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Electrochemistry Modulated Interfacial Processes: Fundamental and Application

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A special issue of Electrochem (ISSN 2673-3293).

Deadline for manuscript submissions: closed (30 June 2023) | Viewed by 9053

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Special Issue Editor

Dr. Hsiu-Wei Cheng

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Guest Editor

Department of Chemistry, National Taiwan University, Taipei City 10617, Taiwan
Interests: interfacial process; electrochemistry; surface analysis; instrument analysis

Special Issue Information

Dear Colleagues,

Interfacial processes have governed device performance from various perspectives—in mechanics, it is critical in friction and lubrication for machine efficiency; in chemistry, interfacial chemical properties have great influence on surface activity, which directly determines the catalytical performance, corrosion resistivity, and charge transfer characteristics of functional materials; and in biology, by understanding the essential biochemical reactions/processes of life that take place at the interface of cell membranes, Golgi apparatus and endoplasmic reticulum are crucial for medicine development as well as artificial implants design.

Through the increasing study of the macroscopy features of aforementioned interfaces, a more fundamental, molecular-scope understanding becomes significantly necessary. However, the adequate analytic tools for accessing such an interfacial region, with the typical thickness of a few nanometers, are very limited. In addition, researchers from different fields are very often utilizing very distinct or specialized approaches in their own field only, which, in a certain extent, becomes an obstacle for cross-field interaction.

The proposed Special Issue is dedicated to collecting cutting-edge researches from various fields to provide a platform that can encourage multidisciplinary dialogue. There is specific focus on electrochemically modulated interfacial kinetic studies.

Dr. Hsiu-Wei Cheng
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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Keywords

biointerfaces
tribology
electrochemistry
surface analysis
corrosion
catalysis
charge transfer

Published Papers (4 papers)

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Research

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13 pages, 2375 KiB

Open AccessArticle

The Difference in the Effects of IR-Drop from the Negative Capacitance of Fast Cyclic Voltammograms

by Yuanyuan Liu, Koichi Jeremiah Aoki and Jingyuan Chen

Electrochem 2023, 4(4), 460-472; https://doi.org/10.3390/electrochem4040030 - 23 Oct 2023

Cited by 2 | Viewed by 1317

Abstract

Diffusion-controlled cyclic voltammograms at fast scan rates show peak shifts, as well as decreases in the peak currents from predicted diffusion-controlled currents, especially when the currents are large in a low concentration of supporting electrolytes. This has been conventionally recognized as an IR-drop effect due to solution resistance on the peaks, as well as a heterogeneously kinetic effect. It is also brought about by the negatively capacitive currents associated with charge transfer reactions. The reaction product generates dipoles with counterions to yield a capacitance, the current of which flows oppositely to that of the double-layer capacitance. The three effects are specified here in the oxidation of a ferrocenyl derivative using fast scan voltammetry. The expression for voltammograms complicated with IR-drop is derived analytically and yields deformed voltammograms. The peak shift is approximately linear with the IR-voltage, but exhibits a convex variation. The dependence of some parameters on the peaks due to the IR-drop is compared with those due to the negative capacitance. The latter is more conspicuous than the former under conventional conditions. The two effects cannot be distinguished specifically except for variations in the conductance of the solution. Full article

(This article belongs to the Special Issue Electrochemistry Modulated Interfacial Processes: Fundamental and Application)

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12 pages, 2791 KiB

Open AccessArticle

by Yuanyuan Liu, Koichi Jeremiah Aoki and Jingyuan Chen

Electrochem 2023, 4(2), 301-312; https://doi.org/10.3390/electrochem4020021 - 13 Jun 2023

Cited by 2 | Viewed by 1599

Abstract

Chronoamperometric curves for the oxidation of a ferrocenyl derivative via a potential step, calculated using the Cottrell equation, showed less diffusion-controlled currents on a platinum wire electrode. This lower deviation cannot be explained via Butler–Volmer heterogeneous kinetics, but was ascribed to the negatively capacitive current associated with a redox reaction. The deviation in fully oxidized electrical potential corresponds to the non-zero concentration at the electrode surface, which cannot be predicted using the Nernst equation. This equation expresses the relationship between the electrical potential and activity at the electrode surface rather than the concentration. The diffusion equation determines the relationship between the current and surface concentration rather than activity. Negative capacitance or a non-zero concentration may arise from structure formation on the electrode owing to dipole–dipole interactions, which are similar to the generation of double-layer capacitance, including frequency dispersion. Following this concept, we derive expressions for a lowered diffusion-controlled current and time-dependent surface concentration. The negatively capacitive current shows the time dependence of t^−0.9, which is similar to the decay of double-layer capacitive currents. The surface concentration decays with t^−0.4-dependence. Full article

(This article belongs to the Special Issue Electrochemistry Modulated Interfacial Processes: Fundamental and Application)

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10 pages, 2422 KiB

Open AccessArticle

Enhancement of the Negative Capacitance Associated with the Dissolution of Silver by Salt Concentrations by Means of Anodic Stripping Voltammetry

by Ru Wang, Koichi Jeremiah Aoki and Jingyuan Chen

Electrochem 2022, 3(3), 397-406; https://doi.org/10.3390/electrochem3030027 - 25 Jul 2022

Cited by 2 | Viewed by 1357

Abstract

The amount of anodically dissolved charge of silver by linear sweep stripping voltammetry has been observed to be smaller than that of the potentiostatically deposited charge. The imbalance in the charge is opposite to the participation in the double-layer capacitance. This can be explained in terms of the negative capacitive current, which is caused by dipoles of generated redox charge (Ag⁺) with counterions (NO₃⁻). Lower concentrations of counterions may suppress the capacitance to retain the equality of the charge. This prediction is examined in this work by the oxidation of silver film at various concentrations of NO₃⁻ by anodic stripping voltammetry. The capacitance decreased with a decrease in the salt concentrations less than 0.05 mol dm⁻³. Low concentrations of salts prevent loss of the anodic charge in electroanalysis. This dependence was related with the lifespan of generated silver nitrate dipoles and is described theoretically. Full article

(This article belongs to the Special Issue Electrochemistry Modulated Interfacial Processes: Fundamental and Application)

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Review

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37 pages, 1471 KiB

Open AccessReview

Use of Inner/Outer Sphere Terminology in Electrochemistry—A Hexacyanoferrate II/III Case Study

by John F. Cassidy, Rafaela C. de Carvalho and Anthony J. Betts

Electrochem 2023, 4(3), 313-349; https://doi.org/10.3390/electrochem4030022 - 11 Jul 2023

Cited by 8 | Viewed by 3949

Abstract

Salts of hexacyanoferrate II/III anions have been widely used as redox couple probe molecules to determine the characteristics of electrode surfaces. Examples include the assessment of electrocatalysts for energy applications and electrocatalysts for the detection of biological or chemical species, as well as the determination of electrochemically active surface areas. An examination of the electrochemical literature, based largely on cyclic voltammetric investigations, reveals a wide range of peak separation and/or heterogeneous electron transfer rate constants, classified sometimes as inner or outer sphere electron transfer processes. Originally developed for the mechanistic interpretation of inorganic transition metal compounds in solution, this terminology has since been extended to account for heterogeneous electron transfer occurring at electrodes. In the case of the hexacyanoferrate II/III anions, there can be a number of reasons why it sometimes behaves as an outer sphere probe and at other times displays inner sphere electron transfer characteristics. After examining some of the structural and chemical properties of the hexacyanoferrate II/III species, the methods used to determine such classifications are described. The most common method involves measuring peak-to-peak separation in a cyclic voltammogram to ascertain a heterogeneous rate constant, but it has inherent flaws. This paper reviews the reasons for the classification disparity, including the effects of various oxygen surface species, the influence of organic surface films, the nature of the cation counter-ion, surface adsorption and surface hydrophilicity/hydrophobicity. Other surface interactions may also take place, such as those occurring with Au corrosion or pH effects. These can impact the electrical double layer and thus may affect the electron transfer process. Consequently, it is recommended that hexacyanoferrate II/III should be considered a multi-sphere or alternatively a surface-sensitive electron transfer species. Full article

(This article belongs to the Special Issue Electrochemistry Modulated Interfacial Processes: Fundamental and Application)

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