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首页> 外文期刊>Physical chemistry chemical physics: PCCP >Adsorption and reaction of methanol on supported palladium catalysts: microscopic-level studies from ultrahigh vacuum to ambient pressure conditions
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Adsorption and reaction of methanol on supported palladium catalysts: microscopic-level studies from ultrahigh vacuum to ambient pressure conditions

机译：负载型钯催化剂上甲醇的吸附和反应：从超高真空到环境压力条件的微观水平研究

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摘要

We investigated the decomposition and ( partial) oxidation of methanol on Pd based catalysts in an integrated attempt, simultaneously bridging both the pressure and the materials gap. Combined studies were performed on well-defined Pd model catalysts based on ordered Al2O3 and Fe3O4 thin films, on well-defined particles supported on powders and on Pd single crystals. The interaction of Pd nanoparticles and Pd( 111) with CH3OH and CH3OH/O-2 mixtures was examined from ultrahigh vacuum conditions up to ambient pressures, utilizing a broad range of surface specific vibrational spectroscopies which included IRAS, TR-IRAS, PM-IRAS, SFG, and DRIFTS. Detailed kinetic studies in the low pressure region were performed by molecular beam methods, providing comprehensive insights into the microkinetics of the reaction system. The underlying microscopic processes were studied theoretically on the basis of specially designed 3-D nanocluster models containing similar to 10(2) metal atoms. The efficiency of this novel modelling approach was demonstrated by rationalizing and complementing pertinent experimental results. In order to connect these results to the behavior under ambient conditions, kinetic and spectroscopic investigations were performed in reaction cells and lab reactors. Specifically, we focused on ( 1) particle size and structure dependent effects in methanol oxidation and decomposition, ( 2) support effects and their relation to activity and selectivity, ( 3) the influence of poisons such as carbon, and ( 4) the role of oxide and surface oxide formation on Pd nanoparticles.
机译：我们以整合尝试研究了甲醇在Pd基催化剂上的分解和（部分）氧化，同时弥合了压力和材料间隙。对基于有序Al2O3和Fe3O4薄膜的明确定义的Pd模型催化剂，粉末上负载的明确定义的颗粒和Pd单晶进行了联合研究。在超高真空条件下至环境压力下，使用多种表面比振动光谱仪（包括IRAS，TR-IRAS，PM-IRAS）检查了Pd纳米颗粒和Pd（111）与CH3OH和CH3OH / O-2混合物的相互作用，SFG和DRIFTS。通过分子束方法对低压区域进行了详细的动力学研究，从而深入了解了反应系统的微动力学。在特殊设计的包含与10（2）个金属原子相似的3-D纳米簇模型的基础上，对潜在的微观过程进行了理论研究。通过合理化和补充相关实验结果证明了这种新颖建模方法的效率。为了将这些结果与环境条件下的行为联系起来，在反应池和实验室反应器中进行了动力学和光谱研究。具体来说，我们重点研究（1）甲醇氧化和分解过程中颗粒大小和结构的影响，（2）支持作用及其与活性和选择性的关系，（3）毒物如碳的影响，以及（4）作用钯纳米粒子上氧化物和表面氧化物的形成

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