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双（N-杂环亚胺）配体支持的特屈伦-特屈酮-铁配合物的分离与反应活性

Isolation and Reactivity of Tetrylene-Tetrylone-Iron Complexes Supported by Bis(N-Heterocyclic Imine) Ligands.

作者信息

Zhao Xuan-Xuan, Szilvási Tibor, Hanusch Franziska, Kelly John A, Fujimori Shiori, Inoue Shigeyoshi

机构信息

School of Natural Sciences, Department of Chemistry, WACKER-Institute of Silicon Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstraße 4, 85748, Garching bei München, Germany.

Department of Chemical and Biological Engineering, University of Alabama, Tuscaloosa, AL 35487, USA.

出版信息

Angew Chem Int Ed Engl. 2022 Sep 26;61(39):e202208930. doi: 10.1002/anie.202208930. Epub 2022 Aug 25.

DOI:10.1002/anie.202208930
PMID:35925668
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9804675/
Abstract

The germanium iron carbonyl complex 3 was prepared by the reaction of dimeric chloro(imino)germylene [IPrNGeCl] (IPrN=bis(2,6-diisopropylphenyl)imidazolin-2-iminato) with one equivalent of Collman's reagent (Na Fe(CO) ) at room temperature. Similarly, the reaction of chloro(imino)stannylene [IPrNSnCl] with Na Fe(CO) (1 equiv) resulted in the Fe(CO) -bridged bis(stannylene) complex 4. We observed reversible formation of bis(tetrylene) and tetrylene-tetrylone character in complexes 3 vs. 5 and 4 vs. 6, which was supported by DFT calculations. Moreover, the Li/Sn/Fe trimetallic complex 12 has been isolated from the reaction of [IPrNSnCl] with cyclopentadienyl iron dicarbonyl anion. The computational analysis further rationalizes the reduction pathway from these chlorotetrylenes to the corresponding complexes.

摘要

通过二聚氯（亚氨基）锗烯[IPrNGeCl]（IPrN = 双（2,6 - 二异丙基苯基）咪唑啉 - 2 - 亚氨基）与一当量的科尔曼试剂（NaFe(CO)）在室温下反应制备了锗铁羰基配合物3。类似地，氯（亚氨基）锡烯[IPrNSnCl]与NaFe(CO)（1当量）反应生成了Fe(CO)桥连的双（锡烯）配合物4。我们观察到在配合物3与5以及4与6中双（四价烯）和四价烯 - 四价酮特征的可逆形成，这得到了密度泛函理论计算的支持。此外，Li/Sn/Fe三金属配合物12是从[IPrNSnCl]与环戊二烯基铁二羰基阴离子的反应中分离得到的。计算分析进一步阐明了从这些氯代四价烯到相应配合物的还原途径。

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