The structure of the electric double layer: Atomistic versus continuum approaches

Sakong, Sung; Huang, Jun; Eikerling, Michael; Groß, Axel

doi:10.1016/j.coelec.2022.100953

Cited by 12 publications

(8 citation statements)

References 50 publications

(64 reference statements)

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“…Therefore, when the modified graphite felt is used as the electrode of the iron‐chromium flow battery, the surface groups of the solid electrode tend to selectively absorb some charged ions from the electrolyte and gather near the electrode. Since the whole system is electrically neutral, as shown in Figure 11, a large number of equally charged anisotropic ions will also accumulate in the electrolyte, thus forming a thin electric double layer at the junction of the electrode and the electrolyte [21] …”

Section: Resultsmentioning

confidence: 99%

Research on the Performance of Cobalt Oxide Decorated Graphite Felt as Electrode of Iron‐Chromium Flow Battery

Ren

Zhao

et al. 2023

ChemElectroChem

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In this paper, cobalt oxide-modified graphite felt electrodes were prepared by electrodepositing cobalt nitrate on graphite felt and calcined. The surface morphology of graphite felt modified by cobalt oxide was characterized in detail by scanning electron microscope X-ray diffraction and X-ray photoelectron spectroscopy. Shape, microstructure, etc. And using the three-electrode system to conduct cyclic voltammetry, electrochemical impedance spectroscopy, and single-cell constant current charge and discharge detection on the graphite felt electrodes modified with different concentrations of cobalt oxide, and study its use as an electrode for iron-chromium redox flow battery performance. The results show that the method of calcination after electrodeposition successfully attaches cobalt oxide to the graphite felt fiber uniformly in granular form, increases a large number of oxygen-containing functional groups, and has the highest coulombic efficiency for the first charge-discharge cycle at a current density of 142mAcm À 2 It can reach 82 %, and the charging capacity is also increased by 1.59 times compared with the original graphite felt.

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Section: Resultsmentioning

confidence: 99%

Research on the Performance of Cobalt Oxide Decorated Graphite Felt as Electrode of Iron‐Chromium Flow Battery

Ren

Zhao

et al. 2023

ChemElectroChem

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“…Second, we have treated the EDL as a serial connection of an adlayer and a diffuse layer. Atomic-scale understanding from first-principles calculations can be used to obtain parameters of the EDL model. , Third, we have assumed the surface charging effect on the adsorption energy of intermediate simply as a linear relation. DFT-based calculations should be employed to gain explicit insights into this relation. , Fourth, the steady-state assumption has been used in this work.…”

Section: Discussionmentioning

confidence: 99%

“…Atomic-scale understanding from first-principles calculations can be used to obtain parameters of the EDL model. 76 , 77 Third, we have assumed the surface charging effect on the adsorption energy of intermediate simply as a linear relation. DFT-based calculations should be employed to gain explicit insights into this relation.…”

Section: Discussionmentioning

confidence: 99%

pH Effects in a Model Electrocatalytic Reaction Disentangled

Zhu

Huang

Eikerling

2023

JACS Au

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Varying the solution pH not only changes the reactant concentrations in bulk solution but also the local reaction environment (LRE) that is shaped furthermore by macroscopic mass transport and microscopic electric double layer (EDL) effects. Understanding ubiquitous pH effects in electrocatalysis requires disentangling these interwoven factors, which is a difficult, if not impossible, task without physical modeling. Herein, we demonstrate how a hierarchical model that integrates microkinetics, double-layer charging, and macroscopic mass transport can help understand pH effects of the formic acid oxidation reaction (FAOR). In terms of the relation between the peak activity and the solution pH, intrinsic pH effects without consideration of changes in the LRE would lead to a bell-shaped curve with a peak at pH = 6. Adding only macroscopic mass transport, we can already reproduce qualitatively the experimentally observed trapezoidal shape with a plateau between pH 5 and 10 in perchlorate and sulfate solutions. A quantitative agreement with experimental data requires consideration of EDL effects beyond Frumkin correlations. Specifically, the peculiar nonmonotonic surface charging relation affects the free energies of adsorbed intermediates. We further discuss pH effects of FAOR in phosphate and chloride-containing solutions, for which anion adsorption becomes important. This study underpins the importance of a full consideration of multiple interrelated factors for the interpretation of pH effects in electrocatalysis.

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“…As our society is on the course toward a sustainable energy economy by embracing batteries, fuel cells, and electrolyzers for energy storage and conversion, electrochemistry has become a vibrant field of research. Among various rapidly developing research fronts of electrochemistry, the electric double layer (EDL) is of particular fundamental interest and importance. − Although the EDL is an essential part of any electrochemical cell, it is notoriously difficult to assess in experiment and theory. The grand challenge for experimental studies is separating the weak EDL signal from the dominant background of the contacting solid and bulk solution phases and determining the local properties at the interface.…”

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confidence: 99%

Comparing Ab Initio Molecular Dynamics and a Semiclassical Grand Canonical Scheme for the Electric Double Layer of the Pt(111)/Water Interface

Huang

Zhang

et al. 2023

J. Phys. Chem. Lett.

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The theoretical modeling of metal/water interfaces centers on an appropriate configuration of the electric double layer (EDL) under grand canonical conditions. In principle, ab initio molecular dynamics (AIMD) simulations would be the appropriate choice for treating the competing water−water and water−metal interactions and explicitly considering the atomic and electronic degrees of freedom. However, this approach only allows simulations of relatively small canonical ensembles over a limited period (shorter than 100 ps). On the other hand, computationally efficient semiclassical approaches can treat the EDL model based on a grand canonical scheme by averaging the microscopic details. Thus, an improved description of the EDL can be obtained by combining AIMD simulations and semiclassical methods based on a grand canonical scheme. By taking the Pt(111)/water interface as an example, we compare these approaches in terms of the electric field, water configuration, and double-layer capacitance. Furthermore, we discuss how the combined merits of the approaches can contribute to advances in EDL theory.

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The structure of the electric double layer: Atomistic versus continuum approaches

Cited by 12 publications

References 50 publications

Research on the Performance of Cobalt Oxide Decorated Graphite Felt as Electrode of Iron‐Chromium Flow Battery

Research on the Performance of Cobalt Oxide Decorated Graphite Felt as Electrode of Iron‐Chromium Flow Battery

pH Effects in a Model Electrocatalytic Reaction Disentangled

Comparing Ab Initio Molecular Dynamics and a Semiclassical Grand Canonical Scheme for the Electric Double Layer of the Pt(111)/Water Interface

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