Mass spectrometric investigation of ethanol and acetaldehyde adsorbates electrooxidation on Pt electrocatalyst

Delpeuch, Antoine Bach; Chatenet, Marian; Cremers, Carsten; Tübke, T.

doi:10.1016/j.electacta.2014.06.143

Cited by 12 publications

(10 citation statements)

References 22 publications

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“…6 and Table 2). Finally, the lack of m/z = 15 signal close to the hydrogen evolution region rules out any methane formation, as formerly found for palladium [68] or platinum-based electrocatalyst [69,70]. Based on this study we can conclude that the addition of add-atoms can increase a catalytic activity of palladium for electrooxidation of oxygenated fuels.…”

Section: Tablementioning

confidence: 69%

Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels

Serov

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Padilla

et al. 2016

Applied Catalysis B: Environmental

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a b s t r a c tNanostructured palladium-copper electrocatalysts with Pd:Cu ratios of 1:3, 1:1, and 3:1 were synthesized using a Sacrificial Support Method (SSM) in combination with the thermal reduction of metal precursors. The materials were comprehensively characterized by X-ray diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS), Scanning and Transmission Electron Microscopy (SEM and TEM), surface area measurements (Brunauer-Emmett-Teller, BET) and Differential Electrochemical Mass Spectroscopy (DEMS). The SSM method enables the preparation of nano-sized unsupported Pd-Cu catalysts with uniformlydistributed particles and high surface area, in the range of 40 m 2 g catalyst −1 . Their catalytic activity for the electrooxidation of several alcohols (methanol, ethanol, ethylene glycol and glycerol) was investigated in alkaline media. In situ Infrared Reflection Adsorption Spectroscopy (IRRAS) and Density Functional Theory (DFT) calculations were used in order to understand the mechanism of the various alcohols electrooxidation reactions.

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Section: Tablementioning

confidence: 69%

Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels

Serov

Asset

Padilla

et al. 2016

Applied Catalysis B: Environmental

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“…This slightly better ethanol oxidation initiation on the bi‐ and tri‐metallic electrocatalysts may be attributed to an enhancement of ethanol adsorption at low potential possibly followed by a better dehydrogenation into acetaldehyde. Based on the knowledge that ethanol adsorption on Pt/C surface is inhibited by the presence of H ad ‐species 20, 33, 34, a modification of Pt electronic structure, as mentioned in the CO‐stripping section, induced by the presence of rhodium, and possibly tin, in the lattice could reduce Pt hydrogen adsorption affinity. The dehydrogenation of the platinum surface by rhodium in Pt‐Rh/C electrocatalysts was already mentioned in 15, 16, 18, 20.…”

Section: Resultsmentioning

confidence: 99%

Influence of the Temperature for the Ethanol Oxidation Reaction (EOR) on Pt/C, Pt‐Rh/C and Pt‐Rh‐SnO₂/C

et al. 2015

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The electrocatalytic activity of Pt/C, Pt-Rh/C and Pt-RhSnO 2 /C electrocatalysts toward the ethanol oxidation reaction (EOR) was investigated in a three-electrode assembly at 25°C, 40°C and 70°C in acidic medium. The 10 wt.% electrocatalysts were prepared with a modified polyol method and physically characterized by both X-Ray Diffraction (XRD) and Transmission Electron Microscopy (TEM). The CO-stripping study revealed that CO ad oxidation initiates at lower potential on Pt-Rh/C and Pt-Rh-SnO 2 /C than on Pt/C and shifts negatively when the temperature increases. The positive effect of the temperature is maintained for the EOR: the three electrocatalysts exhibit a higher activity and a negative shift of the EOR wave at higher temperature. Pt-Rh-SnO 2 /C demonstrates the lowest EOR onset potential of the three electrocatalysts. The steady-state Tafel slopes and apparent activation energies E a were determined in 0.5 M H 2 SO 4 + 0.1 M EtOH between E = 0.4 and 0.7 V vs. RHE in the temperature range 25-70°C. The results show rather comparable rate determining steps (rds) for the ethanol electrooxidation on Pt/C and Pt-Rh/C in the ranges of potential and temperature studied. The EOR on Pt-Rh-SnO 2 /C seems less influenced by the potential than on Pt/C and Pt-Rh/C electrocatalysts, but is more temperature sensitive.

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“…Indeed, ethanol adsorbate stripping studies have shown that the C-C bond breaking can occur at potentials as low as E = 0.05 V vs. RHE on Pt-based carbonsupported electrocatalysts. 24,31 As such, spending a longer time between E = 0.07 (CV initial potential) and E = 0.6 V vs. RHE (CO 2 generation initiation) during a slow-scan CV was expected to enhance ethanol dissociative adsorption and boost the amount of CO-like adsorbates at the electrocatalyst surface at the beginning of the CO 2 generation. At E Z 0.7 V vs. RHE, the degree at which the CCE decreases against the potential is rather different depending on the sweep rate: the CCE at E = 0.7 V vs. RHE is twice lower at n = 2 mV s À1 (CCE = 0.09) than at n = 10 mV s À1 (CCE = 0.18).…”

Section: Effect Of the Scan Ratementioning

confidence: 99%

The influence of mass-transport conditions on the ethanol oxidation reaction (EOR) mechanism of Pt/C electrocatalysts

Delpeuch

Jacquot

Chatenet

et al. 2016

Phys. Chem. Chem. Phys.

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This study aims to provide further understanding of the influence of different parameters that control mass-transport (the revolution rate of the rotating disk electrode and the potential scan rate) on the ethanol oxidation reaction (EOR). The experiments were conducted on a home-made carbon-supported 20 wt% Pt/C electrocatalyst, synthesized using a modified polyol method, and characterized in terms of physicochemical properties by thermogravimetric analysis (TGA), powder X-ray diffraction (XRD) and transmission electron microscopy (TEM). The EOR at the thin active layer of this electrocatalyst was characterized using both differential electrochemical mass spectrometry (DEMS) in a flow cell configuration and the rotating disc electrode (RDE). The results demonstrate that operating under stationary conditions (low scan rate and high RDE speed) hinders complete ethanol electrooxidation into CO and favors the poisoning of the electrocatalyst surface by hydroxide and strong ethanol adsorbates. As such, the EOR appears to be more efficient and faster under dynamic conditions than in near steady-state.

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Mass spectrometric investigation of ethanol and acetaldehyde adsorbates electrooxidation on Pt electrocatalyst

Cited by 12 publications

References 22 publications

Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels

Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels

Influence of the Temperature for the Ethanol Oxidation Reaction (EOR) on Pt/C, Pt‐Rh/C and Pt‐Rh‐SnO₂/C

The influence of mass-transport conditions on the ethanol oxidation reaction (EOR) mechanism of Pt/C electrocatalysts

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Mass spectrometric investigation of ethanol and acetaldehyde adsorbates electrooxidation on Pt electrocatalyst

Cited by 12 publications

References 22 publications

Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels

Highly-active Pd–Cu electrocatalysts for oxidation of ubiquitous oxygenated fuels

Influence of the Temperature for the Ethanol Oxidation Reaction (EOR) on Pt/C, Pt‐Rh/C and Pt‐Rh‐SnO2/C

The influence of mass-transport conditions on the ethanol oxidation reaction (EOR) mechanism of Pt/C electrocatalysts

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Influence of the Temperature for the Ethanol Oxidation Reaction (EOR) on Pt/C, Pt‐Rh/C and Pt‐Rh‐SnO₂/C