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由非经典镧系化合物衍生的d/f-多氮族化合物：合成、小分子活化及光学性质

d/f-Polypnictides Derived by Non-Classical Ln Compounds: Synthesis, Small Molecule Activation and Optical Properties.

作者信息

Reinfandt Niklas, Michenfelder Nadine, Schoo Christoph, Yadav Ravi, Reichl Stephan, Konchenko Sergey N, Unterreiner Andreas N, Scheer Manfred, Roesky Peter W

机构信息

Institut für Anorganische Chemie, Karlsruher Institut für Technologie (KIT), Engesserstr. 15, Geb. 30.45, 76131, Karlsruhe, Germany.

Institut für Physikalische Chemie, Karlsruher Institut für Technologie (KIT), Fritz-Haber-Weg 2, Geb. 30.44, 76131, Karlsruhe, Germany.

出版信息

Chemistry. 2021 May 20;27(29):7862-7871. doi: 10.1002/chem.202100605. Epub 2021 May 3.

DOI:10.1002/chem.202100605
PMID:33780594
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8252591/
Abstract

Reduction chemistry induced by divalent lanthanides has been primarily focused on samarium so far. In light of the rich physical properties of the lanthanides, this limitation to one element is a drawback. Since molecular divalent compounds of almost all lanthanides have been available for some time, we used one known and two new non-classical reducing agents of the early lanthanides to establish a sophisticated reduction chemistry. As a result, six new d/f-polyphosphides or d/f-polyarsenides, [K(18-crown-6)] [Cp'' Ln(E )FeCp*] (Ln=La, Ce, Nd; E=P, As) were obtained. Their reactivity was studied by activation of P , resulting in a selective expansion of the P rings. The obtained compounds [K(18-crown-6)] [Cp'' Ln(P )FeCp*] (Ln=La, Nd) are the first examples of an activation of P by a f-element-polypnictide complex. Additionally, the first systematic femtosecond (fs)-spectroscopy investigations of d/f-polypnictides are presented to showcase the advantages of having access to a broader series of lanthanide compounds.

摘要

到目前为止，二价镧系元素引发的还原化学主要集中在钐上。鉴于镧系元素丰富的物理性质，将研究局限于一种元素是一个缺点。由于几乎所有镧系元素的分子二价化合物已经问世一段时间了，我们使用了一种已知的和两种新的早期镧系元素的非经典还原剂来建立复杂的还原化学。结果，得到了六种新的d/f-多磷化物或d/f-多砷化物，即[K(18-冠-6)][Cp''Ln(E)FeCp*](Ln = La、Ce、Nd；E = P、As)。通过P的活化研究了它们的反应性，导致P环的选择性扩展。所得到的化合物[K(18-冠-6)][Cp''Ln(P)FeCp*](Ln = La、Nd)是f-元素-多氮族化物配合物活化P的首例。此外，还展示了对d/f-多氮族化物进行首次系统的飞秒(fs)光谱研究，以展示获得更广泛系列镧系化合物的优势。

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