On the impedance response of reactions influenced by mass transfer

Tribollet, Bernard; Vivier, Vincent; Orazem, Mark E.

doi:10.1134/s1023193517090142

Cited by 18 publications

(16 citation statements)

References 31 publications

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“…At a potential of −0.5 V, the charge-transfer resistance is very large, as would be expected for an irreversible reaction. The potential of −3.0 V represents the mass-transfer limit, where, as discussed in Tran et al, 41 the charge-transfer resistance approaches a finite value, and the diffusion impedance becomes very large.…”

Section: Journal Of Thementioning

confidence: 99%

The Influence of Homogeneous Reactions on the Impedance Response of a Rotating Disk Electrode

Harding

Tribollet

Vivier

et al. 2017

J. Electrochem. Soc.

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A mathematical model was developed for the impedance response associated with coupled homogeneous chemical and heterogeneous electrochemical reactions. The model includes a homogeneous reaction in the electrolyte in which species AB reacts reversibly to form A − and B + and B + reacts electrochemically on a rotating disk electrode to produce B. The resulting diffusion impedance has two asymmetric capacitive loops, one associated with convective diffusion and the other with the homogeneous reaction. For an infinitely fast homogeneous reaction, the system is shown to behave as though AB is the electroactive species. A modified Gerischer impedance was found to provide a good fit to the simulated data. The coupling of homogeneous chemical reactions and heterogeneous electrochemical reactions has drawn substantial interest over the past 80 years. Koutecky and Levich 1-3 developed a steady-state model for a homogeneous reaction coupled with an electrochemical reaction on a rotating disk electrode. The homogenous reaction was assumed to follow linear kinetics, all diffusion coefficients were assumed to be equal, and the Schmidt number was assumed infinite. Koutecky and Levich defined a characteristic dimension for the homogeneous reaction, termed the thickness of the kinetic layer and represented bywhere α = k f +k b , k f and k b are respectively the forward and backward rate constants of the homogeneous reaction, and D is the diffusion coefficient. Bossche et al. 4 describe finite-difference calculations under assumption of a steady state for an electrochemical system controlled by diffusion, migration, convection, and nonlinear homogeneous reaction kinetics. Their convection term used a three-term expansion appropriate for positions close to the electrode surface.5 Deslouis et al. 6 used a submerged impinging jet cell to measure interfacial pH during the reduction of dissolved oxygen in the presence of carbonate. Their analysis considered the homogeneous reaction involving water and hydroxide, bicarbonate, and carbonate ions. Remita et al. 7 have shown that, for a deaerated aqueous electrolyte containing dissolved carbon dioxide, hydrogen evolution is enhanced by the homogeneous dissociation of CO 2 . Tran et al. 8 demonstrated that homogeneous dissociation of acetic acid enhances cathodic reduction of hydronium ions. Smith 9,10 used AC Polarography to study different linear firstorder homogeneous reaction mechanisms, including preceding, following, and catalytic chemical reactions coupled with electrochemical reactions. Jurczakowski and Polczynski 11 developed an AC model with coupled homogenous and heterogeneous reactions accounting for cases where diffusion coefficients are not considered to be equal. The above mechanisms assumed simplified homogeneous reactions, with a maximum of two species considered.Using chronopotentiometry, Delahay and Berzins 12 showed that cadmium cyanide complexes undergo a dissociation before electrore- * Electrochemical Society Student Member. * * Electrochemical Society Fellow. * * * ...

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Section: Journal Of Thementioning

confidence: 99%

The Influence of Homogeneous Reactions on the Impedance Response of a Rotating Disk Electrode

Harding

Tribollet

Vivier

et al. 2017

J. Electrochem. Soc.

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“…To study the electrical behaviour of the samples, Electrochemical Impedance Spectroscopy (EIS) measurements using ferro/ferricyanide species as redox probe, were performed. Because the ferro/ferricyanide electron transfer reaction [Fe(CN) 6 ] 4− aq → [Fe(CN) 6 ] 3− aq + (e − ) has a well-know kinetic behaviour, changes in the electrochemical response may be attributed to modifications in the electrode conductive properties 53 . Figure 8a,b show complex plane representations (Nyquist diagrams) at different scales of the impedance response for the substrate, substrate/GO, substrate/Py NWs and substrate/Py NWs/GO composite electrodes in 10 mM [Fe(CN) 6 ] 4− /[Fe(CN) 6 ] 3− solutions.…”

Section: Resultsmentioning

confidence: 99%

Permalloy nanowires/graphene oxide composite with enhanced conductive properties

Jaimes

Márquez

Ovalle

et al. 2020

Sci Rep

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carbon-metal-based composites arise as advanced materials in the frontiers with nanotechnology, since the properties inherent to each component are multiplexed into a new material with potential applications. in this work, a novel composite consisting of randomly oriented permalloy nanowires (py nWs) intercalated among the sheets of multi-layered graphene oxide (Go) was performed. py nWs were synthesized by electrodeposition inside mesoporous alumina templates, while Go sheets were separated by means of sonication. Sequential deposition steps of Py NWs and GO flakes allowed to reach a reproducible and stable graphene oxide-based magnetic assembly. Microscopic and spectroscopic results indicate that py nWs are anchored on the surface as well as around the edges of the multi-layered Go, promoted by the presence of chemical groups, while magnetic characterization affords additional support to our hypothesis regarding the parallel orientation of the Py NWs with respect to the GO film, and also hints the parallel stacking of GO sheets with respect to the substrate. the most striking result remains on the electrochemical performance achieved by the composite that evidences an enhanced conductive behaviour compared to a standard electrode. Such effect provides an approach to the development of permalloy nanowires/graphene oxide-based electrodes as attractive candidates for molecular sensing devices. Composite materials arise as versatile candidates that could be designed to satisfy diverse technological applications due to their multifunctional behaviour. Since composites are obtained by combining two or more materials that have different attributes, such assembly provides to the composite of unique properties. In fact, several examples exist that have demonstrated the industrial development behind their production, being the concrete a well-known composite, where its strength under compression is improved by adding metal rods, wires, mesh or cables in order to create reinforced concrete. Most of the current composites have been made by carbon allotropes 1, 2. In particular, when graphene is combined with the metallic copper, a new material around 500 times stronger than copper is achieved 3. Likewise, composites constituted by graphene and nickel yield a strength larger than 180 times of nickel 4. A soft Ni-rich ferromagnet 5, 6 , that is widely employed as a magnetic core material in diverse technological applications, such as magnetic recording heads 7-9 , microinductors and magnetoresistive random access memories (MRAM) 10, 11 , is the so called permalloy (Py), an alloy with about 20% iron and 80% nickel content. On the one hand, bulk Py exhibits large magnetic permeability, enhanced sensitivity in sensing devices 12 , as well as low coercivity and remanence, of interest in magnetic shielding 13. In addition, it is a material with nearly zero magnetostriction, an attribute that promotes an easier integration in different devices 13. Besides, the high Ni content provides an excellent corrosion resistance to the alloy...

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“…Where i k is the kinetic current (A/cm 2 ), k is the kinetic constant (cm/s), c ox (∞) is the bulk concentration and b c is the cathodic Tafel slope (b c =αnF/RT) [31]. For instance, the charge transfer region at a scan rate of 10 mV/s starts from -1.41 to -0.68 V (730 mV), whereas at 0.5 mV/s, it goes from -1.53 to -1.2 V (330 mV).…”

Section: Influence Of the Potential Scan Rate On Cathodic Polarizatiomentioning

confidence: 99%

“…Generally, in the case of faradaic reactions influenced by transport of the reacting species to the electrode surface, straight lines are obtained [31,34,35]. Therefore, determination of the electron number involved in the reaction can be determined from the slopes values.…”

Section: Cathodic Polarization Curves On Al Pre-treated At -2 V Oxidmentioning

confidence: 99%

“…From Figure 5b, one can see that the fitted lines obtained for Al pre-treated at -2 V yield non-zero intercept unlike the ones drawn for Pt. Hence, the reduction of 3 6 Fe(CN)  ions is a mixed kinetic-diffusion process and subsequently obeyed the Koutecky-Levich equation [31,33] given by equation (11):…”

Section: Cathodic Polarization Curves On Al Pre-treated At -2 V Oxidmentioning

confidence: 99%

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Cathodic behavior of pure Al in sulfate media

2019

Int. J. Corros. Scale Inhib.

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The cathodic behavior of Al in 0.5 M Na 2 SO 4 solution was studied by electrochemical methods. It was shown that the reduction of 3 6 Fe(CN)  was difficult when an oxide layer was formed on the electrode surface during 1 h immersion in 0.5 M Na 2 SO 4 solution due to the poor ionic and electronic conductivities of Al hydroxides. This reaction required a high cathodic overpotential on Al surface pre-treated at-2 V/SCE Al and was kinetically more difficult in comparison to platinum. Rotating disk electrode measurements showed that oxygen reduction reaction (ORR) was controlled by kinetics on both Al pre-treated at-2 V/SCE and oxidized Al cathodic dissolution was controlled by the supply of OHions through H 2 evolution and by ORR on both oxidized Al electrode and the Al surface pretreated at-2 V/SCE. Polarization curves obtained at different pH values showed that no dissolution behavior was observed at pH 5, whereas in neutral and alkaline solutions, OHions production induced chemical dissolution of the hydroxide layer. In O 2 supersaturated solution, it was shown that ORR kinetics were slightly favored.

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On the impedance response of reactions influenced by mass transfer

Cited by 18 publications

References 31 publications

The Influence of Homogeneous Reactions on the Impedance Response of a Rotating Disk Electrode

The Influence of Homogeneous Reactions on the Impedance Response of a Rotating Disk Electrode

Permalloy nanowires/graphene oxide composite with enhanced conductive properties

Cathodic behavior of pure Al in sulfate media

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