Estimation of kinetic and transport parameters by quantitative evaluation of EIS and XPS data

I. Betova, M. Bojinov (Corresponding Author), V. Karastoyanov, Petri Kinnunen, Timo Saario

Research output: Contribution to journalArticleScientificpeer-review

18 Citations (Scopus)

Abstract

The relatively large number of adjustable parameters often precludes the unambiguous interpretation of electrochemical impedance spectra in terms of a unique kinetic model. In the present paper, the possibilities offered by a combination between in situ electrochemical impedance spectroscopic data and ex situ surface analytical information to improve the credibility of the estimates of the kinetic and transport parameters are discussed. Two electrode systems in which passive oxide films are formed—stainless steel in simulated pressurised water reactor coolant and tungsten in sulphate–fluoride solutions—are used as representative examples to demonstrate the different approaches taken to analyse the experimental data in terms of the Mixed-Conduction Model. Ways to extract information on the rate-limiting steps of the process of passive film formation, growth and restructuring by quantitative comparison of the model equations to electrochemical impedance and X-ray photoelectron spectroscopic data are described and the significance of the obtained parameters for the kinetics of the overall process of metal and alloy dissolution in the passive state is discussed.

Original languageEnglish
Pages (from-to)6163-6173
Number of pages11
JournalElectrochimica Acta
Volume55
Issue number21
DOIs
Publication statusPublished - 2010
MoE publication typeA1 Journal article-refereed

Fingerprint

X ray photoelectron spectroscopy
Kinetics
Tungsten
Steel
Pressurized water reactors
Photoelectrons
Coolants
Oxide films
Dissolution
Metals
X rays
Electrodes

Keywords

  • Kinetic model
  • Electrochemical impedance spectroscopy
  • X-ray photoelectron spectroscopy
  • Passive film

Cite this

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title = "Estimation of kinetic and transport parameters by quantitative evaluation of EIS and XPS data",
abstract = "The relatively large number of adjustable parameters often precludes the unambiguous interpretation of electrochemical impedance spectra in terms of a unique kinetic model. In the present paper, the possibilities offered by a combination between in situ electrochemical impedance spectroscopic data and ex situ surface analytical information to improve the credibility of the estimates of the kinetic and transport parameters are discussed. Two electrode systems in which passive oxide films are formed—stainless steel in simulated pressurised water reactor coolant and tungsten in sulphate–fluoride solutions—are used as representative examples to demonstrate the different approaches taken to analyse the experimental data in terms of the Mixed-Conduction Model. Ways to extract information on the rate-limiting steps of the process of passive film formation, growth and restructuring by quantitative comparison of the model equations to electrochemical impedance and X-ray photoelectron spectroscopic data are described and the significance of the obtained parameters for the kinetics of the overall process of metal and alloy dissolution in the passive state is discussed.",
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author = "I. Betova and M. Bojinov and V. Karastoyanov and Petri Kinnunen and Timo Saario",
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year = "2010",
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Estimation of kinetic and transport parameters by quantitative evaluation of EIS and XPS data. / Betova, I.; Bojinov, M. (Corresponding Author); Karastoyanov, V.; Kinnunen, Petri; Saario, Timo.

In: Electrochimica Acta, Vol. 55, No. 21, 2010, p. 6163-6173.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - Estimation of kinetic and transport parameters by quantitative evaluation of EIS and XPS data

AU - Betova, I.

AU - Bojinov, M.

AU - Karastoyanov, V.

AU - Kinnunen, Petri

AU - Saario, Timo

N1 - Project code: 6402

PY - 2010

Y1 - 2010

N2 - The relatively large number of adjustable parameters often precludes the unambiguous interpretation of electrochemical impedance spectra in terms of a unique kinetic model. In the present paper, the possibilities offered by a combination between in situ electrochemical impedance spectroscopic data and ex situ surface analytical information to improve the credibility of the estimates of the kinetic and transport parameters are discussed. Two electrode systems in which passive oxide films are formed—stainless steel in simulated pressurised water reactor coolant and tungsten in sulphate–fluoride solutions—are used as representative examples to demonstrate the different approaches taken to analyse the experimental data in terms of the Mixed-Conduction Model. Ways to extract information on the rate-limiting steps of the process of passive film formation, growth and restructuring by quantitative comparison of the model equations to electrochemical impedance and X-ray photoelectron spectroscopic data are described and the significance of the obtained parameters for the kinetics of the overall process of metal and alloy dissolution in the passive state is discussed.

AB - The relatively large number of adjustable parameters often precludes the unambiguous interpretation of electrochemical impedance spectra in terms of a unique kinetic model. In the present paper, the possibilities offered by a combination between in situ electrochemical impedance spectroscopic data and ex situ surface analytical information to improve the credibility of the estimates of the kinetic and transport parameters are discussed. Two electrode systems in which passive oxide films are formed—stainless steel in simulated pressurised water reactor coolant and tungsten in sulphate–fluoride solutions—are used as representative examples to demonstrate the different approaches taken to analyse the experimental data in terms of the Mixed-Conduction Model. Ways to extract information on the rate-limiting steps of the process of passive film formation, growth and restructuring by quantitative comparison of the model equations to electrochemical impedance and X-ray photoelectron spectroscopic data are described and the significance of the obtained parameters for the kinetics of the overall process of metal and alloy dissolution in the passive state is discussed.

KW - Kinetic model

KW - Electrochemical impedance spectroscopy

KW - X-ray photoelectron spectroscopy

KW - Passive film

U2 - 10.1016/j.electacta.2009.11.100

DO - 10.1016/j.electacta.2009.11.100

M3 - Article

VL - 55

SP - 6163

EP - 6173

JO - Electrochimica Acta

JF - Electrochimica Acta

SN - 0013-4686

IS - 21

ER -