Understanding the effects of catalyst surface structure on a catalytic reaction is of fundamental importance in catalysis chemistry. Herein, a series of Pt-on-Au (Pt_m^Au, m refers to the atomic Pt/Au ratio; Au size: 3.2 ± 0.4 nm) nanostructures with Pt dispersion in the range of 38% to 100% are used to study the structure sensitivity of the hydrogenation reactions of 1,3-butadiene and ethylene, respectively. The specific catalytic rates for both reactions are observed to increase with a decrease in the Pt dispersion or increasing m in Pt_m^Au, demonstrating the structure-sensitive nature of both reactions over the Pt_m^Au nanostructures. These observations strongly contrast with the structure insensitivity of the same reactions over our deliberately prepared counterpart Pt/SiO₂ catalysts with Pt dispersion varying in 6%∼100% and also those documented in literature and thus identify a distinct feature of Pt in the Pt_m^Au nanostructures. Characterization results from XANES spectroscopy and DRIFTS of adsorbed CO show that the variation of Pt dispersion or m in Pt_m^Au resulted in systematical changes in the electronic property of Pt, which uncover the nature of the structure sensitivity. These findings would have important implications for better understanding the dimension and richness of the structure-sensitivity concept and the features of Pt-on-Au nanostructures in catalysis and nanomaterial chemistry, as well as its related fields.

中文翻译：

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纳米结构的Au上Pt催化剂对烯烃的加氢反应是否仍保持对Pt不敏感的结构？

理解催化剂表面结构对催化反应的影响在催化化学中至关重要。在此，使用一系列Pt-on-Au（Pt _m ^ Au，m表示原子Pt / Au比； Au尺寸：3.2±0.4 nm）纳米结构，其Pt分散度在38％至100％的范围内。分别研究了1,3-丁二烯和乙烯加氢反应的结构敏感性。对于两个反应中特定的催化速率观察到与增加的Pt分散的减少或增加米中的Pt_米^的Au，这证明两个反应的结构敏感性质在Pt_米^ Au纳米结构。这些观察结果与我们精心制备的对应Pt / SiO ₂催化剂（Pt分散度在6％〜100％之间变化）中相同反应的结构不敏感性形成鲜明对比，而且这些文献也有文献记载，从而确定了Pt _m中Pt的显着特征。^ Au纳米结构。从XANES表征结果光谱和所吸附的CO显示DRIFTS该铂分散体或变化米中的Pt_米^ Au导致Pt的电子性质发生系统性变化，从而揭示了结构敏感性的本质。这些发现对更好地理解结构敏感性概念的大小和丰富性以及催化和纳米材料化学及其相关领域中的Pu-on-Au纳米结构的特征具有重要意义。