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首页> 外文期刊>Chemistry: A European journal >Extending the Row of Lanthanide Tetrafluorides: A Combined Matrix-Isolation and Quantum-Chemical Study
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Extending the Row of Lanthanide Tetrafluorides: A Combined Matrix-Isolation and Quantum-Chemical Study

机译：扩大镧系四氟化物的行：组合的基质分离和量子化学研究

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摘要

Only the neutral tetrafluorides of Ce, Pr, and Tb as well as the [LnF(7)](3-) anions of Dy and Nd, with the metal in the +IV oxidation state, have been previously reported. We report our attempts to extend the row of neutral lanthanide tetrafluorides through the reaction of laser-ablated metal atoms with fluorine and their stabilization and characterization by matrix-isolation IR spectroscopy. In addition to the above three tetrafluorides, we found two new tetrafluorides, (NdF4)-Nd-3 and (DyF4)-Dy-7, both of which are in the +IV oxidation state, which extends this lanthanide oxidation state to two new metals. Our experimental results are supported by quantum-chemical calculations and the role of the lanthanide oxidation state is discussed for both the LnF(4) and [LnF(4)](-) species. Most of the LnF(4) species are predicted to be in the +IV oxidation state and all of the [LnF(4)](-) anions are predicted to be in the +III oxidation state. The LnF(4) species are predicted to be strong oxidizing agents and the LnF(3) species are predicted to be moderate to strong Lewis acids.
机译：先前仅报道了Ce，Pr和Tb的中性四氟化物以及Dy和Nd的[LnF（7）]（3-）阴离子，其中金属处于+ IV氧化态。我们报告了我们的尝试，通过激光烧蚀的金属原子与氟的反应，以及通过基质隔离红外光谱对它们的稳定化和表征，扩展了中性镧系四氟化物的行。除了上述三种四氟化物外，我们还发现了两个新的四氟化物（NdF4）-Nd-3和（DyF4）-Dy-7，它们都处于+ IV氧化态，从而将镧系元素的氧化态扩展为两个新的金属。我们的实验结果得到了量子化学计算的支持，并且讨论了镧系元素氧化态对LnF（4）和[LnF（4）]（-）物种的作用。预计大多数LnF（4）物种处于+ IV氧化态，而所有[LnF（4）]（-）阴离子均被预测为+ III氧化态。 LnF（4）物种被预测为强氧化剂，LnF（3）物种被预测为中等至强路易斯酸。

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