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首页> 外文期刊>Journal of Alloys and Compounds: An Interdisciplinary Journal of Materials Science and Solid-state Chemistry and Physics >New alkali metal osmium- and ruthenium hydrides
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New alkali metal osmium- and ruthenium hydrides

机译：新型碱金属和钌氢化物

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摘要

Previously unknown ternary metal hydrides A_xOsH_z and A_xRuH_z (A = alkali metal) were synthesized by the reaction of alkali metal hydrides with osmium or ruthenium under a hydrogen pressure up to 6000 bar. The crystal structures of the hydrides were determined using a combination of X-ray and neutron diffraction experiments with deuterated compounds on powdered samples. Na_3OsH_7 and Na_3RuH_7 crystallize at room temperature in a tetragonal structure type (space group: P4_2/mnm), which is characterized by isolated (OsH_7)- or (RuH_7) anions. The coordination polyhedron formed by the seven hydrogen (deuterium) ligands can be described as a distorted pentagonal bipyramide. Magnetic susceptibility measurements on Na_3OsH_7 in the temperature range between 3.5 K and room temperature revealed a weak temperature independent paramagnetism. Quantum mechanical calculations confirm these facts and show in detail that the large value of the spin-orbit coupling constant is responsible for the magnetic behaviour of these compounds with the oxidation state +4 for the transition metal atoms. With the heavier alkali metals transition metal(IV) hydrides A_(3- #delta#)OsH_(7- #delta#) and A_(3- #delta#)RuH_(7- #delta#) could be synthesized. They crystallize with isotypic atomic arrangements related to the cryolite structure type. Highest hydrogen pressure during the reaction leads to the osmium(VI) hydrides Cs_3OsH_9 and Rb_3OsH_9. The atomic arrangement is characterized by (OsH_8) polyhedra intercalated in a cubic HA_3 framework which corresponds to the ReO_3 structure type. Within these polyhedra the hydrogen ligands occupy two 24-fold positions with a statistical distribution.
机译：先前未知的三元金属氢化物A_xOsH_z和A_xRuH_z（A =碱金属）是通过使碱金属氢化物与或钌在高达6000 bar的氢气压力下反应而合成的。使用X射线和中子衍射实验结合粉末样品上的氘代化合物确定氢化物的晶体结构。 Na_3OsH_7和Na_3RuH_7在室温下以四方结构类型（空间群：P4_2 / mnm）结晶，其特征在于分离的（OsH_7）-或（RuH_7）阴离子。由七个氢（氘）配体形成的配位多面体可以描述为扭曲的五边形双吡amide酰胺。在3.5 K和室温之间的温度范围内，对Na_3OsH_7的磁化率测量显示弱的温度独立顺磁性。量子力学计算证实了这些事实，并详细表明，自旋轨道耦合常数的较大值决定了这些化合物的过渡金属原子的氧化态为+4的磁性行为。用较重的碱金属过渡金属（IV）氢化物，可以合成A_（3-＃δ＃）OsH_（7-δ＃）和A_（3-＃δ＃）RuH_（7-δ＃）。它们以与冰晶石结构类型有关的同型原子排列结晶。反应期间的最高氢气压力会导致氢化（VI）Cs_3OsH_9和Rb_3OsH_9。原子排列的特征是（OsH_8）多面体插入与ReO_3结构类型相对应的立方HA_3框架中。在这些多面体中，氢配体以统计分布占据两个24-位。

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