Electrochemical and adsorption behaviour of ethylene glycol and its oxidative derivatives at platinum electrodes

Horányi, G.; Kazarinov, V.E.; Vassiliev, Yu.B.; Андреев, В. Н.

doi:10.1016/s0022-0728(83)80071-0

Cited by 63 publications

(53 citation statements)

References 9 publications

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“…17 It was also proposed that that the adsorption and oxidation of OA might be independent processes. 51,52 These two findings together with the fact that the last two steps in the calculated OA oxidation mechanism are exothermic (Figure 10), confirm that the rate limiting step on Pt(111) surface is the first e-transfer from adsorbed OA (or its ions) to either the metal surface or adsorbed OH.…”

Section: 14mentioning

confidence: 57%

Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study

Perry

Babanova

Matanović

et al. 2016

J. Electrochem. Soc.

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In this study we combined experimental approaches and density functional theory to evaluate novel platinum-based materials as electrocatalysts for oxalic acid oxidation. Several Pt alloys, PtSn (1:1), PtSn (19:1), PtRu (1:4), PtRuSn (5:4:1), and PtRhSn (3:1:4), were synthetized using sacrificial support method and tested for oxidation of oxalic acid at pH 4. It was shown that PtSn (1:1) and PtRu (1:4) have higher mass activity relative to Pt. These two materials along with Pt and one of the least active alloys, PtSn (19:1), were further analyzed for the oxidation of oxalic acid at different pHs. The results show that all samples tested followed an identical trend of decreased onset potential with increased pH and increased catalytic activity with decreased pH. Density functional theory was further utilized to gain a fundamental knowledge about the mechanism of oxalic acid oxidation on Pt, PtSn (1:1), and PtRu (1:4). The results of the calculations along with the experimentally observed dependence of generated currents on the oxalic acid concentration indicate that the mechanism of oxalic acid oxidation on Pt proceeds without the participation of surface oxidizing species, while on Pt alloys it involves their participation.

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Section: 14mentioning

confidence: 57%

Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study

Perry

Babanova

Matanović

et al. 2016

J. Electrochem. Soc.

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Section: 4-9mentioning

confidence: 99%

“…[18][19][20][21][22][23][24] The adsorbed CO and oxidation by-products block the Pt active sites, which results in a performance loss for both ORR and HOR.…”

Section: 4-9mentioning

confidence: 99%

“…The electrochemical oxidation of EG on the Pt/C catalyst in acid media has attracted interest because of its potential application as a fuel for direct alcohol fuel cells. [17][18][19][20][21][22][23][24][25] In addition to the complete oxidation product CO 2 , the electro-oxidation of EG produces numerous stable, adsorbed species and partly oxidized by-products such as adsorbed CO, glycolic acid, oxalic acid, glycolaldehyde, glyoxal, glyoxylic acid, formaldehyde, and formic acid. [18][19][20][21][22][23][24] The adsorbed CO and oxidation by-products block the Pt active sites, which results in a performance loss for both ORR and HOR.…”

mentioning

confidence: 99%

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Effects of Ethylene Glycol and Caprolactam on the ORR and HOR Performances of Pt/C Catalysts

Zhai

St‐Pierre

2016

J. Electrochem. Soc.

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Ethylene glycol (EG) and caprolactam are two representative contaminant species either present in the fuel cell system or released by fuel cell system materials. The contamination effects of EG and caprolactam on the electro-catalytic performances of a Pt/C catalyst toward the oxygen reduction reaction (ORR) and hydrogen oxidation reaction (HOR) were investigated in acid media using the rotating ring/disk electrode (RRDE) technique. The Pt surface coverage increased with EG and caprolactam concentrations. The H 2 O 2 yield also significantly increased because of the effects of the two contaminants. The EG-and caprolactam-derived adsorbates reduce the ORR and HOR rates and modify the rate-determining step (change in Tafel Considering the inevitable depletion of conventional fossil fuels and the release of greenhouse gases into the Earth's atmosphere, it is necessary to look for renewable and clean energy supplies. Proton exchange membrane fuel cells (PEMFCs) are promising as clean energy sources for future automotive applications. However, the performance and durability of PEMFCs can be significantly decreased by the presence of contaminants in air and hydrogen or released by fuel cell system materials.1-3 Such species may adsorb on the Pt catalyst, penetrate into the ionomer and membrane, or compete with the main reactions, which decreases the active surface area, ionic conductivity of the catalyst layer and membrane, and cell performance. 2,4-9In addition, H 2 O 2 , which is a side product of the oxygen reduction reaction (ORR), and its associated yield often increases in the presence of organic contaminants such as acetylene, acetonitrile, propene, naphthalene, and methyl methacrylate. 10-13 A larger H 2 O 2 generation rate exerts an undetermined effect on the performance and durability of PEMFCs. The formation of H 2 O 2 has been linked to the radical attack decomposition of the Nafion ionomer, which is accelerated by the presence of Fe 2+ and Cu 2+ ions. 14,15 The Nafion ionomer is used as an electrolyte membrane and added to the catalyst layer to exploit its binding property and improve catalyst utilization. Consequently, the decomposition of the Nafion ionomer is a significant risk to the PEMFC performance and durability. Therefore, it is necessary to investigate the ORR, hydrogen oxidation reaction (HOR), and H 2 O 2 yield in the presence of contaminants to understand their effects on PEMFCs.This study was initiated with a list of system contaminants identified by the National Renewable Energy Laboratory (NREL).16 These were separated into 2 classes: linear and more structurally complex molecules including cyclic molecules (ring-shaped). One molecule of each class was chosen for these initial studies. Ethylene glycol (EG) is interesting because it is widely used as a coolant, antifreeze agent, and de-icing solution. De-icing of airport runways and airplanes is the primary source of EG in the environment. EG is also dispersed in the environment by the disposal of products that contain it. In addition, 1,6...

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“…Several studies have been carried out on the electrochemistry of glyoxylic acid (GA) on polycrystalline surfaces of different electrode materials such as vitreous carbon 6 , gold 7 ,palladium 8 and platinum [9][10][11] . The effect of the crystallographic orientation is fundamental from an electrocatalytic point of view, and although GA oxidation was found to be structure sensitive on Pt 11 , in situ studies about GA adsorption and reactivity at well-defined metal/solution interfaces are rather scarce 7,11 .…”

Section: Introductionmentioning

confidence: 99%

Weakening the C C bond: On the behavior of glyoxylic acid on Pt(111) and its vicinal surfaces

Martínez‐Hincapié

Arán‐Ais

Feliu

2016

Journal of Electroanalytical Chemistry

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Electrochemical and adsorption behaviour of ethylene glycol and its oxidative derivatives at platinum electrodes

Cited by 63 publications

References 9 publications

Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study

Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study

Effects of Ethylene Glycol and Caprolactam on the ORR and HOR Performances of Pt/C Catalysts

Weakening the C C bond: On the behavior of glyoxylic acid on Pt(111) and its vicinal surfaces

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