在定制离子化合物中通过电负性协同匹配创建 cyclo-N$_5$$^{+}$ 阳离子并组装 N$_5$$^{+}$N$_5$$^{-}$ 盐
Creating cyclo-N$_5$$^{+}$ cation and assembling N$_5$$^{+}$N$_5$$^{-}$ salt via electronegativity co-matching in tailored ionic compounds
AI总结：
该研究提出利用离子化合物中主体离子的电负性协同匹配来氧化/还原 cyclo-N$_5$ 物种，并通过计算结构搜索发现可在高压及环境条件下稳定的 XN$_5$N$_5$F。
摘要：
近期结晶态五唑盐的发现标志着多氮科学的一项重大进展，并提升了制备长期备受关注的高能推进剂 N$_5$$^{+}$N$_5$$^{-}$ 盐的前景。然而，尽管已在五唑盐中合成 cyclo-N$_5$$^{-}$ 阴离子，由于五唑离子具有强氧化能力，对应的反阳离子 cyclo-N$_5$$^{+}$ 仍难以获得；此外，已知纯 N$_5$$^{+}$N$_5$$^{-}$ 盐并不稳定。本文提出一种新策略，用于在定制离子化合物中制备稀有的 cyclo-N$_5$$^{+}$ 阳离子并组装长期寻求的 N$_5$$^{+}$N$_5$$^{-}$ 盐，其中负/正主体离子充当氧化/还原剂，以形成 cyclo-N$_5$$^{+}$/N$_5$$^{-}$ 物种。该策略通过先进的计算晶体结构搜索实施，识别出 XN$_5$N$_5$F（X = Li、Na、K）化合物；基于从头算分子动力学模拟，这些化合物在高压下稳定，并在常温常压条件下仍可保持可行。这一发现为在离子化合物中创建并稳定 N$_5$$^{+}$N$_5$$^{-}$ 盐组装体开辟了途径，其中 cyclo-N$_5$ 物种通过与高/低电负性主体离子的协同匹配而被氧化/还原。当前结果展示了新颖的多氮化学，这些发现也为设计和合成多种具有异常电荷态、成键结构和优异功能的化学物种提供了新的见解与前景。
英文摘要：
The recent discovery of crystalline pentazolates marks a major advance in polynitrogen science and raises prospects of making the long-touted potent propellant N$_5$$^{+}$N$_5$$^{-}$ salt. However, despite the synthesis of cyclo-N$_5$$^{-}$ anion in pentazolates, counter cation cyclo-N$_5$$^{+}$ remains elusive due to the strong oxidizing power of pentazole ion; moreover, pure N$_5$$^{+}$N$_5$$^{-}$ salt is known to be unstable. Here, we devise a new strategy for making rare cyclo-N$_5$$^{+}$ cation and assembling the long-sought N$_5$$^{+}$N$_5$$^{-}$ salt in tailored ionic compounds, wherein the negative/positive host ions act as oxidizing/reducing agents to form cyclo-N$_5$$^{+}$/N$_5$$^{-}$ species. This strategy is implemented via an advanced computational crystal structure search, which identifies XN$_5$N$_5$F (X = Li, Na, K) compounds that stabilize at high pressures and remain viable at ambient pressure-temperature conditions based on \textit{ab initio} molecular dynamics simulations. This finding opens an avenue for creating and stabilizing N$_5$$^{+}$N$_5$$^{-}$ salt assembly in ionic compounds, where cyclo-N$_5$ species are oxidized/reduced via co-matching with host ions of high/low electronegativity. The present results demonstrate novel polynitrogen chemistry, and these findings offer new insights and prospects in the design and synthesis of diverse chemical species that exhibit unusual charge states, bonding structures, and superior functionality.
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