Journal Article FZJ-2021-01348

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Impedance Response of Electrochemical Interfaces: Part II – Chemisorption

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2021
IOP Publ. Bristol

Journal of physics / Condensed matter 33, 164003 () [10.1088/1361-648X/abef9d]

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Abstract: Physical modelling helps to acquire fundamental insights from experimental data when electrochemical impedance spectroscopy is employed for mechanistic understandings of electrocatalytic reactions. Herein, we report an analytical solution for chemisorption impedance from a consistent treatment of ion transport in the solution and electron transfer on the surface. Our formulation avoids both a priori decoupling of double-layer charging and electron transfer reaction, and a strict separation of double-layer charging and ion transport. Ion transport in the entire solution region is described by the Poisson-Nernst-Planck theory and electron transfer kinetics on the electrode surface by the Frumkin-Butler-Volmer theory. Surface dipoles caused by partially charged chemisorbates are considered. The classical Frumkin-Melik-Gaikazyan model for chemisorption is retrieved as a limiting case. The obtained formula is validated using experimental data of hydrogen adsorption at Pt(111). Characteristic frequencies and asymptotic behaviors of chemisorption impedance are analyzed.

Classification:

Contributing Institute(s):
  1. IEK-13 (IEK-13)
Research Program(s):
  1. 122 - Elektrochemische Energiespeicherung (POF4-122) (POF4-122)

Appears in the scientific report 2021
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Medline ; Creative Commons Attribution CC BY 4.0 ; OpenAccess ; Clarivate Analytics Master Journal List ; Current Contents - Electronics and Telecommunications Collection ; Current Contents - Physical, Chemical and Earth Sciences ; Essential Science Indicators ; IF < 5 ; JCR ; National-Konsortium ; NationallizenzNationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection
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 Record created 2021-03-15, last modified 2024-07-12


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