Thermal decomposition and combustion performance of high-energy ammonium perchlorate-based molecular perovskite

The development of high-energy ammonium perchlorate (NH₄ClO₄, AP)-based energetic materials is of great significance for promoting their potential applications. In this study, AP-based molecular perovskite energetic materials (H₂dabco)[NH₄(ClO₄)₃] were prepared via molecular assembly strategy with the facile one-pot reaction of AP, HClO₄ and triethylenediamine (dabco). The as-obtained sample was characterized by X-ray diffraction (XRD) and Fourier transform infrared (FT-IR). The thermal decomposition and combustion performance was investigated by thermo-gravimetric/differential scanning calorimeter (TG-DSC), high speed photography and three-dimensional FT-IR. The results showed that combined with the oxidizer perchlorate and fuel dabco at the molecular level, ternary molecular perovskite (H₂dabco)[NH₄(ClO₄)₃] possessed a more stable thermal decomposition temperature (385.0 °C) than the monocomponent AP and the heat release is also as high as 3421 J g⁻¹. The thermal decomposition activation energy (181.070 kJ mol⁻¹) of thermal decomposition of (H₂dabco)[NH₄(ClO₄)₃] had been expectably reduced from the activation energy (200.259 kJ mol⁻¹) of high-temperature decomposition stage of AP, despite of low-temperature decomposition stage. The synergistic catalysis thermal decomposition mechanism based on the molecular perovskite structures was proposed. And the combustion performance demonstrated molecular perovskite (H₂dabco)[NH₄(ClO₄)₃] had a high energy-releasing efficiency. This work provides a proof-of-principle concept for the design and fabrication of high-performance solid propellants based on molecular perovskite (H₂dabco)[NH₄(ClO₄)₃].