2013
DOI: 10.1149/05052.0003ecst
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On the Structure of the Helmholtz Layer and its Implications on Electrode Kinetics

Abstract: Concepts and selected experiments on the structure of the Helmholtz double layer at the metal-and semiconductor -electrolyte phase boundary are reviewed. The widely used microcapacitor approach of the double layer and its limitations are assessed. Observations on the influence of the electrode potential on the energetic position of surface states at the Ag-electrolyte contact are compared to the predictions of classical charge transfer models that are based on transition state theory where adiabatic tunneling … Show more

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Cited by 10 publications
(8 citation statements)
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“…The distance t is determined by the number of solvent molecules that surround the ion and are physisorbed on the electrode surface, and is typically a few Å. 6,9 In Figure 2 we show a schematic of how we envision the equivalent process in PEDOT:PSS, a degenerately doped ptype semiconductor in which holes on the PEDOT are compensated by sulfonate anions on the PSS. This material is synthesized by polymerizing PEDOT oligomers along a PSS backbone.…”
mentioning
confidence: 99%
“…The distance t is determined by the number of solvent molecules that surround the ion and are physisorbed on the electrode surface, and is typically a few Å. 6,9 In Figure 2 we show a schematic of how we envision the equivalent process in PEDOT:PSS, a degenerately doped ptype semiconductor in which holes on the PEDOT are compensated by sulfonate anions on the PSS. This material is synthesized by polymerizing PEDOT oligomers along a PSS backbone.…”
mentioning
confidence: 99%
“…Chemical bonds, whether they are ionic, covalent, or even weaker of the van der Waals type, increase the concentration of species (ions) at an electrochemical interface. In the picture of the electrochemical double layer structure, such species are transferred either from the bulk electrolyte or from the outer to the inner Helmholtz layer to the surface during the adsorption process . The amount of adsorbed species is usually given in terms of the relative coverage which describes the fraction of the electrode surface coverage Γ I with respect to the maximum value Γ I , max of the respective adsorbate type at a certain absorption site.…”
Section: Theorymentioning
confidence: 99%
“…In the picture of the electrochemical double layer structure, such species are transferred either from the bulk electrolyte or from the outer to the inner Helmholtz layer to the surface during the adsorption process. 10 The amount of adsorbed species is usually given in terms of the relative coverage…”
Section: Introductionmentioning
confidence: 99%
“…We do not discuss continuum-based approaches that could be adapted for kinetic modeling of PEC operation; towards this end, there are a number of recent publications and reviews describing the specific application of continuum models to the properties and performance of photoelectrodes. [182][183][184][185][186][187][188] Nevertheless, it should be emphasized that one of the most pressing current research needs in the PEC community is the development of simulation frameworks that combine the power and accuracy of atomistic approaches with the flexibility of continuum approaches. This would allow for simulation of the kinetics of PEC operation at the system level under ''realistic'' conditions of varying pH, illumination, bias, and electrolyte composition/concentration.…”
Section: Modeling and Simulation Of Photoelectrode Operation At Smallmentioning
confidence: 99%