Strain Controlling Catalytic Efficiency of Water Oxidation for Ni1−xFexOOH Alloy

Hamal, Ester Korkus; Toroker, Maytal Caspary

doi:10.1007/978-981-33-6639-8_1

Cited by 2 publications

(2 citation statements)

References 43 publications

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“…The identification of universal scaling relationships mediating η CHE for the OER on oxides established an entire body of literature aimed at identifying strategies to circumvent the observed scaling relationships; ,− for a detailed review see ref . An early effort sought to investigate how substitutional doping of Ti in a rutile-type TiO 2 (110) surface with various transition metals (M = V, Nb, Ta, Cr, Mo, W, Mn, Fe, Ru, Ir, Ni) would impact the theoretical OER overpotential .…”

Section: Ab Initio Atomistic Thermodynamics and The Computational Hyd...mentioning

confidence: 99%

“…Despite the evidence against the relevance of the single-site nucleophilic attack mechanism, ,,,,,, it remains a mainstay in the literature, and the possibility to break the scaling relationships associated with it through the participation of multiple sites has prompted significant research into multisite mechanisms within the CHE. These range from the cooperative effects of dopants − ,, and vacancies, − to metal ions in different oxidation states, , to using interfaces as the source of multiple sites. ,,, Strain and geometric distortion too have often been invoked as possible means of breaking scaling relationships and increasing catalytic activity. − ,− However, all such studies ultimately rely on both the assumptions underlying the CHE and the accuracy of the assumed mechanism, but there is often limited mechanistic proof. Without mechanistic evidence supporting the predictions made using the CHE, design may be accomplished more readily with other descriptions.…”

Section: Ab Initio Atomistic Thermodynamics and The Computational Hyd...mentioning

confidence: 99%

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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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Section: Ab Initio Atomistic Thermodynamics and The Computational Hyd...mentioning

confidence: 99%

Section: Ab Initio Atomistic Thermodynamics and The Computational Hyd...mentioning

confidence: 99%

Toward Realistic Models of the Electrocatalytic Oxygen Evolution Reaction

Jones,

Teschner,

Piccinin

2024

Chem. Rev.

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Low-spin state of Fe in Fe-doped NiOOH electrocatalysts

Tesch

Eslamibidgoli

et al. 2023

Nat Commun

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Doping with Fe boosts the electrocatalytic performance of NiOOH for the oxygen evolution reaction (OER). To understand this effect, we have employed state-of-the-art electronic structure calculations and thermodynamic modeling. Our study reveals that at low concentrations Fe exists in a low-spin state. Only this spin state explains the large solubility limit of Fe and similarity of Fe-O and Ni-O bond lengths measured in the Fe-doped NiOOH phase. The low-spin state renders the surface Fe sites highly active for the OER. The low-to-high spin transition at the Fe concentration of ~ 25% is consistent with the experimentally determined solubility limit of Fe in NiOOH. The thermodynamic overpotentials computed for doped and pure materials, η = 0.42 V and 0.77 V, agree well with the measured values. Our results indicate a key role of the low-spin state of Fe for the OER activity of Fe-doped NiOOH electrocatalysts.

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Strain Controlling Catalytic Efficiency of Water Oxidation for Ni1−xFexOOH Alloy

Cited by 2 publications

References 43 publications

Toward Realistic Models of the Electrocatalytic Oxygen Evolution Reaction

Toward Realistic Models of the Electrocatalytic Oxygen Evolution Reaction

Low-spin state of Fe in Fe-doped NiOOH electrocatalysts

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