Predictions on High-Power Trivalent Metal Pentazolate Salts

High-energy-density materials (HEDMs) have been intensively studied for their significance in fundamental sciences and practical applications. Here, using the molecular crystal structure search method based on first-principles calculations, we have predicted a series of metastable energetic trivalent metal pentazolate salts MN₁₅ (M= Al, Ga, Sc, and Y). These compounds have high energy densities, with the highest nitrogen content among the studied nitrides so far. Pentazolate N₅^- molecules stack up face-to-face and form wave-like patterns in the C222₁ and Cc symmetries. The strong covalent bonding and very weak noncovalent interactions with nonbonded overlaps coexist in these ionic-like structures. We find MN₁₅ molecular structures are mechanically stable up to high temperature (∼1000 K) and ambient pressure. More importantly, these trivalent metal pentazolate salts have high detonation pressure (∼80 GPa) and velocity (∼12 km/s). Their detonation pressures exceeding that of TNT and HMX make them good candidates for high-brisance green energetic materials.