Syntheses, structures, properties, and calculation of a family of ionic crystals based on 1,3‐bis(5‐tetrazolyl)triazene

Sodium salt of 1,3‐bis(5‐tetrazolyl)triazene (NaH 2 BTT ⋅ 4H 2 O) was obtained through diazo‐couple reaction with 5‐aminotetrazole as starting reactants, and a family of energetic ionic crystals of the 1,3‐bis(5‐tetrazolyl)triazene anions H n BTT (3−n)− with different cations were investigated, including protonated amines (ethanediamine, hydrazinium, aminoguanidine, methylhydrazinium) and Y(H 2 O) 8 3+ . The structures and physicochemical properties of these compounds were characterized by IR, Raman, X‐ray diffraction (XRPD) and TG‐DSC. Ethanediamine salt is the best thermal stable, while hydrazinium salt possesses a highest nitrogen rich value of 79.76 %. Both of them show a rapid collapse of the BTT main frame, and almost all of the dissociation products are released in the form of gas.