The search for high energy density materials (HEDMs) in polymeric nitrogen compounds has gained considerable attention. Previous theoretical predictions and experiments have revealed that metal ions can be used to stabilize the pentazolate (N ⁻₅ ) anion. In this work, by employing a machine learning-accelerated crystal structure searching method and first-principles calculations, we found that the new pentazolate salts, CaN₁₀ and BaN₁₀, are energetically favorable at high pressures. Phonon dispersion calculations reveal that they are quenchable at ambient pressure. Ab initio molecular dynamics simulations verify their dynamic stability at finite temperature. Bader charge and electron localization function illustrates that alkaline earth atoms serve as electron donors, contributing to the stability of N₅ rings. Bonding calculations reveal covalent bonds between nitrogen atoms and weak interactions between N₅ rings. Similar to other pentazolate salts, these polymeric nitrides have high energy densities of approximately 2.35 kJ/g for CaN₁₀ and 1.32 kJ/g for BaN₁₀. The predictions of CaN₁₀ and BaN₁₀ structures indicate that these salts are potential candidates for green nitrogen-rich HEDMs.

在聚合氮化合物中寻找高能量密度材料（HEDMs）已引起广泛关注。先前的理论预测和实验表明，金属离子可用于稳定戊唑酸酯（N ^- ₅）阴离子。在这项工作中，通过采用机器学习加速的晶体结构搜索方法和第一性原理计算，我们发现，在高压下，新型五唑盐CaN ₁₀和BaN ₁₀在能量上是有利的。声子色散计算表明，它们在环境压力下可淬灭。从头算 分子动力学仿真证明了它们在有限温度下的动态稳定性。较差的电荷和电子定位功能说明碱土原子充当电子供体，有助于N ₅环的稳定性。结合计算揭示了氮原子之间的共价键和N ₅环之间的弱相互作用。与其他五唑盐类似，这些聚合氮化物的高能量密度，对于CaN ₁₀为约2.35 kJ / g，对于BaN ₁₀为1.32 kJ / g 。CaN ₁₀和BaN ₁₀结构的预测表明，这些盐是富含绿色氮的HEDM的潜在候选物。