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最重的可瓶装金属烯：一种单原子零价铅配合物（“铅烯”）的合成

The Heaviest Bottleable Metallylone: Synthesis of a Monatomic, Zero-Valent Lead Complex ("Plumbylone").

作者信息

Xu Jian, Pan Sudip, Yao Shenglai, Frenking Gernot, Driess Matthias

机构信息

Department of Chemistry: Metalorganics and Inorganic Materials, Technische Universität Berlin, Strasse des 17. Juni 115, Sekr. C2, 10623, Berlin, Germany.

Philipps-Universität Marburg, Fachbereich Chemie, 35032, Marburg, Germany.

出版信息

Angew Chem Int Ed Engl. 2022 Sep 19;61(38):e202209442. doi: 10.1002/anie.202209442. Epub 2022 Aug 8.

DOI:10.1002/anie.202209442
PMID:35848899
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9545849/
Abstract

The elusive plumbylone {[Si (Xant)Si ]Pb } 3 stabilized by the bis(silylene)xanthene chelating ligand 1, [Si (Xant)Si =PhC(NtBu) Si(Xant)Si(NtBu) CPh], and its isolable carbonyl iron complex {[Si (Xant)Si ]Pb Fe(CO) } 4 are reported. The compounds 3 and 4 were obtained stepwise via reduction of the lead(II) dibromide complex {[Si (Xant)Si ]PbBr } 2, prepared from the bis(silylene)xanthene 1 and PbBr , employing potassium naphthalenide and K Fe(CO) , respectively. While the genuine plumbylone 3 is rather labile even at -60 °C, its Pb →Fe(CO) complex 4 turned out to be relatively stable and bottleable. However, solutions of 4 decompose readily to elemental Pb and {[Si (Xant)Si ]Fe(CO) } 5 at 80 °C. Reaction of 4 with [Rh(CO) Cl] leads to the formation of the unusual dimeric [(OC) RhPb(Cl)Fe(CO) ] complex 6 with trimetallic Rh-Pb-Fe bonds. The molecular and electronic structures of 3 and 4 were established by Density Functional Theory (DFT) calculations.

摘要

报道了由双（硅烯）占吨螯合配体1稳定的难以捉摸的铅烯{[Si(Xant)Si]Pb}₃，[Si(Xant)Si = PhC(NtBu)Si(Xant)Si(NtBu)CPh]，以及其可分离的羰基铁配合物{[Si(Xant)Si]PbFe(CO)}₄。化合物3和4分别通过萘基钾和K₂Fe(CO)₅还原由双（硅烯）占吨1和PbBr₂制备的二溴化铅配合物{[Si(Xant)Si]PbBr₂}逐步获得。虽然真正的铅烯3即使在-60°C时也相当不稳定，但其Pb→Fe(CO)配合物4相对稳定且可保存。然而，4的溶液在80°C时很容易分解为元素铅和{[Si(Xant)Si]Fe(CO)}₅。4与[Rh(CO)₂Cl]反应生成具有三金属Rh-Pb-Fe键的不寻常二聚体[(OC)₂RhPb(Cl)Fe(CO)₂]配合物6。通过密度泛函理论（DFT）计算确定了3和4的分子和电子结构。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/23a5b82bd1ab/ANIE-61-0-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/fed90110e28c/ANIE-61-0-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/9d1afe2152f3/ANIE-61-0-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/4bd0c2755185/ANIE-61-0-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/ea4661a605b1/ANIE-61-0-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/b04716b4c873/ANIE-61-0-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/23a5b82bd1ab/ANIE-61-0-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/fed90110e28c/ANIE-61-0-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/9d1afe2152f3/ANIE-61-0-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/4bd0c2755185/ANIE-61-0-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/ea4661a605b1/ANIE-61-0-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/b04716b4c873/ANIE-61-0-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a54/9545849/23a5b82bd1ab/ANIE-61-0-g005.jpg

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