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An electrochemical evaluation of ruthenium-based electrocatalysts for oxygen evolution.

机译:钌基电催化剂的氧气析出的电化学评估。

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摘要

A study of ruthenium oxide-based oxygen evolution catalysts for use in proton exchange membrane (PEM) electrolyzers was performed. In this work, oxygen evolution catalysts were fabricated via sol-gel, high energy ball milling, and thermal processing techniques. Thermal analysis techniques such as differential scanning calorimetry (DSC), differential thermal analysis (DTA), and thermal gravimetric analysis (TGA) were used to determine the optimum processing temperatures to be used for catalysts fabrication and annealing. The materials properties of the catalysts were studied with scanning electron microscopy, energy dispersive analysis (EDAX), X-ray diffraction, and X-ray photo-electron spectroscopy.;Electrodes were fabricated from the oxygen evolution catalysts and tested in electrolysis and three-electrode cells. The catalysts fabricated via sol-gel techniques included a ruthenium oxide and an iridium-ruthenium oxide catalyst. Three families of the thermally processed catalysts were developed: iridium-ruthenium oxide, lead-ruthenium oxide, and tin ruthenium oxide. A lead oxide: ruthenium oxide catalyst was fabricated via high energy ball-milling to be used as a fabrication comparison to the thermally processed catalysts.;The electrochemical evaluations for the oxygen evolution catalysts fabricated as electrolysis cells included current-step polarization and constant current electrolysis. The current step polarization experiments were used to determine the relative performance of the catalysts as well as to determine the kinetic parameters for the oxygen evolution reaction. The constant-current electrolysis experiments were used to estimate the degradation of the catalysts during operation. In these studies, it was determined that the thermal processing technique could produce stable and high performing catalysts. The thermally processed iridium ruthenium oxide catalysts with 9 to 12 mole percent iridium had the lowest overpotential for oxygen evolution of the electrolysis cells tested.;The electrochemical evaluation of the oxygen evolution catalysts in the three electrode cell included potentiodynamic and electrochemical impedance spectroscopy (EIS) studies. The potentiodynamic polarization studies were used to rank the relative performance of catalysts being studied. The EIS studies were also used to rank the relative performance as well as to provide an estimate of the electrochemically active surface area of the catalysts. The three families of thermally processed catalysts were studied in the three-electrode cell. The results of these studies include identifying that the mechanism of oxygen evolution changed when ruthenium oxide was thermally processed with iridium and lead. Iridium, lead, and tin were all found to stabilize ruthenium oxide at oxygen evolution potentials. The three-electrode cell studies confirmed that the thermally processed iridium-ruthenium oxide with 12 mole percent iridium was the superior catalysts for oxygen evolution.
机译:进行了用于质子交换膜(PEM)电解槽的氧化钌基氧气析出催化剂的研究。在这项工作中,通过溶胶-凝胶,高能球磨和热处理技术制造了析氧催化剂。使用诸如差示扫描量热法(DSC),差示热分析(DTA)和热重分析(TGA)之类的热分析技术来确定用于催化剂制造和退火的最佳加工温度。通过扫描电子显微镜,能量色散分析(EDAX),X射线衍射和X射线光电子能谱研究了催化剂的材料性能;用析氧催化剂制备了电极,并在电解和三电极单元。通过溶胶-凝胶技术制备的催化剂包括氧化钌和铱-钌氧化物催化剂。开发了三个系列的热处理过的催化剂:铱钌氧化物,铅钌氧化物和锡钌氧化物。通过高能球磨制备氧化铅:氧化钌催化剂,并与热处理的催化剂进行制备比较。;作为电解池制备的析氧催化剂的电化学评估包括电流步极化和恒流电解。使用当前的一步极化实验来确定催化剂的相对性能以及确定氧气释放反应的动力学参数。恒流电解实验被用来估计催化剂在操作过程中的降解。在这些研究中,确定了热处理技术可以生产稳定且高性能的催化剂。具有9至12摩尔%铱的热处理过的铱钌氧化物催化剂对于所测试的电解池的氧气释放具有最低的超电势。;三电极池中氧气释放催化剂的电化学评估包括电位动力学和电化学阻抗谱(EIS)学习。电位动力学极化研究用于对所研究催化剂的相对性能进行排名。 EIS研究还用于对相对性能进行排名,并提供催化剂的电化学活性表面积的估算值。在三电极电池中研究了三类热处理过的催化剂。这些研究的结果包括确定当用铱和铅对氧化钌进行热处理时,氧气释放的机理发生了变化。铱,铅和锡都被发现可以将氧化钌稳定在氧气释放电位上。三电极电池研究证实,具有12摩尔百分比的铱的热处理铱-钌氧化物是产生氧气的优良催化剂。

著录项

  • 作者

    Valdez, Thomas I.;

  • 作者单位

    University of Southern California.;

  • 授予单位 University of Southern California.;
  • 学科 Engineering Materials Science.
  • 学位 Ph.D.
  • 年度 2010
  • 页码 200 p.
  • 总页数 200
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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