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Formic Acid Oxidation on Pt/Ru Nanoparticles: Temperature Effects

机译:甲酸氧化在Pt / Ru纳米粒子上:温度效应

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The formic acid oxidation on Pt/Ru nanoparticles in acid solution over the temperature range 298-333 K has been studied by thin-film rotating disk method (RDE). Transmission electron microscopy in combination with scanning tunneling microscopy was used to determine the size (4.3 ± 0.3 nm) and shape (cuboctahedral) of the particles. Kinetic analysis revealed that at elevated temperatures (313 K, 333 K) the reaction rate is much higher than at room temperature (295 K), indicating that formic acid oxidation on supported Pt/Ru catalyst is a highly activated process. Based on experimental kinetic parameters we propose that the HCOOH oxidation on the PtRu alloy most likely follows a dual pathway, but the branching ratio is still very high, i.e. Pt-like. The principal effect of opening the dehydration channel at steady-state (via the presence of Ru in the surface) is to lower the coverage of CO_(ads) on Pt sites and permit the dehydrogenation path to increase in rate.
机译:通过薄膜旋转盘法(RDE)研究了在温度范围内酸溶液中的酸溶液中Pt / Ru纳米颗粒的甲酸氧化。透射电子显微镜与扫描隧道显微镜相结合用于确定颗粒的尺寸(4.3±0.3nm)和形状(副叶锥面向)。动力学分析显示,在升高的温度下(313 k,333k),反应速率远高于室温(295 k),表明支持的Pt / Ru催化剂上的甲酸氧化是一种高活性的方法。基于实验动力学参数,我们提出了PTRU合金的HCOOH氧化最可能遵循双路途径,但分支比仍然非常高,即PT样。在稳态上打开脱水通道的主要效果(表面在表面中的存在)是降低PT位点上的CO_(ADS)的覆盖率,并允许脱氢途径增加速率。

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