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Iron coordination chemistry of nitrogen,diazene,hydrazin,and ammonia : Investigating the mechanism of nitrogen reduction to ammonia.

机译：氮，二氮杂，肼和氨的铁配位化学：研究氮还原为氨的机理。

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摘要

The coordination chemistry of iron with N2 is becoming increasingly important as chemists try to find alternative routes to the production of ammonia. Current biological and industrial processes use iron to catalyze the formation of ammonia from N2; however, huge amounts of energy are required for this conversion. Understanding how dinitrogen and other intermediates of dinitrogen reduction interact with iron could lead to energy efficient processes for the production of ammonia.;This dissertation explores the synthesis and reactivity of an iron dinitrogen complex that reacts with acid to produce ammonia at room temperature and pressure. This dissertation also explores the progress toward determining the mechanism of this reaction in hopes of improving the yields of ammonia.;Chapter I describes both the biological nitrogen fixation process and the industrial production of ammonia and provides an in-depth look at progress toward an alternative route to ammonia using iron complexes described in the literature thus far.;Chapter II details the synthesis, characterization, and reactivity of dihydrogen and dinitrogen complexes of iron. These complexes are precursors to the active ammonia producing complex and are among a handful of dihydrogen and dinitrogen complexes that have been structurally characterized. Chapter III explores the synthesis and stability of Fe(DMeOPrPE)2N 2. This complex produces ammonia and hydrazine upon protonation with a strong acid. Optimizing the yield of ammonia from this protonation is also described.;Chapter IV discusses the synthesis and reactivity of several complexes of iron containing intermediates relevant to dinitrogen reduction, including diazene (N2H2), hydrazine (N2H4), and ammonia. By studying these intermediates, a mechanism of ammonia formation from the protonation of Fe(DMeOPrPE)2N2 is proposed that may also provide insights into the mechanism of nitrogenase. Chapter V provides a summary of this research.;This dissertation includes previously published and unpublished co-authored material.
机译：随着化学家试图寻找生产氨的替代途径，铁与N2的配位化学变得越来越重要。当前的生物和工业过程使用铁来催化由N2形成氨。但是，这种转换需要大量的能量。了解二氮和其他二氮还原的中间体如何与铁相互作用可以导致产生氨的能量高效过程。本论文探讨了铁二氮配合物的合成和反应活性，该铁二氮配合物在室温和压力下与酸反应生成氨。本论文还探讨了确定该反应机理的进展，以期提高氨的收率。第一章介绍了生物固氮工艺和氨的工业生产，并深入探讨了替代方法的进展。到目前为止，已使用文献中描述的铁络合物合成氨的路线。这些络合物是产生活性氨的络合物的前体，并且在少数已被结构表征的二氢和二氮络合物中。第三章探讨了Fe（DMeOPrPE）2N 2的合成和稳定性。该配合物在用强酸质子化时会产生氨和肼。还描述了通过该质子化优化氨的收率。第四章讨论了与二氮还原有关的含铁中间体的几种配合物的合成和反应性，其中包括重氮（N2H2），肼（N2H4）和氨。通过研究这些中间体，提出了由Fe（DMeOPrPE）2N2的质子化形成氨的机理，这也可能为了解固氮酶的机理提供参考。第五章对本研究进行了总结。本论文包括以前发表和未发表的合著材料。

著录项

  • 作者

    Crossland, Justin L.;

  • 作者单位

    University of Oregon.;

  • 授予单位 University of Oregon.;
  • 学科 Chemistry Inorganic.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 250 p.
  • 总页数 250
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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