Electrocatalytic oxidation of ethylene glycol (EG) on supported Pt and Au catalysts in alkaline media: Reaction pathway investigation in three-electrode cell and fuel cell reactors

草酸 乙醇酸 乙二醇 甲酸 催化作用 过电位 阳极 化学 无机化学 铂金 膜电极组件 电化学 核化学 电极 有机化学 物理化学 细菌 乳酸 生物 遗传学
作者
Le Xin,Zhiyong Zhang,Ji Qi,David J. Chadderdon,Wenzhen Li
出处
期刊:Applied Catalysis B-environmental [Elsevier BV]
卷期号:125: 85-94 被引量:134
标识
DOI:10.1016/j.apcatb.2012.05.024
摘要

Carbon supported Pt and Au nanoparticles with small sizes (2.4 nm for Pt/C, and 3.5 nm for Au/C) and narrow size distributions were prepared though a modified solution-phase reduction method, and served as the working catalysts for an investigation of electrocatalytic oxidation of EG in alkaline media. Our three-electrode cell with an on-line sample collection system showed that with applied potential increasing, glycolic acid, oxalic acid and formic acid were sequentially produced from EG oxidation on Pt/C, while only glycolic acid and formic acid were detected on Au/C. Oxalic acid is a fairly stable product, and Pt/C is inactive to its further oxidation reaction. On Au/C, glycolic acid is the primary product, and no oxalic acid was found at specified test conditions. We clarified that formic acid was produced preferably from direct CC bond cleavage of EG not glycolic acid on both Pt/C and Au/C catalysts. The single anion exchange membrane-direct EG fuel cell (AEM-DEGFC) with Pt/C and Au/C anode catalysts showed consistent results with the three-electrode cell tests. The AEM-DEGC with Pt/C anode catalyst demonstrated a peak power density of 71.0 mW cm−2, which is much higher than that with the Au/C (only 7.3 mW cm−2) at 50 °C. With the fuel cell operation voltage decreasing (anode overpotential increasing), deeper-oxidized products oxalic acid and formic acid were generated in the Pt/C anode AEM-DEGFC with higher selectivity. No formic acid was detected in the Pt anode AEM-DEGFC when glycolic acid was employed as fuel. On Au/C anode catalyst, very high selectivity to glycolic acid (>98%) was achieved. The AEM-DEGFC results confirmed the EG electro-oxidation pathways proposed by using an on-line sample collection system.
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