Quantitative Kinetic Analysis of a PdAu<sub>3</sub>Alloy Catalyst for Oxygen Electro-Reduction

Kurnatowski, Martin von; Bortz, Michael; Klein, Peter; Kintzel, Birgit; Cremers, Carsten

doi:10.1149/2.0751714jes

“…Furthermore, We listed promising candidates predicted to be more active, selective and acid-stable than PtHg 4 , where they were categorized with respect to the acid-stability (Table S4) and CuAu 3 were found to satisfy all conditions to outperform PtHg 4 in acid, and we note that some of them were already synthesized and tested for the 2e ORR. 33,34 Although we have focused on the acid-condition in this work, we note that the same analysis can be done using neutral-stability and base-stability to suggest promising candidates in different…”

Section: Discussionmentioning

confidence: 99%

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

Back

¹

,

Na²,

Ulissi³

2020

Preprint

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<div> <div> <div> <p>Electrochemical reduction of O2 provides a clean and decentralized pathway to produce H2O2 compared to the current energy-intensive anthraquinone process. As the electrochemical reduction of O2 proceeds via either two-electron or four-electron path- way, it is thus essential to control the selectivity as well as to maximize the catalytic activity. Siahrostami et al. demonstrated a novel approach to control the reaction pathway by optimizing an adsorption ensemble to tune adsorption sites of reaction intermediates, and identified Pt-Hg catalysts from density functional theory (DFT) calculations and experimentally validated this catalyst (Nat. Mater. 2013, 12, 1137). Inspired by this concept, in this work, we apply a state-of-the-art high-throughput screening to develop O2 reduction catalyst for selective H2O2 production. Starting from Materials Project database, we evaluate activity, selectivity and electrochemical stability. To efficiently perform the screening, we introduce an active motif based approach which pre-screens unpromising materials and only performs DFT calculations for promising materials, which significantly reduce the number of the required calculations. We not only provide a list of promising candidates identified by DFT calculations, but also suggest element species to achieve high catalytic activity or H2O2 selectivity for future experimental attempts. Finally, we discuss a strategy for efficient future high-throughput screening using a machine learning pipeline consisting of a non-linear dimension reduction and a density-based clustering. </p> </div> </div> </div>

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“…32 and CuAu 3 were found to satisfy all conditions to outperform PtHg 4 in acid, and we note that some of them were already synthesized and tested for the 2e ORR. 33,34 Although we have focused on the acid-condition in this work, we note that the same analysis can be done using neutral-stability and base-stability to suggest promising candidates in different environments. For example, CuSe 2 is expected to be unstable under the acidic condition (∆G Pourbaix =0.51 eV/atom), while it showed better stability under the neutral condition (∆G Pourbaix =0.20 eV/atom).…”

Section: Discussionmentioning

confidence: 99%

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

Back

¹

,

Na²,

Ulissi³

2020

Preprint

View full text Add to dashboard Cite

<div> <div> <div> <p>Electrochemical reduction of O2 provides a clean and decentralized pathway to produce H2O2 compared to the current energy-intensive anthraquinone process. As the electrochemical reduction of O2 proceeds via either two-electron or four-electron path- way, it is thus essential to control the selectivity as well as to maximize the catalytic activity. Siahrostami et al. demonstrated a novel approach to control the reaction pathway by optimizing an adsorption ensemble to tune adsorption sites of reaction intermediates, and identified Pt-Hg catalysts from density functional theory (DFT) calculations and experimentally validated this catalyst (Nat. Mater. 2013, 12, 1137). Inspired by this concept, in this work, we apply a state-of-the-art high-throughput screening to develop O2 reduction catalyst for selective H2O2 production. Starting from Materials Project database, we evaluate activity, selectivity and electrochemical stability. To efficiently perform the screening, we introduce an active motif based approach which pre-screens unpromising materials and only performs DFT calculations for promising materials, which significantly reduce the number of the required calculations. We not only provide a list of promising candidates identified by DFT calculations, but also suggest element species to achieve high catalytic activity or H2O2 selectivity for future experimental attempts. Finally, we discuss a strategy for efficient future high-throughput screening using a machine learning pipeline consisting of a non-linear dimension reduction and a density-based clustering. </p> </div> </div> </div>

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“…on Au–Pd further confirmed this conclusion. In addition, the Au@Ni core–shell structure 59 and PdAu 3 alloy 60 catalysts also have high catalytic activity for H 2 O 2 . In the Au@Ni core–shell structure, the Ni(OH) 2 –Ni–Au interface is the ORR active center.…”

Section: Research Advances In Electrocatalytic Orr For H2o2 Productionmentioning

confidence: 99%

Research progress of electrocatalysts for the preparation of H₂O₂ by electrocatalytic oxygen reduction reaction

Ren

¹

,

Dong

²

,

Liu

³

et al. 2023

SusMat

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As an eco‐friendly oxidant and energy carrier, H2O2 is used in various fields. The industrial production of H2O2 mostly depends on the large‐scale anthraquinone oxidation processes with high costs. Electrocatalytic production of H2O2 has attracted attention as a renewable and cost‐effective approach to replace traditional ones. With the recent development of oxygen reduction reaction (ORR) catalysts, remarkable progress in electrocatalysts for electrocatalytic H2O2 production by 2e− ORR has been reported. This review summarizes a detailed overview of the recent progress in 2e− ORR for H2O2 production with the mechanism and various efficient catalysts. The catalysts were divided into three parts: noble metal‐based catalyst, non‐noble metal‐based catalyst, and non‐metal‐based catalyst. The influences of the catalytic activity and selectivity were also discussed. Finally, this review explores the prospects of electrocatalytic 2e− ORR for H2O2 synthesis and potential research directions for electrocatalysts. It aims to offer guidance in designing efficient 2e− ORR electrocatalysts and inspire further innovation in electrocatalytic H2O2 synthesis.

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Quantitative Kinetic Analysis of a PdAu₃Alloy Catalyst for Oxygen Electro-Reduction

Cited by 6 publications

References 38 publications

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

Research progress of electrocatalysts for the preparation of H₂O₂ by electrocatalytic oxygen reduction reaction

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Quantitative Kinetic Analysis of a PdAu3Alloy Catalyst for Oxygen Electro-Reduction

Cited by 6 publications

References 38 publications

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

Research progress of electrocatalysts for the preparation of H2O2 by electrocatalytic oxygen reduction reaction

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Product

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Quantitative Kinetic Analysis of a PdAu₃Alloy Catalyst for Oxygen Electro-Reduction

Research progress of electrocatalysts for the preparation of H₂O₂ by electrocatalytic oxygen reduction reaction