Fundamental Atomic Insight in Electrocatalysis

Bagger, Alexander; Castelli, Ivano E.; Hansen, Martin Hangaard

doi:10.1007/978-3-319-44680-6_8

Cited by 3 publications

(12 citation statements)

References 69 publications

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“…Predictive-quality first-principles calculations based on DFT have undoubtedly become a cornerstone in modern materials, catalysis, and energy research. In the specific context of catalysis at electrified interfaces, this development is largely connected to the ingenious computational hydrogen electrode (CHE) approach of Rossmeisl, Nørskov, and co-workers. , It is difficult to understate the impact that this single approach has made on the design of electrocatalysts or the unraveling of electrochemical reaction mechanisms. ,,,− By the very nature of its approximation, the CHE puts the predominant emphasis on the electrode site. Over the past decade or so, first-principles electrocatalysis research at solid–liquid interfaces (SLIs) was correspondingly dominated by finding optimum catalyst materials that lie at the top of reaction volcanos or gaining mechanistic understanding in terms of surface chemical bonds, yet without much caring for the electrolyte side of the SLI.…”

Section: Discussionmentioning

confidence: 99%

“…Figure illustrates this with corresponding work from McCrum et al for the Pt(111) surface in a water environment. Such kinds of CHE surface phase diagrams are nowadays widely used to draw first conclusions on the actual surface structures and compositions of electrodes under true operating conditions, and we refer to excellent reviews on this topic ,,,− for a more detailed overview of the uses and merits of this kind of most popular CHE application.…”

Section: Implicit Solvation Models Applied To Electrified Slismentioning

confidence: 99%

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Implicit Solvation Methods for Catalysis at Electrified Interfaces

et al. 2021

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Implicit solvation is an effective, highly coarse-grained approach in atomic-scale simulations to account for a surrounding liquid electrolyte on the level of a continuous polarizable medium. Originating in molecular chemistry with finite solutes, implicit solvation techniques are now increasingly used in the context of first-principles modeling of electrochemistry and electrocatalysis at extended (often metallic) electrodes. The prevalent ansatz to model the latter electrodes and the reactive surface chemistry at them through slabs in periodic boundary condition supercells brings its specific challenges. Foremost this concerns the difficulty of describing the entire double layer forming at the electrified solid–liquid interface (SLI) within supercell sizes tractable by commonly employed density functional theory (DFT). We review liquid solvation methodology from this specific application angle, highlighting in particular its use in the widespread ab initio thermodynamics approach to surface catalysis. Notably, implicit solvation can be employed to mimic a polarization of the electrode’s electronic density under the applied potential and the concomitant capacitive charging of the entire double layer beyond the limitations of the employed DFT supercell. Most critical for continuing advances of this effective methodology for the SLI context is the lack of pertinent (experimental or high-level theoretical) reference data needed for parametrization.

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Section: Discussionmentioning

confidence: 99%

Section: Implicit Solvation Models Applied To Electrified Slismentioning

confidence: 99%

Implicit Solvation Methods for Catalysis at Electrified Interfaces

et al. 2021

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“…One key assumption of the CHE approach is that the adsorption energy of the reaction intermediates is independent of the electrostatic field present at the electrode/electrolyte interface. 450 Using a Pt (111) surface model, Karlberg et al 128 computed how the adsorption energy of the intermediates of the ORR/OER (*O, *OH, *OOH) depends on the strength of an external electric field. To model the water solvent, the authors included a water bilayer in the case of *O, while for *OH and *OOH the authors included one water molecule per *OH and *OOH molecule.…”

Section: Modeling Electrochemical Systems At Fixed Potentialmentioning

confidence: 99%

Section: Modeling the Electrified Solid/liquid Interfacementioning

confidence: 99%

Toward Realistic Models of the Electrocatalytic Oxygen Evolution Reaction

Jones,

Teschner,

Piccinin

2024

Chem. Rev.

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The electrocatalytic oxygen evolution reaction (OER) supplies the protons and electrons needed to transform renewable electricity into chemicals and fuels. However, the OER is kinetically sluggish; it operates at significant rates only when the applied potential far exceeds the reversible voltage. The origin of this overpotential is hidden in a complex mechanism involving multiple electron transfers and chemical bond making/breaking steps. Our desire to improve catalytic performance has then made mechanistic studies of the OER an area of major scientific inquiry, though the complexity of the reaction has made understanding difficult. While historically, mechanistic studies have relied solely on experiment and phenomenological models, over the past twenty years ab initio simulation has been playing an increasingly important role in developing our understanding of the electrocatalytic OER and its reaction mechanisms. In this Review we cover advances in our mechanistic understanding of the OER, organized by increasing complexity in the way through which the OER is modeled. We begin with phenomenological models built using experimental data before reviewing early efforts to incorporate ab initio methods into mechanistic studies. We go on to cover how the assumptions in these early ab initio simulationsno electric field, electrolyte, or explicit kineticshave been relaxed. Through comparison with experimental literature, we explore the veracity of these different assumptions. We summarize by discussing the most critical open challenges in developing models to understand the mechanisms of the OER.

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“…which implies a theoretical overpotential of ∼0.37 V. These linear correlations are known as scaling relationships and reveal reactivity trends in elementary reactions, in which related intermediates bind through the same atom or on the same site [70]. These relationships impose limits to the minimum overpotentials required for a process to occur and the maximum catalytic activity that may be obtained [71].…”

Section: Classification Of Nickel-based Electrocatalysts By Compositionmentioning

confidence: 99%

Nickel-Based Electrocatalysts for Water Electrolysis

et al. 2022

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Currently, hydrogen production is based on the reforming process, leading to the emission of pollutants; therefore, a substitute production method is imminently required. Water electrolysis is an ideal alternative for large-scale hydrogen production, as it does not produce any carbon-based pollutant byproducts. The production of green hydrogen from water electrolysis using intermittent sources (e.g., solar and eolic sources) would facilitate clean energy storage. However, the electrocatalysts currently required for water electrolysis are noble metals, making this potential option expensive and inaccessible for industrial applications. Therefore, there is a need to develop electrocatalysts based on earth-abundant and low-cost metals. Nickel-based electrocatalysts are a fitting alternative because they are economically accessible. Extensive research has focused on developing nickel-based electrocatalysts for hydrogen and oxygen evolution. Theoretical and experimental work have addressed the elucidation of these electrochemical processes and the role of heteroatoms, structure, and morphology. Even though some works tend to be contradictory, they have lit up the path for the development of efficient nickel-based electrocatalysts. For these reasons, a review of recent progress is presented herein.

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Fundamental Atomic Insight in Electrocatalysis

Cited by 3 publications

References 69 publications

Implicit Solvation Methods for Catalysis at Electrified Interfaces

Implicit Solvation Methods for Catalysis at Electrified Interfaces

Toward Realistic Models of the Electrocatalytic Oxygen Evolution Reaction

Nickel-Based Electrocatalysts for Water Electrolysis

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