Anionic N 18 Macrocycles and a Polynitrogen Double Helix in Novel Yttrium Polynitrides YN 6 and Y 2 N 11 at 100 GPa
Anionic N 18 Macrocycles and a Polynitrogen Double Helix in Novel Yttrium Polynitrides YN 6 and Y 2 N 11 at 100 GPa
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100 GPa 下新型聚氮化钇 YN 6 和 Y 2 N 11 中的阴离子 N 18 大环化合物和多氮双螺旋
DOI：
10.1002/ange.202207469
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发表时间：
2022
影响因子：
--
通讯作者：
Aslandukov A
中科院分区：
文献类型：
--
作者：
Aslandukov A
在100 GPa和3000 K的激光加热金刚石对顶砧装置中，通过钇和氮的直接反应合成了两种新型的钇氮化物YN 6和Y2 N11。 高压同步辐射单晶X射线衍射显示，YN 6和Y2 N11的晶体结构具有独特的氮原子组织-以前未知的阴离子N18大环和多氮双螺旋。密度泛函理论计算证实了YN 6和Y2 N11化合物的动力学稳定性，显示出阴离子驱动的金属性，解释了多氮单元中不寻常的键级。由于Y2 N11中多氮双螺旋的电荷状态与以前在Hf 2N 11中发现的不同，并且由于N18大环从未被预测或观察到，它们的发现显着扩展了多氮化物的化学性质。
Two novel yttrium nitrides, YN6and Y2N11, were synthesized by direct reaction between yttrium and nitrogen at 100 GPa and 3000 K in a laser‐heated diamond anvil cell. High‐pressure synchrotron single‐crystal X‐ray diffraction revealed that the crystal structures of YN6and Y2N11feature a unique organization of nitrogen atoms—a previously unknown anionic N18macrocycle and a polynitrogen double helix, respectively. Density functional theory calculations, confirming the dynamical stability of the YN6and Y2N11compounds, show an anion‐driven metallicity, explaining the unusual bond orders in the polynitrogen units. As the charge state of the polynitrogen double helix in Y2N11is different from that previously found in Hf2N11and because N18macrocycles have never been predicted or observed, their discovery significantly extends the chemistry of polynitrides.