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Synthesis and characterization of metal complexes with redox active ligand (bis(tetrazinyl)-pyridine: Towards activation of small substrates.

机译：具有氧化还原活性配体（双（四嗪基）-吡啶的金属配合物的合成和表征：朝着小的底物的活化。

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摘要

A substantial part of contemporary research focuses on renewable and alternative energy sources as well as the transformation of greenhouse gases into useful byproducts using unsaturated metal complexes. Of particular interest is the bond activation by metal complexes in which both the metal core and the ligand can play active and synergistic roles, thereby providing new catalytic opportunities. One class of ligands that can potentially play this active role are redox active ligands. Redox active ligands are defined as when the oxidation state of the metal becomes ambiguous due to the character of the ligand and the effect it has on the molecular orbitals within a complex.;A brand new redox-active pincer ligand synthesized by Dr. Kumar Parimal, is a 2,2',2"--terpyridine analog called bis(tetrazinyl)pyridine (bTzP). The novelty of bTzP lies in the tetrazinyl fragment's low lying LUMO (?*) combined with stable radical anions and unusually low reduction potentials, making it ideal for redox chemistry. The ligand has not one, but two tetrazinyl "arms", effectively increasing the number of electrons stored on the ligand. In effect, we envision this as a way to dramatically expand the number of possible redox states that a transition metal complex may sample during a catalytic cycle.;To understand the redox activity of the ligand, electrochemical studies were done on the bTzP ligand and a variety of bTzP-metal complexes. Specifically, the ligand was studied with transition metals at various oxidation states (Ni, Cu, V) to not only ascertain the coordination chemistry of the ligand but study the redox chemistry as well. Future work will focus on modifications to the ligand, future directions of synthesized metals, synthesis with early transition metals, and activation of small substrates.
机译：当代研究的很大一部分集中在可再生和替代能源，以及使用不饱和金属配合物将温室气体转化为有用的副产物。特别令人感兴趣的是金属配合物的键活化，其中金属核和配体都可以发挥活性和协同作用，从而提供了新的催化机会。可以潜在地发挥这种活性作用的一类配体是氧化还原活性配体。氧化还原活性配体定义为当金属的氧化态由于该配体的特性及其对络合物内分子轨道的影响而变得模棱两可时; Kumar Parimal博士合成的一种全新的氧化还原活性夹钳配体，是2,2'，2“-吡啶类类似物，称为双（四嗪基）吡啶（bTzP）。bTzP的新颖之处在于四嗪基片段的低位LUMO（？*），具有稳定的自由基阴离子和异常低的还原电位因此，它非常适合氧化还原化学，该配体没有一个，而是两个四嗪基“臂”，有效地增加了配体上存储的电子数量，实际上，我们设想这是一种显着扩大可能的氧化还原态数量的方法为了了解配体的氧化还原活性，对bTzP配体和各种bTzP-金属配合物进行了电化学研究，特别是对过渡配体进行了转移在各种氧化态（Ni，Cu，V）的金属上进行氧化，不仅可以确定配体的配位化学，还可以研究氧化还原化学。未来的工作将集中在配体的修饰，合成金属的未来发展方向，早期过渡金属的合成以及小型底物的活化上。

著录项

  • 作者

    Hui, Alice Kay.;

  • 作者单位

    Indiana University.;

  • 授予单位 Indiana University.;
  • 学科 Inorganic chemistry.
  • 学位 M.S.
  • 年度 2016
  • 页码 304 p.
  • 总页数 304
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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