Electrochemical impedance spectroscopy: the journey to physical understanding
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FEATURE ARTICLE
Electrochemical impedance spectroscopy: the journey to physical understanding Mark E. Orazem 1 Received: 10 June 2020 / Revised: 10 June 2020 / Accepted: 11 June 2020 # Springer-Verlag GmbH Germany, part of Springer Nature 2020
When I was young, I used to devour magazines such as Popular Science or Popular Mechanics that periodically offered fanciful visions of the future. I recall reading about flying cars in every garage and tiered moving sidewalks that would speed pedestrians to their destinations at velocities of up to 60 miles per hour. I do not imagine that my vision of the future would be any more reliable. For the present essay, I prefer to describe not the future of electrochemical impedance spectroscopy, but what I want the future to be. The history of electrochemical impedance spectroscopy has been addressed by a number of authors. Macdonald [1] argued that the history of electrochemical impedance spectroscopy rightfully begins with the linear systems theory foundation laid by Heaviside [2, 3] in the late nineteenth century. Gabrielli [4] taught that the field begins in 1869 with the work of Kohlrausch [5], who used impedance spectroscopy as a way to measure electrolyte resistance with greater accuracy. Bernard Tribollet and I [6] suggested that the field began in 1894 with the work of Nernst [7], who used impedance spectroscopy to measure dielectric constants of electrolytes. In the early days, much effort was made to establish the science of the electrochemical impedance spectroscopy technique. For example, the influence of mass transfer on impedance was explored by Warburg [8, 9] at the end of the nineteenth century. In 1947, Randles [10] presented a model for an electrochemical reaction influenced by mass transfer that extended the work of Warburg. In 1951, Gerischer [11] presented a model for the impedance of a heterogeneous reactions influenced by mass transfer and homogeneous reactions. Gerischer and Mehl [12] developed a model for the impedance response that, by accounting for the coupling of Volmer and Heyrovsky steps in the hydrogen evolution reaction, * Mark E. Orazem [email protected] 1
Department of Chemical Engineering, University of Florida, Gainesville, FL 32611, USA
explained inductive loops in the low-frequency part of the spectrum. Epelboin and Loric [13] addressed the role of reaction intermediates in causing low-frequency inductive loops. Kinetic models accounting for reaction intermediates were addressed in greater detail in publications by Armstrong et al. [14] and Epelboin et al. [15]. The influence of electrode geometry was explored by de Levie [16], who developed transmission line models for the impedance response of porous and rough electrodes. Newman [17] showed that the non-uniform current and potential distribution of disk electrodes can result in high-frequency timeconstant dispersion. Levart and Schuhmann [18] developed a model for the diffusion impedance of a rotating disk that accounted for the influence of homogeneous chemical reactions. Work has progr
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