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描绘抗衡离子对U(IV) 林德奎斯特多金属氧酸盐配合物的结构和振动性质的影响。

Delineating the Effects of Counterions on the Structural and Vibrational Properties of U(IV) Lindqvist Polyoxometalate Complexes.

作者信息

Subintoro Primadi J, Carter Korey P

机构信息

Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States.

出版信息

Inorg Chem. 2025 Jun 16;64(23):11380-11397. doi: 10.1021/acs.inorgchem.5c00033. Epub 2025 May 30.

DOI:10.1021/acs.inorgchem.5c00033
PMID:40445109
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12175120/
Abstract

Herein we conducted a full investigation into the fundamental structural and vibrational properties of uranium(IV) Peacock-Weakley-type lacunary Lindqvist (W) polyoxometalate (POM) complexes. We recently demonstrated the importance of the secondary lattice elements in tuning the distortion of the D symmetry in W POM complexes, and here, we synthesized eight UW complexes with different alkali metal counterions and evaluated how the composition and packing of counterion species affected complex structural and vibrational properties. Single-crystal X-ray diffraction analysis on complexes revealed changes in structural distortion parameters as a function of differences in counterion configurations, while far-infrared and Raman spectra for - also demonstrated that vibrational mode frequencies were sensitive to changes in counterion composition and packing. To more effectively compare different counterion configurations, we developed counterion effective ionic radius (eIR) as a new structural parameter, and comparisons between structural distortion parameters and eIR values strongly suggested that modulation by the secondary lattice elements can affect structural and vibrational manifolds within POM complexes. Partial least squares (PLS) analysis was used to quantitatively evaluate correlations observed within this investigation, and PLS statistical models showed a strong correlation between counterion eIR and both structural distortion parameters and vibrational mode frequencies.

摘要

在此，我们对铀(IV)孔雀石-韦克利型缺位林德奎斯特(W)多金属氧酸盐(POM)配合物的基本结构和振动性质进行了全面研究。我们最近证明了二级晶格元素在调节W POM配合物中D对称性畸变方面的重要性，在此，我们合成了八种具有不同碱金属抗衡离子的UW配合物，并评估了抗衡离子物种的组成和堆积如何影响配合物的结构和振动性质。对配合物进行的单晶X射线衍射分析揭示了结构畸变参数随抗衡离子构型差异的变化，而对配合物的远红外和拉曼光谱也表明振动模式频率对抗衡离子组成和堆积的变化敏感。为了更有效地比较不同的抗衡离子构型，我们开发了抗衡离子有效离子半径(eIR)作为一个新的结构参数，结构畸变参数与eIR值之间的比较强烈表明，二级晶格元素的调制可以影响POM配合物中的结构和振动流形。使用偏最小二乘法(PLS)分析来定量评估本研究中观察到的相关性，PLS统计模型表明抗衡离子eIR与结构畸变参数和振动模式频率之间存在很强的相关性。

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本文引用的文献

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