Impact of the Alkali Metal on the Structural and Dynamic Properties of the Anionic Pentahydride Ruthenium Complexes [M(THF)x][RuH5(PCy3)2] (M = Li, Na, K),Organometallics

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Impact of the Alkali Metal on the Structural and Dynamic Properties of the Anionic Pentahydride Ruthenium Complexes [M(THF)x][RuH5(PCy3)2] (M = Li, Na, K)
Organometallics ( IF 2.5 ) Pub Date : 2021-08-27 , DOI: 10.1021/acs.organomet.1c00384
Ramaraj Ayyappan ₁ , Koushik Saha _{1,

2} , Mary Grellier ₁ , Eric Clot ₃ , Laure Vendier ₁ , Sundargopal Ghosh ₂ , Sylviane Sabo-Etienne ₁ , Sébastien Bontemps ₁

Affiliation

A series of anionic ruthenium pentahydride complexes with the general formula [M(THF)_x][RuH₅(PCy₃)₂] (M = Li, Na, K) were synthesized. Their characterization by multinuclear NMR, IR, X-ray diffraction, and DFT techniques show that these complexes can adopt different structural features (monomer/dimer, cis/trans phosphines, hydride/dihydrogen ligands) depending on the countercation, the solvent, and/or the temperature. While the X-ray diffraction analyses offer snapshots of three out of five isomeric structures found by DFT, the solution and solid-state NMR analysis proved that these complexes exhibit a highly dynamic behavior. Rapid H–D exchange was found between Ru–H and D₂, which was attributed to the presence of Ru–H·····M interactions in the absence of crown-ether.

中文翻译：

碱金属对阴离子五氢化钌配合物 [M(THF)x][RuH5(PCy3)2] (M = Li, Na, K) 的结构和动态性能的影响

合成了一系列具有通式[M(THF) _x ][RuH ₅ (PCy ₃ ) ₂ ] (M = Li, Na, K)的阴离子五氢化钌配合物。它们通过多核 NMR、IR、X 射线衍射和 DFT 技术的表征表明，这些配合物可以采用不同的结构特征（单体/二聚体、顺式/反式膦、氢化物/二氢配体），具体取决于抗衡阳离子、溶剂和/或温度。虽然 X 射线衍射分析提供了 DFT 发现的五分之三的异构结构的快照，但溶液和固态核磁共振分析证明这些配合物表现出高度动态的行为。在 Ru-H 和 D ₂之间发现了快速的 H-D 交换, 这归因于在没有冠醚的情况下存在 Ru-H·····M 相互作用。

更新日期：2021-09-13

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