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Electrochemical designing of Au/Pt core shell nanoparticles as nanostructured catalyst with tunable activity for oxygen reduction

机译:具有可调氧还原活性的Au / Pt核壳纳米粒子的电化学设计

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摘要

Au/Pt core shell nanoparticles (NPs) have been prepared via a layer-by-layer growth of Pt layers on An NPs using underpotential deposition (UPD) redox replacement technique. A single UPD Cu monolayer replacement with Pt(11) yielded a uniform Pt film on Au NPs, and the shell thickness can be tuned by controlling the number of UPD redox replacement cycles. Oxygen reduction reaction (ORR) in air-saturated 0.1 M H2SO4 was used to investigate the electrocatalytic behavior of the as-prepared core shell NPs. Cyclic voltammograms of ORR show that the peak potentials shift positively from 0.32 V to 0.48 V with the number of Pt layers increasing from one to five, suggesting the electrocatalytic activity increases with increasing the thickness of Pt shell. The increase in electrocatalytic activity may originate mostly from the large decrease of electronic influence of Au cores on surface Pt atoms. Rotating ring-disk electrode voltammetry and rotating disk electrode voltammetry demonstrate that ORR is mainly a four-electron reduction on the as-prepared modified electrode with 5 Pt layers and first charge transfer is the rate-determining step.
机译:Au / Pt核壳纳米粒子(NPs)已通过使用电位不足沉积(UPD)氧化还原置换技术在NPs上逐层生长Pt层而制备。用Pt(11)进行单个UPD Cu单层替换会在Au NP上产生均匀的Pt膜,并且可以通过控制UPD氧化还原替换循环的次数来调整壳的厚度。空气饱和的0.1 M H2SO4中的氧还原反应(ORR)用于研究制备的核壳NP的电催化行为。 ORR的循环伏安图表明,随着Pt层数从1增加到5,峰值电势从0.32 V正移至0.48 V,这表明电催化活性随Pt壳厚度的增加而增加。电催化活性的提高可能主要来自Au核对表面Pt原子的电子影响的大幅降低。旋转环盘电极伏安法和旋转盘电极伏安法表明,ORR主要是在制备的具有5个Pt层的修饰电极上进行四电子还原,并且首先进行电荷转移是速率确定步骤。

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