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首页> 外文学位 >Mono- and Trimetallic Cobalt(II) and Monometallic Cobalt(III) Amine-bis(phenolate) Complexes: Synthesis and Structural Properties.
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Mono- and Trimetallic Cobalt(II) and Monometallic Cobalt(III) Amine-bis(phenolate) Complexes: Synthesis and Structural Properties.

机译：单金属和三金属钴（II）和单金属钴（III）胺-双（酚盐）配合物：合成和结构性质。

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摘要

This thesis describes the syntheses and structures of a series of monometallic and two trimetallic cobalt(II) amine-bis(phenolate) complexes. The protonated tripodal tetradentate ligand precursors dimethylaminoethylamino- N,N-bis(2-methylene-4,6-di-tert-butylphenol), H 2[O2NN']BuBuNMe2 and diethylaminoethylamino- N,N-bis(2-methylene4,6-di-tert-amylphenol), H 2[O2NN']AmAmNEt2 were reacted with cobaltous acetate tetrahydrate under varying conditions to afford both mono- and trimetallic species. X-ray crystallographic data of monometallic complexes [LCo[O 2NN']BuBuNMe2] (L = H2O, CH3OH, CH3COCH3, propylene oxide) showed that the Co II ion adopts a distorted trigonal bipyramidal coordination environment. In the absence of base and in the presence of excess cobaltous acetate, trimetallic complexes were isolated containing a central CoII in an octahedral environment coordinated to four CH3OH and two bridging acetate ligands between two Co[O2NN'] fragments with CoII in a trigonal bipyramidal setting. The mono- and trimetallic CoII complexes reported were also characterized by UV-vis spectroscopy, mass spectrometry, cyclic voltammetry and magnetic measurements. The CoII ions in these complexes are all high-spin and the trimetallic species show very weak antiferromagnetic behaviour when modeled as a linear isotropic trimer. Electrochemical studies reveal that the redox processes are most likely ligand based but a metal centered redox process is also possible. These works have recently been published: U. K. Das, J. Bobak, C. Fowler, S. E. Hann, C. F. Petten, L. N. Dawe, A. Decken, F. M. Kerton* and C. M. Kozak*, Dalton Trans., 2010, 39, 5462.;This thesis also describes several oxidation attempts and a successful synthesis of a monometallic CoIII amine-bis(phenolate) complex. The oxidation reactions were carried out using a variety of oxidizing agents under both aerobic and anaerobic conditions. However, only silver nitrate gave promising results in yielding a monometallic COIII amine-bis(phenolate) complex under aerobic conditions. The monometallic species was characterized by 1H NMR spectroscopy, mass spectrometry, and elemental analysis.
机译：本文描述了一系列单金属和两种三金属钴（II）胺-双（酚盐）配合物的合成和结构。质子化的三足四齿配体前体二甲基氨基乙基氨基-N，N-双（2-亚甲基-4,6-二叔丁基苯酚），H 2 [O2NN'] BuBuNMe2和二乙基氨基乙基氨基-N，N-双（2-亚甲基4,6） -二叔戊基苯酚），H 2 [O2NN'] AmAmNEt2与乙酸钴四水合物在不同条件下反应，以提供单金属和三金属物质。单金属配合物[LCo [O 2NN'] BuBuNMe2]（L = H2O，CH3OH，CH3COCH3，环氧丙烷）的X射线晶体学数据表明，Co II离子采用了扭曲的三角双锥体配位环境。在不存在碱和过量乙酸钴的情况下，在八面体环境中分离出一个含有中心CoII的三金属配合物，该化合物与四个CH3OH和两个Co [O2NN']片段之间的两个桥接乙酸盐配体配成CoII，处于三角双锥体环境。报道的单金属和三金属CoII配合物还通过紫外-可见光谱，质谱，循环伏安法和磁测量进行了表征。这些络合物中的CoII离子都是高自旋的，当建模为线性各向同性三聚体时，三金属物种显示出非常弱的反铁磁行为。电化学研究表明，氧化还原过程很可能是基于配体的，但以金属为中心的氧化还原过程也是可能的。这些作品最近已出版：UK Das，J. Bobak，C. Fowler，SE Hann，CF Petten，LN Dawe，A. Decken，FM Kerton *和CM Kozak *，Dalton Trans。，2010，39，5462。本论文还描述了几种氧化尝试和单金属CoIII胺-双（酚盐）配合物的成功合成。在需氧和厌氧条件下，使用多种氧化剂进行氧化反应。但是，只有硝酸银在有氧条件下产生单金属COIII胺-双（酚盐）配合物的结果令人鼓舞。通过1 H NMR光谱，质谱和元素分析对单金属物质进行表征。

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  • 作者

    Das, Uttam Kumar.;

  • 作者单位

    Memorial University of Newfoundland (Canada).;

  • 授予单位 Memorial University of Newfoundland (Canada).;
  • 学科 Chemistry Inorganic.
  • 学位 M.Sc.
  • 年度 2010
  • 页码 131 p.
  • 总页数 131
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 普通生物学;
  • 关键词

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