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Carbon Monoxide Oxidation on Nanoparticle Catalysts and Gas Phase Reactions of Small Molecules and Volatile Organics with Metal Cations

机译：纳米粒子催化剂上的一氧化碳氧化和带有金属阳离子的小分子和挥发性有机物的气相反应

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This dissertation demonstrates the application of a vapor phase method to synthesize supported and unsupported nanoparticle catalysts for CO oxidation. The method is based on the Laser Vaporization/Controlled Condensation (LVCC) technique. The first part of this dissertation presents the vapor phase synthesis and characterization of gold nanoparticles supported on a variety of oxide supports such as CeO2, TiO2, CuO and MgO.The results indicate that Au nanoparticles supported on CeO2 exhibit higher catalytic activity than Au supported on other oxides. The high activity of the Au/CeO2 catalyst is attributed to the strong interaction of Au with CeO2. The results also indicate that 5% Au loading on CeO2 has higher activity than 2% Au or 10% Au. When comparing the catalytic activity of Au/CeO2 prepared by physical (LVCC) and chemical (deposition-precipitation)methods, it was found that the catalytic activity is higher for Au/CeO2 prepared by the deposition-precipitation method.The effect of alloying Au and Cu nanoparticles on the catalytic activity for low temperature CO oxidation was also investigated. The unsupported Au-Cu alloy nanoparticle catalyst exhibits higher catalytic activity than the activities of the individualcomponents and their physical mixtures. The XRD data of Au-Cu alloy taken after the catalysis test indicates the formation of CuO within the bimetallic nanoparticles, whichimproves the catalytic activity of Au-Cu alloy nanoparticle.The second part of this dissertation investigates the gas phase reactions of Au+ and Cu+ with CO, O2 and H2O molecules using the Laser Vaporization ionization, High-Pressure Mass Spectrometry (LVI-HPMS) technique. The gas phase reactions resulting from the interactions of Au+ with CO and O2 molecules are investigated. Although multiple additions of CO and O2 molecules on Au+ have been observed at room temperature, no evidence was found of the production of CO2. This is attributed to the presence of water molecules which effectively replace the oxygen molecules on Au+ at room temperature.Finally, the role of the metal cations Au+ and Cu+ in initiating the gas phase polymerization of butadiene and isoprene vapors was investigated.
机译：本文证明了气相法在合成负载型和非负载型纳米粒子催化剂中的应用。该方法基于激光蒸发/控制冷凝（LVCC）技术。本文的第一部分介绍了负载在各种氧化物载体如CeO2，TiO2，CuO和MgO上的金纳米颗粒的气相合成和表征。其他氧化物。 Au / CeO2催化剂的高活性归因于Au与CeO2的强相互作用。结果还表明，在CeO2上负载5％的Au具有比2％的Au或10％的Au高的活性。比较物理方法（LVCC）和化学方法（沉积-沉淀）制备的Au / CeO2的催化活性，发现沉积-沉淀法制备的Au / CeO2的催化活性更高。还研究了Cu纳米颗粒对低温CO氧化的催化活性。无载体的Au-Cu合金纳米颗粒催化剂显示出比单个组分及其物理混合物更高的催化活性。催化试验后的Au-Cu合金的XRD数据表明，在双金属纳米粒子中形成了CuO，提高了Au-Cu合金纳米粒子的催化活性。第二部分研究了Au +和Cu +在气相中的反应。 CO，O2和H2O分子使用激光汽化电离高压质谱（LVI-HPMS）技术。研究了Au +与CO和O2分子相互作用产生的气相反应。尽管在室温下已观察到在Au +上多次添加CO和O2分子，但未发现产生CO2的证据。这归因于水分子的存在，该水分子可在室温下有效替代Au +上的氧分子。最后，研究了金属阳离子Au +和Cu +在引发丁二烯和异戊二烯蒸气的气相聚合中的作用。

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