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Enhancement of oxidative electrocatalytic properties of platinum nanoparticles by supporting onto mixed WO3/ZrO2 matrix

机译:通过负载在WO3 / ZrO2混合基质上来增强铂纳米颗粒的氧化电催化性能

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摘要

Nanostructured mixed metal (W, Zr) oxide matrices (in a form of layered intercalated films of WO3 and ZrO2) are considered here for supporting and activating catalytic platinum nanoparticles toward electrooxidation of ethanol. Remarkable increases of electrocatalytic (voltammetric, chronoamperometric) currents measured in 0.5 mol dm(-3) H2SO4 (containing 0.5 mol dm(-3) ethanol) have been observed. Comparison has been made to the behavior of methanol and acetaldehyde under analogous conditions. The enhancement effects are interpreted in terms of specific interactions between platinum nanoparticles and the metal oxide species, high acidity of the mixed oxide sites, as well as high population of surface hydroxyl groups and high mobility of protons existing in close vicinity of Pt catalytic sites. The metal oxide nanostructures are expected to interact competitively (via the surface hydroxyl groups) with adsorbates of the undesirable reaction intermediates, including CO, facilitating their desorption ("third body effect"), or even oxidative removal (e.g., of CO to CO2). The fact that the partially reduced tungsten oxide (HxWO3) component is characterized by fast electron transfers coupled to proton displacements tends to improve the overall charge propagation at the electrocatalytic interface. (C) 2016 Elsevier B.V. All rights reserved.
机译:此处考虑了纳米结构的混合金属(W,Zr)氧化物基质(呈WO3和ZrO2的层状夹层薄膜形式),用于支撑和活化催化性铂纳米颗粒,使其对乙醇进行电氧化。观察到在0.5 mol dm(-3)H2SO4(含0.5 mol dm(-3)乙醇)中测得的电催化(伏安,计时电流)电流显着增加。已经对在类似条件下甲醇和乙醛的行为进行了比较。根据铂纳米颗粒与金属氧化物种类之间的特定相互作用,混合氧化物位点的高酸度,以及在Pt催化位点附近存在的大量表面羟基和质子的高迁移率来解释增强作用。预期金属氧化物纳米结构与不良反应中间体(包括CO)的吸附物竞争性地(通过表面羟基)相互作用,促进其解吸(“第三体效应”),甚至被氧化去除(例如,从CO转化为CO2) 。部分还原的氧化钨(HxWO3)组分的特征是快速电子转移与质子位移耦合,这一事实易于改善电荷在电催化界面处的总体传播。 (C)2016 Elsevier B.V.保留所有权利。

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