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首页> 外文期刊>The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical >Ensemble Size Effects on Toluene Hydrogenation and Hydrogen Chemisorption by Supported Bimetallic Particle Catalysts
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Ensemble Size Effects on Toluene Hydrogenation and Hydrogen Chemisorption by Supported Bimetallic Particle Catalysts

机译:载体大小对负载型双金属颗粒催化剂对甲苯加氢和氢化学吸附的影响

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Silica-supported bimetalic catalysts were prepared by decomposing the molecular clusters Pt_2Au_4 (C ident to C~tBu)_8 and Pt_2Cu_4(C ident to C~tBu)_8. The resulting catalysts were characterized with hydrogen, oxygen, and carbon monoxide chemisorptions. These indicated that CO chemisorption is the preferred method for evaluating metal dispersion. Chemisorption results also suggested that different types of substrate binding sites may be present on the bimetallic particles and that a signficant fraction of the available platinum atoms may not be capable of activating hydrogen. Catalytic activity was evaluated with the toluene hydrogenation reaction. The new catalysts were found to be relatively inactive for this reaction at 60 deg C, despite having high platinum dispersions. Apparent activation energies for toluene hydrogenation were evaluated with Arrhenius plots. Although activities were low at 60 deg C, the cluster-derived catalysts had smaller apparent activation energies than a traditionaly prepared Pt/silica catalyst. Trends in hydrogen chemisorption and toluene hydrogenation are discussed in terms of possible electronic, paraticle size, and ensemble size effects.
机译:通过分解分子簇Pt_2Au_4(C等同于C〜tBu)_8和Pt_2Cu_4(C等同于C〜tBu)_8制备二氧化硅负载的双金属催化剂。用氢,氧和一氧化碳的化学吸附对所得催化剂进行表征。这些表明CO化学吸附是评估金属分散性的优选方法。化学吸附结果还表明,在双金属颗粒上可能存在不同类型的底物结合位点,并且可用铂原子的重要部分可能无法激活氢。用甲苯氢化反应评价催化活性。尽管具有高铂分散度,但发现新催化剂在60℃下对于该反应是相对惰性的。用Arrhenius图评估了甲苯氢化的表观活化能。尽管在60℃下活性较低,但与传统制备的Pt /二氧化硅催化剂相比,簇状催化剂的表观活化能较小。氢化学吸附和甲苯加氢的趋势已从可能的电子,微粒尺寸和整体尺寸效应方面进行了讨论。

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