Abstract
Bistetrazole-based compounds are novel high-nitrogen energetic molecules that have garnered attention in recent years. They possess a higher energy density and lower sensitivity, and are less challenging to synthesize than complex cage-like molecules. This study employed a molecular auto-generation mechanism to generate 35 322 bistetrazole-based molecules with 20 bridgeheads and 29 side substituents. A combination of quantum chemical calculations and machine learning models was used to sequentially screen the molecules based on their oxygen balance index, synthesis difficulty, density, and detonation pressure, thus rapidly narrowing the search scope. Three bistetrazole-based energetic molecules with high potential were identified. The theoretical enthalpy of the formation of the designed molecules was as high as 854.76 kJ mol(-1) and their detonation velocity reached 9.58 km s(-1). Further calculations also demonstrated that these molecules have better macroscopic stability than trinitrotoluene, making them promising candidates for practical applications in developing energetic materials.