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典型的均配型镧系四重夹心结构——合成、机理研究及量子化学研究

The Archetypal Homoleptic Lanthanide Quadruple-Decker-Synthesis, Mechanistic Studies, and Quantum Chemical Investigations.

作者信息

Münzfeld Luca, Hauser Adrian, Hädinger Pauline, Weigend Florian, Roesky Peter W

机构信息

Institute of Inorganic Chemistry, Karlsruhe Institute of Technology, Engesserstrasse 15, 76131, Karlsruhe, Germany.

Fachbereich Chemie, Philipps-Universität Marburg, Hans-Meerwein-Strasse 4, 35032, Marburg, Germany.

出版信息

Angew Chem Int Ed Engl. 2021 Nov 8;60(46):24493-24499. doi: 10.1002/anie.202111227. Epub 2021 Oct 7.

DOI:10.1002/anie.202111227
PMID:34486795
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8596981/
Abstract

Reduction of [Sm (COT )(BH )(thf)] (COT =1,4-( Pr Si) C H ) with KC resulted in [Sm (COT ) ], the first example of a homoleptic lanthanide quadruple-decker. As indicated by an analysis of the bond metrics in the solid-state, the inner Sm ion is present in the divalent oxidation state, while the outer ones are trivalent. This observation could be confirmed by quantum chemical calculations. Mechanistic studies revealed not only insight into possible formation pathways of [Sm (COT ) ] but also resulted in the transformation to other mixed metal sandwich complexes with unique structural properties. These are the 1D-polymeric chain structured [KSm (COT )] and the hexametallic species [(tol)K(COT )Sm (COT )K] which were initially envisioned as possible building blocks as part of different retrosynthetically guided pathways that we developed.

摘要

用KC还原[Sm (COT )(BH )(thf)]（COT =1,4-( Pr Si) C H ）得到了[Sm (COT ) ]，这是首例同配型镧系四重夹心化合物。正如对固态中键参数的分析所示，内部的Sm离子呈二价氧化态，而外部的Sm离子呈三价。这一观察结果可通过量子化学计算得到证实。机理研究不仅揭示了[Sm (COT ) ]可能的形成途径，还导致了向具有独特结构性质的其他混合金属夹心配合物的转化。这些配合物是一维聚合链结构的[KSm (COT )]和六金属物种[(tol)K(COT )Sm (COT )K]，它们最初被设想为我们开发的不同逆合成导向途径中的可能构建单元。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/6052afc06d8a/ANIE-60-24493-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/b51d770c7b69/ANIE-60-24493-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/1665b38b268b/ANIE-60-24493-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/713674b43e48/ANIE-60-24493-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/f99d9ac66995/ANIE-60-24493-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/be776d1404a0/ANIE-60-24493-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/6052afc06d8a/ANIE-60-24493-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/b51d770c7b69/ANIE-60-24493-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/1665b38b268b/ANIE-60-24493-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/713674b43e48/ANIE-60-24493-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/f99d9ac66995/ANIE-60-24493-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/be776d1404a0/ANIE-60-24493-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/385f/8596981/6052afc06d8a/ANIE-60-24493-g006.jpg

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