“…Energetic materials (EMs) are one of the most important components of organics with an irreplaceable role in solid propellants, which possess special properties of energy storage and stability. − However, the currently used EMs, such as hexanitrohexaazaisowurtzitane (CL-20), 1,3,5-triamino-2,4,6-trinitrobenzene (TATB), and 1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX), have some limitations due to their high sensitivity or relatively low catalytic activity. Therefore, it is challenging to design and synthesize EMs with high catalytic activity, high heat of detonation, low sensitivities, and environmental acceptability. − Recently, nitrogen-rich organic materials have attracted immense attention because they produce eco-friendly N 2 gas and release enormous energy during the process of decomposition. − Nevertheless, the conflict of high energy and oxygen balance cannot be resolved completely. The valid strategy is to construct stable ligands containing poly-nitrogen and oxygen-rich fragments. , 3-Amino-1,2,4-triazole-5-carboxylic acid (Hatzc) is one of the high energetic ligands, which possesses a high nitrogen content (N % = 43.8) and possesses high enthalpy of formation from the powerful energy release of C–N, N–N, and NN bonds. , What is more, Hatzc also presents O atoms from carboxylic groups, which can provide a sufficient oxygen content during the explosion …”