Identification of the surface species in electrochemical promotion: ethylene oxidation over a Pt/YSZ catalyst.

Published on Oct 6, 2021in Physical Chemistry Chemical Physics3.676
· DOI :10.1039/D1CP02757C
Arafat Toghan10
Estimated H-index: 10
(Leibniz University of Hanover),
Mark T. Greiner33
Estimated H-index: 33
(MPG: Max Planck Society)
+ 1 AuthorsRonald Imbihl52
Estimated H-index: 52
(Leibniz University of Hanover)
Sources
Abstract
The electrochemical promotion of the C2H4 + O2 total oxidation reaction over a Pt catalyst, interfaced to yttrium stabilized zirconia (YSZ), has been studied at 0.25 mbar and T = 650 K using near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) as an in situ method. The electrochemical promoter effect is linked to the presence of a several layers thick graphitic overlayer that forms on the Pt surface in the presence of C2H4. Our NAP-XPS investigation reveals that electrochemical pumping of the Pt/YSZ catalyst, using a positive potential, leads to the spillover of oxygen surface species from the YSZ support onto the surface of the Pt electrode. Based on the XP spectra, the spillover species on Pt is identical to oxygen chemisorbed from the gas-phase.
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References41
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#1Yasmine M. Hajar (U of O: University of Ottawa)H-Index: 5
#2Laureline Treps (École normale supérieure de Lyon)H-Index: 2
Last. Stephan N. Steinmann (École normale supérieure de Lyon)H-Index: 31
view all 5 authors...
In electrochemical promotion of catalysis (EPOC), the adsorption energies of reactants and products, and subsequently the overall reaction catalytic rate are modified by applying an electrochemical potential to the catalyst. In this paper, the oxidation of ethylene on ruthenium oxide was studied by experiments and theoretical modeling in order to elucidate the atomistic origin of EPOC. The experimental results have shown an increase in the reaction rate under negative and positive polarization. ...
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: Chasing down the active state: Near-ambient-pressure X-ray photoelectron spectroscopy was used to study the surface of a Pt electrode during the oxygen evolution reaction (OER). A hydrated Pt metal phase with dissolved oxygen in the near-surface region is OER-active and considered to be the precursor of the analytically detected PtO2 , which is in fact the deactivation product of the electrode.
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#1Chunjuan Zhang (UMD: University of Maryland, College Park)H-Index: 10
#2Yi YuH-Index: 15
Last. Bryan W. EichhornH-Index: 40
view all 15 authors...
Through the use of ambient pressure X-ray photoelectron spectroscopy (APXPS) and a single-sided solid oxide electrochemical cell (SOC), we have studied the mechanism of electrocatalytic splitting of water (H2O + 2e– → H2 + O2–) and electro-oxidation of hydrogen (H2 + O2– → H2O + 2e–) at ∼700 °C in 0.5 Torr of H2/H2O on ceria (CeO2–x) electrodes. The experiments reveal a transient build-up of surface intermediates (OH– and Ce3+) and show the separation of charge at the gas–solid interface exclusi...
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#1Philippe Vernoux (UCBL: Claude Bernard University Lyon 1)H-Index: 30
#2Leonardo LizarragaH-Index: 11
Last. Elena A. BaranovaH-Index: 27
view all 11 authors...
Philippe Vernoux,*,† Leonardo Lizarraga,† Mihalis N. Tsampas,† Foteini M. Sapountzi,† Antonio De Lucas-Consuegra,‡ Jose-Luis Valverde,‡ Stamatios Souentie, Costas G. Vayenas, Dimitris Tsiplakides, Stella Balomenou, and Elena A. Baranova †Universite de Lyon, Institut de Recherches sur la Catalyse et l’Environnement de Lyon, UMR 5256, CNRS, Universite Claude Bernard Lyon 1, 2 Avenue A. Einstein, 69626 Villeurbanne, France ‡Departamento de Ingenieria Quimica, Facultad de Ciencias y Tecnologias Quim...
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#1S. Peng-ont (Chula: Chulalongkorn University)H-Index: 3
#2Stamatios Souentie (University of Patras)H-Index: 14
Last. C.G. Vayenas (University of Patras)H-Index: 35
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The electrochemical promotion of C2H4 oxidation reaction has been investigated under various feed gas compositions and temperatures over a Pt/Y2O3-stabilized ZrO2 catalyst electrode. It was found that under oxidizing conditions the reaction exhibits electrophobic behavior, i.e. the catalytic rate of CO2 formation increases with anodic potential application, while it shifts to electrophilic behaviour, i.e. the rate increases with cathodic potential application, under near stoichiometric feed cond...
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#1Arafat Toghan (Leibniz University of Hanover)H-Index: 10
#2Rosa Arrigo (MPG: Max Planck Society)H-Index: 27
Last. Ronald Imbihl (Leibniz University of Hanover)H-Index: 52
view all 4 authors...
The electrochemical promotion of the C2H4 + O2 reaction over a bimetallic Pt/Ag catalyst (Pt:Ag ratio ≈ 1.5) interfaced to yttrium stabilized zirconia (YSZ) has been studied at 0.25 mbar and T = 650 K using X-ray photoelectron spectroscopy as in situ method. Applying a positive potential of 2V causes a relative rate increase in the CO2 production up to 120%; the electrocatalytic promotion effect is non-Faradaic (≈ 2). An electrochemical promotion is found to occur only at high enough p(C2H4) w...
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#1H. Pöpke (University of Giessen)H-Index: 6
#2Eva Mutoro (University of Giessen)H-Index: 20
Last. Jürgen Janek (University of Giessen)H-Index: 79
view all 8 authors...
The existence and role of platinum oxide in the solid state electrode system Pt(O2)/yttria-stabilized zirconia is discussed. Covering and porous model-type Pt film electrodes on YSZ single crystals are investigated by cyclic voltammetry, electrochemical impedance spectroscopy, and in situ scanning photoelectron microscopy. The formation of Pt oxide and its amount strongly depend on the experimental conditions, such as temperature, oxygen partial pressure, and oxygen flux towards the electrode du...
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#1Eva Mutoro (University of Giessen)H-Index: 20
#2Christian Hellwig (DLR: German Aerospace Center)H-Index: 2
Last. Jürgen Janek (University of Giessen)H-Index: 79
view all 6 authors...
Electrochemically induced oxygen spillover and diffusion in the Pt(O2)|YSZ system is investigated in a combined experimental and theoretical study. The spreading of spillover oxygen is imaged by photoelectron emission microscopy (PEEM) on dense and epitaxial Pt(111) thin film electrodes prepared by pulsed laser deposition (PLD). Two different models are used to obtain surface diffusion coefficients from the experimental data, (i) an analytical solution of Fick's 2nd law of diffusion, and (ii) a ...
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#1Ronald Imbihl (Leibniz University of Hanover)H-Index: 52
#2Arafat Toghan (Leibniz University of Hanover)H-Index: 10
Source
#1Constantinos G. Vayenas (University of Patras)H-Index: 32
#2Philippe Vernoux (UCBL: Claude Bernard University Lyon 1)H-Index: 30
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