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首页> 外文OA文献 >Carbon monoxide oxidation at the interface of a direct barrier discharge and a thin layer of Yttria-stabilized Zirconia : characterization of discharge properties and determination of reaction rates
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Carbon monoxide oxidation at the interface of a direct barrier discharge and a thin layer of Yttria-stabilized Zirconia : characterization of discharge properties and determination of reaction rates

机译：一氧化碳在直接势垒放电和氧化钇稳定的氧化锆薄层的界面处的氧化：放电特性的表征和反应速率的确定

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摘要

This thesis investigates the carbon monoxide oxidation at the interface between a Direct Barrier Discharge (DBD) and a thin layer of Yttria-stabilized Zirconia (YSZ), which is an oxygen ion conductor. The thin film is deposited on a dielectric consisting of fused silica. The aim of this work was to investigate the reaction rates of the carbon monoxide oxidation according to the new concept of heterogeneous plasma catalysis with an oxygen ion conducting catalyst. In this work the uncoated fused silica dielectrics were used as reference system and compared with coated dielectrics with a thin YSZ film. The temperature dependent behavior of this system and the discharge itself was monitored as there should be differences according to the thermally activated electrode kinetics and oxygen transport processes in the bulk. A second aspect of the investigations was the frequency dependent behavior of the discharge and the influence of the discharge frequency on the catalytic rate enhancement.The different discharge setups were investigated according to the distribution of the ionic and excited species with Optical Emission Spectroscopy (OES). Theses results were compared with data obtained by Quadrupol Mass Spectroscopy (QMS). Additionally plasma ignition voltages according to the different discharge compositions at room and elevated temperatures were measured.The QMS signal intensities were used to compare carbon dioxide reaction rates of the reference and the YSZ coated discharge setups. The obtained data was used to discuss possible kinetic models.The OES investigations showed that the discharge is strongly influenced by the carbon monoxide gas. The dominant lines recorded are related to CO+ ions, only at very low CO partial pressures lines of Ar+ occur. Only rarely and with decreasing intensity at higher oxygen partial pressures oxygen emission lines can be found. This might be a clue to increased concentrations of negatively charged oxygen ions.With all performed observations it can be concluded that the thin film deposition of a YSZ layer on a fused silica dielectric enhances the reaction rate of the carbon monoxide oxidation due to a discharge YSZ surface interaction or to a YSZ surface restructuring, which takes especially place at room temperature conditions. Possible kinetic models were proposed.
机译：本文研究了直接阻挡放电（DBD）与氧化钇稳定的氧化锆（YSZ）薄层之间的界面处的一氧化碳氧化，氧化钇稳定的氧化锆是氧离子导体。薄膜沉积在由熔融石英组成的电介质上。这项工作的目的是根据氧离子传导催化剂的多相等离子体催化的新概念，研究一氧化碳氧化的反应速率。在这项工作中，将未涂覆的熔融石英电介质用作参考系统，并与具有YSZ薄膜的涂覆电介质进行比较。监测该系统的温度依赖性行为和放电本身，因为根据本体中的热活化电极动力学和氧气传输过程应存在差异。研究的第二个方面是放电的频率依赖性行为以及放电频率对催化速率增强的影响。使用电子发射光谱法（OES）根据离子和受激物种的分布研究了不同的放电设置。 。将这些结果与通过Quadrupol质谱（QMS）获得的数据进行比较。此外，还根据室温和高温下不同放电组成的等离子点火电压进行了测量。QMS信号强度用于比较参考样品和YSZ涂层放电设置的二氧化碳反应速率。获得的数据用于讨论可能的动力学模型。OES研究表明，放电受到一氧化碳气体的强烈影响。记录的主要谱线与CO +离子有关，仅在非常低的CO分压下会出现Ar +谱线。仅在极高的氧气分压下极少且强度降低，才能发现氧气排放线。这可能是带负电的氧离子浓度增加的线索。通过所有观察到的结果可以得出结论，由于放电YSZ，YSZ层在熔融石英电介质上的薄膜沉积可提高一氧化碳氧化的反应速率。表面相互作用或YSZ表面重组，尤其是在室温条件下。提出了可能的动力学模型。

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    Steinmüller Sven Ole;

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  • 年度 2014
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