Abstract
High-energy density materials (HEDMs) demand innovative molecular strategies for achieving optimized detonation performance, stability, and insensitivity. Now we present an isomer-driven design of two advanced energetic frameworks: high-energy compound 5, 5-(3,4-dinitro-1H-pyrazol-5-yl)-3-(trinitromethyl)-1H-1,2,4-triazole and zwitterionic compound 11, N-(5-(5-amino-1,3,4-oxadiazol-2-yl)-4-nitro-1H-pyrazol-3-yl)nitramide (11). Compound 5 has an impressive density of 1.926 g/cm³, high detonation velocity of 9206 m/s, outperforming RDX with an acceptable thermal stability of 163.9 oC. Compound 11 has an excellent density of 1.918 g/cm³, an RDX-like detonation velocity of 8797 m/s, exceptional high thermal stability of 242.7 °C, and is insensitive to external stimuli. The outstanding properties of 11 are attributed to its zwitterionic nature, as confirmed by crystal structure analysis, NCI interactions, ESP and aromaticity studies. These findings highlight a paradigm for leveraging positional isomerism and zwitterionic architectures to advance the design of HEDMs with superior performance and stability.