The present research aims to select the optimal molar ratio of hydrazine 3-nitro-1,2,4-triazol-5-one (HNTO) and ammonium nitrate (AN) to produce an energetic co-crystal. For a comparison purpose, the heat release, cost, density and hygroscopicity of the different co-crystals were evaluated. The obtained results indicated that HNTO/AN at the 1 : 3 ratio exhibited a higher heat release, better thermal stability, low water content and a reasonable cost, compared to other co-crystals. This new co-crystal was fully characterized through powder X-ray diffraction (XRD), infrared spectroscopy (FTIR) and differential scanning calorimetry (DSC), confirming that this latter displayed similar characteristics to those of the co-crystal with a 1 : 1 ratio, which was recently developed. On the other hand, the catalytic activity of two energetic coordination polymers of triaminoguanidine-cobalt (T-Co) complexes, with or without graphene oxide (GO-T-Co-T), on the thermolysis of the developed co-crystal has been also assessed by DSC under non-isothermal conditions. It is revealed that these catalysts have greatly decreased the decomposition temperature of the HNTO/AN cocrystal. Moreover, because of the complete decomposition in the case of the (HNTO/AN)/GO-T-Co-T composite, the heat release has been increased as well. Isoconversional integral kinetic methods were exploited to determine the kinetic parameters of the different systems. According to the obtained results, these catalysts have a strong catalytic action on the decomposition of the co-crystal AN/HNTO for which the activation energy and the pre-exponential factor are considerably lowered. Consequently, the developed co-crystal and the energetic catalysts could be considered as potential ingredients for the next generation of composite solid propellant formulations.
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