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The Electrooxidation of Formic Acid on Pd Nanoparticles: an Investigation of Size-Dependent Performance

机译：Pd纳米粒子上甲酸的电氧化：对尺寸依赖性性能的研究

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摘要

Palladium nanoparticles (Pd NPs) were deposited on highly oriented pyrolytic graphite (HOPG) substrates by using a potentiostatic double-pulse technique. The NPs possessed a narrow size distribution and wide dispersion. The particle density was in the order of 10(9) cm(-2). The average height of Pd NPs was controlled in a range of 3 to 50 nm by adjusting the duration of growth pulse. The carbon monoxide (CO) stripping at Pd NPs smaller than 14 nm occurred predominantly at a potential above 1.1 V, which is around 0.2 V more positive than that at bulk Pd and larger Pd NPs, due to the small Pd NPs tending to possess well-ordered (111) facets and a high ratio of edge and corner atoms. The high coverage of adsorbed CO (COads) at small Pd NPs can block the formation of adsorbed hydroxyl (OHads) and drive up the oxidation potential. During formic acid oxidation (FAO), small Pd NPs were quickly poisoned by CO, which was formed initially at edges and corner atoms by electrochemical reduction of FAO product CO2 at low potentials. Based on the overall consideration of the low CO tolerance and the high difficulty to remove CO, it must be stated that Pd NPs smaller than 15 nm without strict shape control are not well suited for FAO.
机译：通过使用恒电位双脉冲技术，将钯纳米颗粒（Pd NPs）沉积在高度定向的热解石墨（HOPG）基底上。 NP具有窄的尺寸分布和宽的分散性。颗粒密度约为10（9）cm（-2）。通过调节生长脉冲的持续时间，将Pd NP的平均高度控制在3至50 nm的范围内。在小于14 nm的Pd NP处发生的一氧化碳（CO）剥离主要发生在高于1.1 V的电势下，这比块状Pd和较大的Pd NP的正电势高约0.2 V，这是因为较小的Pd NP往往具有良好的吸收能力有序（111）的小平面以及高比例的边和角原子。在小的Pd NPs上高覆盖的吸附式CO（COads）可以阻止吸附式羟基（OHads）的形成并提高氧化电位。在甲酸氧化过程中，小的Pd纳米颗粒迅速被CO毒化，CO最初是在低电位下通过电化学还原FAO产品的CO2在边缘和角落的原子上形成的。基于对低CO耐受性和去除CO的高难度的总体考虑，必须指出，在没有严格形状控制的情况下小于15 nm的Pd NP不适合粮农组织。

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