Graphical abstract<'/> Structure reactivity relationships during N_2O hydrogenation over Au-Ag alloys: A study by field emission techniques
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Structure reactivity relationships during N_2O hydrogenation over Au-Ag alloys: A study by field emission techniques

机译：Au-Ag合金N_2O加氢过程中的结构反应性关系：场发射技术研究

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Graphical abstractDisplay OmittedHighlights•Imaging and characterization of Au-Ag model catalyst as field emitter tips.•Providing atomic oxygen at the surface of Au-based catalyst.•Surface structure/reactivity relationship during N2O+H2reaction.•Improved efficiency of Au-Ag catalysts as compared to Au.AbstractTo make available atomic oxygen at the surface of a catalyst is the key step for oxidation reactions on Au-based catalysts. In this context, Au-Ag alloys catalysts exhibit promising properties for selective oxidation reactions of alcohols: low temperature activity and high selectivity. The presence of O(ads) and its effects on the catalytic reactivity is studied via the N2O dissociative adsorption and subsequent hydrogenation. Field emission techniques are particularly suited to study this reaction: Field Ion Microscopy (FIM) and Field Emission Microscopy (FEM) enable to image the extremity of sharp metallic tips, the size and morphology of which are close to those of one single catalytic particle.The reaction dynamics is studied in the 300–320 K temperature range and at a pressure of 3.5 × 10−3Pa. The main results are a strong structure/reactivity relationship during N2O + H2reaction over Au-8.8 at.%Ag model catalysts. Comparison of high-resolution FIM images of the clean sample and FEM images during reaction shows a sensitivity of the reaction to the local structure of the facets, independently of the used partial pressures of both N2O and H2. This suggests a localised dissociative adsorption step for N2O and H2with the formation of a reactive interface around the {210} facets.
机译： 图形摘要 < ce：simple-para>省略显示 突出显示 • 作为场发射器尖端的Au-Ag模型催化剂。 • 在Au基催化剂的表面提供原子氧。 • 表面结构/反应性关系在N 2 O + H 2 反应期间。 • 提高了Au-Ag的效率与Au相比的催化剂。 摘要 在Au基催化剂上进行氧化反应的关键步骤是在催化剂表面提供原子氧。在这种情况下，Au-Ag合金催化剂对醇的选择性氧化反应显示出良好的性能：低温活性和高选择性。通过N 2 O解离吸附和随后的氢化反应研究了O（ads）的存在及其对催化反应性的影响。场发射技术特别适合研究该反应：场离子显微镜（FIM）和场发射显微镜（FEM）可以对尖锐金属尖端的末端成像，其尖端和形态与单个催化颗粒的尖端和形态相近。 研究了在300-320 K温度范围和3.5 × < / mml：math> 10 -3 Pa。主要结果是在N 2 O + H 2 反应期间有很强的结构/反应关系超过Au-8.8 at。％Ag模型催化剂。比较干净样品的高分辨率FIM图像和反应期间的FEM图像，可以看出反应对刻面局部结构的敏感性，与N 2所使用的分压无关。 O和H 2 。这表明N 2 O和H 2 的局部解离吸附步骤形成了{210}构面周围的反应性接口。

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  • 来源
    《Applied Surface Science》 |2018年第30期|914-919|共6页
  • 作者

    Luc Jacobs; Cédric Barroo; Natalia Gilis; Sten V. Lambeets; Eric Genty; Thierry Visart de Bocarmé;

  • 作者单位

    Chemical Physics of Materials and Catalysis, Université libre de Bruxelles, Faculty of Sciences;

    Chemical Physics of Materials and Catalysis, Université libre de Bruxelles, Faculty of Sciences,Interdisciplinary Centre for Nonlinear Phenomena and Complex Systems (CENOLI), Université libre de Bruxelles (ULB), Faculty of Sciences;

    Chemical Physics of Materials and Catalysis, Université libre de Bruxelles, Faculty of Sciences;

    Chemical Physics of Materials and Catalysis, Université libre de Bruxelles, Faculty of Sciences;

    Chemical Physics of Materials and Catalysis, Université libre de Bruxelles, Faculty of Sciences;

    Chemical Physics of Materials and Catalysis, Université libre de Bruxelles, Faculty of Sciences,Interdisciplinary Centre for Nonlinear Phenomena and Complex Systems (CENOLI), Université libre de Bruxelles (ULB), Faculty of Sciences;

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  • 正文语种 eng
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  • 关键词

    Gold catalysis; Field emission microscopy; Au-Ag alloy; Nanocatalysis; Structure/reactivity;

    机译：金催化;场发射显微镜;Au-Ag合金;纳米催化;结构/反应性;

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