Impedance Spectra and Surface Coverages Simulated Directly from the Electrochemical Reaction Mechanism: A Nonlinear State-Space Approach

George, Kiran; Berkel, M. van; Zhang, Xueqing; Sinha, Rochan; Bieberle‐Hütter, Anja

doi:10.1021/acs.jpcc.9b01836

Cited by 19 publications

(33 citation statements)

References 80 publications

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“…In this regard, multiscale computational models which connect the thermodynamics and kinetics of the elementary steps at the atomistic level to the activity at laboratory scale and which can simulate electrochemical measurements, are of high interest. 2,9 From a molecular perspective, this requires an electrochemical model which can provide the rate constants for elementary transformations at the solid-liquid interface as a function of the operando conditions.…”

Section: Introductionmentioning

confidence: 99%

A multiscale modelling approach to elucidate the mechanism of the oxygen evolution reaction at the hematite–water interface

et al. 2021

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Section: Introductionmentioning

confidence: 99%

A multiscale modelling approach to elucidate the mechanism of the oxygen evolution reaction at the hematite–water interface

et al. 2021

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“…The charge transferred in the formation of the adsorbed OER intermediates is analogous to charge carriers getting trapped at the surface. Previously, we developed a microkinetic model of OER specifically for semiconductor electrodes . In the current paper, we add illumination and charge carrier dynamics to the same framework of the microkinetic model of the OER.…”

Section: Introductionmentioning

confidence: 99%

“…For simulating r-SS, a monoenergetic state with energy E T and density N T (T stands for “trap”) is assumed within the band gap of the semiconductor . Thus, we present in this paper an extended model to George et al which brings together the elementary steps in the OER and charge carrier dynamics within the semiconductor. Modeling of charge carrier dynamics has been done before in the literature. , However, the charge carrier dynamics has so far not been coupled to the multistep mechanism of the OER at the interface.…”

Section: Introductionmentioning

confidence: 99%

Understanding the Impact of Different Types of Surface States on Photoelectrochemical Water Oxidation: A Microkinetic Modeling Approach

et al. 2020

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The oxygen evolution reaction (OER) has been identified as one of the performance-limiting processes in solar water splitting using photoelectrochemical (PEC) cells. One of the reasons for the low OER performance is related to the existence of different types of surface states at the semiconductor–electrolyte interface: recombining surface states (r-SS) and surface states due to intermediate species (i-SS). Since the impact of surface states on OER is still under debate, we investigate how different types of surface states affect PEC water oxidation and how they impact experimental measurements. In a new computational approach, we combine a microkinetic model of the OER on the semiconductor surface with the charge carrier dynamics within the semiconductor. The impact of r-SS and i-SS on the current–voltage curves, hole flux, surface state capacitance, Mott–Schottky plots, and chopped light measurements is systematically investigated. It is found that (a) r-SS results in a capacitance peak below the OER onset potential, while i-SS results in a capacitance peak around the onset potential; (b) r-SS leads to an increase in the OER onset potential and a decrease in the saturation current density; (c) r-SS leads to Fermi-level pinning before the onset potential, while i-SS does not result in Fermi-level pinning; and (d) a smaller capacitance peak of i-SS can be an indication of the lower catalytic performance of the semiconductor surface. Our approach in combination with experimental comparison allows distinguishing the impact of r-SS and i-SS in PEC experiments. We conclude that r-SS reduces the OER performance and i-SS mediates the OER.

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“…As a variety of adsorption intermediates are produced on the anode surface in the OER reaction, the reversible specific adsorption of the OER intermediates is represented by the adsorption capacitance CPE ads and the adsorption resistance R ads during the EIS experiment and data analysis. [33][34][35] Figure 5a,b shows the relationship between MIE and R ct or R ads , respectively. The changing trend of MIE and R ct or R ads is consistent with that of MIE and Tafel slope corresponding to the results in Figure 4b.…”

Section: The Relationship Between the Mie And The Intrinsic Oer Activity Of Mofsmentioning

confidence: 99%

Correlation and Improvement of Bimetallic Electronegativity on Metal–Organic Frameworks for Electrocatalytic Water Oxidation

Ying

Tang

Zhao

et al. 2021

Adv Energy and Sustain Res

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Development of efficient energy conversion and storage devices such as electrolyzers, regenerative fuel cells, and rechargeable fuel cells is vital to solve the deteriorating environmental issue caused by the consumption of fossil fuels. [1][2][3] However, the overall performance of these devices are still hindered, due to the sluggish kinetics of oxygen evolution reaction (OER) which is a complex four-electron transfer reaction. [4][5][6][7] To promote OER in the electrocatalytic overall water splitting, electrocatalysts based on noble metals and/or noble metal oxides are required. However, the large-scale production and commerical applications has been impeded by the high cost and poor stability of noble metal catalysts. [8][9][10] Therefore, it is highly desirable to exploit the readily available and cost-effective OER electrocatalysts that can replace the noble-metal-based catalysts.Metal-organic frameworks (MOFs) formed by coordination bonds between metal atom nodes and organic ligands with periodic structural units have a larger surface area (up to more than 10 000 m 2 g À1 ), more catalytic sites, and easier adjustment of structure (the metal sites and/or the organic linkers). [11] Altogether, MOFs combine the benefits of homogeneous catalysts (e.g., well-defined structure and/or ligand environment) and the heterogeneous catalysts (e.g., site isolation and/or recyclability). [12][13][14] Hence, MOFs have become promising candidates for electrocatalysts. [15,16] However, due to the poor charge transport and inappropriate intermediates absorption energy, the electrocatalytic performance of MOF materials has long been unsatisfactory. [13,17,18] To overcome these obstacles,

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Impedance Spectra and Surface Coverages Simulated Directly from the Electrochemical Reaction Mechanism: A Nonlinear State-Space Approach

Cited by 19 publications

References 80 publications

A multiscale modelling approach to elucidate the mechanism of the oxygen evolution reaction at the hematite–water interface

A multiscale modelling approach to elucidate the mechanism of the oxygen evolution reaction at the hematite–water interface

Understanding the Impact of Different Types of Surface States on Photoelectrochemical Water Oxidation: A Microkinetic Modeling Approach

Correlation and Improvement of Bimetallic Electronegativity on Metal–Organic Frameworks for Electrocatalytic Water Oxidation

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