Construction of an Unusual Two-Dimensional Layered Structure for Fused-Ring Energetic Materials with High Energy and Good Stability

The creation of high-performance energetic materials with good mechanical sensitivities has been a great challenge over the past decades, since such materials have huge amounts of energy and are thus essentially unstable. Here, we report on a promising fused-ring energetic material with an unusual two-dimensional (2D) structure, 4-nitro-7-azido-pyrazol-[3,4-d]-1,2,3-triazine-2-oxide (NAPTO), whose unique 2D structure has been confirmed by single-crystal X-ray diffraction. Experimental studies show that this novel energetic compound has remarkably high energy (detonation velocity D = 9.12 km·s⁻¹; detonation pressure P = 35.1 GPa), excellent sensitivities toward external stimuli (impact sensitivity IS = 18 J; friction sensitivity FS = 325 N; electrostatic discharge sensitivity EDS = 0.32 J) and a high thermal decomposition temperature (203.2 °C), thus possessing the dual advantages of high energy and low mechanical sensitivities. To our knowledge, NAPTO is the first fused-ring energetic material with 2D layered crystal stacking. The stabilization mechanism toward external stimuli were investigated using molecular simulations, and the theoretical calculation results demonstrate that the ultraflat 2D layered structure can buffer external mechanical stimuli more effectively than other structures by converting the mechanical energy acting on the material into layer sliding and compression. Our study reveals the great promise of the fused-ring 2D layered structure for creating advanced energetic materials.