A C–N Coupling-BasedMolecular Assembly Strategyfor Synergistically Enhancing Energy and Safety in Energetic Materials

Abstract The pursuit of energetic materials (EMs) that concurrently deliver high energy density and low sensitivity is a longstanding goal. This study presents an efficient modular assembly strategy based on C–N coupling to address this challenge. Using 5-amino-3-nitro-1,2,4-triazole (ANTA) as a key building block, its coupling with various chloroazaarenes afforded three novel tricyclic EMs (LSH-1, LSH-2, LSH-3). Impressively, all compounds showcase a superior combination of properties: high thermal stability (Td up to 350 °C), outstanding detonation performance (Dv: 8329–8897 m·s–1), and notably low mechanical sensitivity (IS > 30 J, FS > 360 N). The structure–property relationships, further rationalized by quantum chemical calculations, highlight how extended conjugation and hydrogen-bonding networks contribute to these balanced characteristics. Our findings underscore the C–N coupling strategy as a powerful and promising approach for designing advanced EMs with an optimal energy–safety profile.