegativity. Based on these parameters, the resulting changes in chemical and thermal stability were assessed. The results achieved highlight the significant role of ionic bonding in enhancing both the stability and density of the compounds. Our results indicate that the benzimidazoles enriched by energetic groups possess energetic properties better than TNT, with some variants surpassing HMX. The analysis of the stability and sensitivity based on oxygen balance investigation suggests that by varying the incorporated substituents, it is possible to design both primary and secondary explosives from a common molecular scaffold.