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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Versatile reactivities of rare-earth metal dialkyl complexes supported by a neutral pyrrolyl-functionalized beta-diketiminato ligand
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Versatile reactivities of rare-earth metal dialkyl complexes supported by a neutral pyrrolyl-functionalized beta-diketiminato ligand

机译：由中性吡咯基官能化的β-二酮氨基硅酸盐配体支持的稀土金属二烷基复合物的多功能反应性

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摘要

Herein, rare-earth metal dialkyl complexes supported by a neutral pyrrolyl-functionalized -diketiminato ligand with the formula LRE(CH2SiMe3)(2)(thf) (RE = Y (1a), Dy (1b), Er (1c), Yb (1d); L = MeC(NDipp)CHC(Me)NCH2CH2NC4H2-2,5-Me-2, Dipp = 2,6-(Pr2C6H3)-Pr-i) were synthesized via the reactions of the -diketimine HL with the rare-earth metal trialkyl complexes RE(CH2SiMe3)(3)(thf)(2) in high yields. The reactivities of 1 with pyridine derivatives, unsaturated substrates, and elemental sulfur were investigated, and some interesting chemical transformations were observed. Ligand exchange and activation of sp(2) and sp(3) C-H bonds occurred during the reactions with pyridine derivatives to afford different types of mononuclear rare-earth metal pyridyl complexes, namely, LEr(CH2SiMe3)(2)((1)-NC5H4) (2c), LRE((3)-CH2-2-NC5H2-4,6-Me-2)(2) (RE = Y (3a), Er (3c)), and LRE(CH2SiMe3)((2)-(C,N)-2-(2-C6H4NC5H4)) (RE = Er (4c), Yb = (4d)). Similarly, activation of the sp C-H bond occurred during the reaction of phenylacetylene with 1c to produce the dinuclear erbium alkynyl complex [LEr(CH2SiMe3)(-C?CPh)](2) (5c). The mixed amidinate--diketiminato ytterbium complex LYb[(Dipp)NC(CH2SiMe3)N(Dipp)](CH2SiMe3) (6d) was obtained by the insertion of bis(2,6-diisopropylphenyl)carbodiimide into a Yb-alkyl bond, as well as via the direct alkane elimination of a CH2SiMe3 moiety with bis(2,6-diisopropylphenyl)formamidine to afford the erbium complex LEr(DippNCHNDipp)(CH2SiMe3) (7c). A rare sp(2) C-H bond oxidation of the -diketiminato backbone with elemental sulfur insertion was detected to provide the unprecedented dinuclear rare-earth metal thiolate complexes (LRE)(2)(-SCH2SiMe3)(2)(-SCC(Me)(NDipp)C(Me)NCH2CH2NC4H2Me2-2,5) (RE = Y (8a), Er (8c)) in the reactions of S-8 with 1a and 1c, respectively. The molecular structures of the complexes 1-8 were determined by single-crystal X-ray diffraction analyses.
机译：在此，由中性吡咯基官能化的-diketiminato配体负载的稀土金属二烷基复合物，其中式LRE（CH2SIME3）（2）（THF）（RE = Y（1a），Dy（1b），er（1c），yb （1D）; L = MEC（NDIPP）CHC（ME）NCH2CH2NC4H2-2,5-ME-2，DIPP = 2,6-（PR2C6H3）-PR-I）通过-DIKETIMINE HL的反应合成稀土化金属三烷基复合物Re（CH2Sime3）（3）（THF）（2）高收率。研究了用吡啶衍生物，不饱和基底和元素硫的反应性，观察到一些有趣的化学转化。 Ligand交换和Sp（2）和SP（3）CH键的激活在与吡啶衍生物的反应中发生，得到不同类型的单核稀土金属吡啶基络合物，即LER（CH2SIME3）（2）（（1） - NC5H4）（2C），LRE（（3）-CH2-2-NC5H2-4,6-ME-2）（2）（RE = Y（3A），ER（3C））和LRE（CH2SIME3）（（ 2） - （C，N）-2-（2-C6H4NC5H4））（RE = ER（4C），YB =（4D））。类似地，在苯乙烯的反应期间，在苯乙烯与1C的反应期间发生SP C-H键的激活，以产生二核alkynyl络合物[LER（CH2SIME3）（ - C 2 CPH）]（2）（5℃）。通过将双（2,6-二异丙基苯基）碳二亚胺插入YB-烷基键，得到混合的脒基 - Diketiminato镱络合物[（dipp）Nc（Ch 2 Sime3）（6d）获得，以及通过与双（2,6-二异丙基苯基）甲脒的CH2Sime3部分的直接烷烃消除，得到铒复合物（Dippnchndipp）（CH2Sime3）（7c）。检测到具有元素硫插入的-diketiminato骨架的稀有SP（2）CH键氧化，以提供前所未有的二核稀土金属硫醇酸酯配合物（LRE）（2）（ - SCH2SIME3）（2）（ - SCC（ME） （NDIPP）C（ME）NCH2CH2NC4H2ME2-2,5）（RE = Y（8A），ER（8C）分别具有1A和1C的S-8的反应。通过单晶X射线衍射分析来确定复合物1-8的分子结构。

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    Zhu Xiancui; Li Yang; Guo Dianjun; Wang Shaowu; Wei Yun; Zhou Shuangliu;

  • 作者单位

    Anhui Normal Univ Key Lab Funct Mol Solids Anhui Lab Mol Based Mat Minist Educ Coll Chem &

    Mat Sci Wuhu 241000 Anhui Peoples R China;

    Anhui Normal Univ Key Lab Funct Mol Solids Anhui Lab Mol Based Mat Minist Educ Coll Chem &

    Mat Sci Wuhu 241000 Anhui Peoples R China;

    Anhui Normal Univ Key Lab Funct Mol Solids Anhui Lab Mol Based Mat Minist Educ Coll Chem &

    Mat Sci Wuhu 241000 Anhui Peoples R China;

    Anhui Normal Univ Key Lab Funct Mol Solids Anhui Lab Mol Based Mat Minist Educ Coll Chem &

    Mat Sci Wuhu 241000 Anhui Peoples R China;

    Anhui Normal Univ Key Lab Funct Mol Solids Anhui Lab Mol Based Mat Minist Educ Coll Chem &

    Mat Sci Wuhu 241000 Anhui Peoples R China;

    Anhui Normal Univ Key Lab Funct Mol Solids Anhui Lab Mol Based Mat Minist Educ Coll Chem &

    Mat Sci Wuhu 241000 Anhui Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;无机化学;
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