Accelerating the Discovery of Oxygen Reduction Electrocatalysts: High‐Throughput Screening of Element Combinations in Pt‐Based High‐Entropy Alloys

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(37)

Published: June 27, 2024

The vast number of element combinations and the explosive growth composition space pose significant challenges to development high-entropy alloys (HEAs). Here, we propose a procedural research method aimed at accelerating discovery efficient electrocatalysts for oxygen reduction reaction (ORR) based on Pt-based quinary HEAs. begins with an library provided by large language model (LLM), combined microscale precursor printing pulse high-temperature synthesis techniques prepare multi-element combination HEA array in one step. Through high-throughput measurement using scanning electrochemical cell microscopy (SECCM), precise identification highly active exploration specific are achieved. Advantageous further validated practical electrocatalytic evaluations. contributions individual sites synergistic effects among elements such HEAs enhancing activity elucidated via density functional theory (DFT) calculations. This integrates experiments, catalyst validation, DFT calculations, providing new pathway materials field energy catalysis.

Language: Английский

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Accelerating the Discovery of Efficient High-Entropy Alloy Electrocatalysts: High-Throughput Experimentation and Data-Driven Strategies

Nano Letters, Journal Year: 2024, Volume and Issue: 24(37), P. 11632 - 11640

Published: Sept. 3, 2024

High-entropy alloys (HEAs) present both significant potential and challenges for developing efficient electrocatalysts due to their diverse combinations compositions. Here, we propose a procedural approach that combines high-throughput experimentation with data-driven strategies accelerate the discovery of HEA hydrogen evolution reaction (HER). This enables rapid preparation arrays various element composition ratios within model system. The intrinsic activity is swiftly screened using scanning electrochemical cell microscopy (SECCM), providing precise composition-activity data sets An ensemble machine learning (EML) then used predict database subspace Based on these results, two groups promising catalysts are recommended validated through actual electrocatalytic evaluations. approach, which strategies, provides new pathway electrocatalysts.

Language: Английский

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Rational design of transition metal-based heterostructure electrocatalysts for high-performance oxygen evolution reaction

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 127, P. 717 - 736

Published: April 16, 2025

Language: Английский

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Discovery of Efficient Acidic Oxygen Evolution Electrocatalyst: High‐Throughput Computational Screening of MgIrRu Oxide

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 18, 2025

Abstract Ensuring high catalytic activity and durability remains a significant challenge in the development of electrocatalysts toward oxygen evolution reaction (OER) proton exchange membrane water electrolyzer (PEMWE). This study introduces new research paradigm through high‐throughput density functional theory (DFT) calculations to screen efficient acidic OER electrocatalysts, guided by principle minimizing thermodynamic free energy optimizing adsorption energies intermediates. The incorporation Ir increases formation vacancies suppresses lattice mechanism (LOM) RuO 2 , thereby enhancing its stability. In addition, Mg modulates electronic structure Ru optimizes intermediates, thus improving . Electrochemical results reveal that 0.23 0.13 0.64 O exhibits low overpotential 191 mV at 10 mA cm −2 superior mass 338.6 A g noble‐metal −1 1.46 V. PEMWE with as anode catalyst achieves current 1.0 electrolysis voltage 1.81 V steadily operates 0.5 for 42 h decay only 909.5 µV work offers rational design highly active robust electrocatalysts.

Language: Английский

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Amorphous/Crystalline Heterostructure Nickel–Cobalt Oxides with Rich Oxygen Vacancies for Electrocatalytic Production of Benzoic Acid Coupled with Nitrate Reduction

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

Selective four-electron mild electrochemical oxidation of benzyl alcohol to high-value-added benzoic acid is regarded as a green alternative conventional synthesis methods under moderate conditions. Herein, we synthesize oxygen vacancy-rich amorphous/crystalline heterostructure spinel-type oxides NiCo2O4 bifunctional electrocatalyst by pulse voltammetry treatment process, which can be utilized for the anode (AOR) and cathode nitrate reduction reaction (NO3RR), respectively. The designed NiCo2O4-x-25/NF delivers only 1.18 V vs RHE at 10 mA cm-2, Faraday efficiency ∼100%. systematic studies reveal that amorphous structure generates abundant vacancies, promoting rapid generation active sites intermediate species adsorption. Meanwhile, presence crystalline accelerates electron transfer maintains structural stability, thereby improving overall performance. Impressively, it exhibits excellent electrocatalytic performance AOR coupled with NO3RR in an integrated electrolyzer, achieving current density 100 cm-2 applied low cell voltage 1.38 maintaining superior catalytic withstanding continuous electrolysis 144 h. This work provides facile approach high performance, holding great potential paired electrosynthesis value-added chemicals.

Language: Английский

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The potential of high-entropy alloys as catalyst materials in water-splitting application

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 134, P. 64 - 83

Published: May 4, 2025

Language: Английский

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Single Nanoparticle Collision Electrocatalysis Driven by Ultrafast High-Temperature Precision Synthesis

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: May 9, 2025

The single nanoparticle (NP) collision strategy offers a promising alternative to traditional ensemble methods in electrocatalysis, providing unique insights into catalytic behavior that cannot be captured by ensemble-based techniques. However, synthesizing colloidal NP catalysts with tunable composition, uniform size, and near-pristine surfaces remains significant challenge. Here, using PtxRu1-x alloys as model system, we propose an innovative combines ultrafast high-temperature precision synthesis ultrasonic exfoliation. This approach enables the preparation of desired properties, which were previously difficult achieve. Single electrocatalysis uncovers composition-dependent intrinsic activity methanol oxidation reaction (MOR) at industrial current densities, bypassing mass transfer limitations. Density functional theory (DFT) calculations highlight Pt-Ru synergistic effect optimizing MOR performance. study, for first time, integrates new framework development highly efficient catalysts.

Language: Английский

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Recent Trends and Perspectives in Single-Entity Electrochemistry: A Review with Focus on a Water Splitting Reaction

Critical Reviews in Analytical Chemistry, Journal Year: 2024, Volume and Issue: unknown, P. 1 - 17

Published: June 3, 2024

Electrochemical measurements involving single nanoparticles have attracted considerable research attention. In recent years, various studies been conducted on single-entity electrochemistry (SEE) for the in-depth analyses of catalytic reactions. Although, several electrocatalysts developed H2 energy production, designing innovative this purpose remains a challenging task. Stochastic collision is gaining increased attention because it has led to new findings in SEE field. Importantly, facilitates establishing structure activity relationships by monitoring transient signals. This article reviews achievements related hydrogen evolution reaction (HER) and oxygen (OER) using different at nanoscale level. particular, discusses electrocatalytic activities noble metal nanoparticles, including Ag, Au, Pt, Pd single-particle Because heterogeneity key factor affecting nanostructures, our work focuses influence heterogeneities materials OER HER activities. These results may help achieve better understanding fundamental processes involved water splitting reaction.

Language: Английский

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Accelerating the Discovery of Oxygen Reduction Electrocatalysts: High‐Throughput Screening of Element Combinations in Pt‐Based High‐Entropy Alloys

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(37)

Published: June 27, 2024

Abstract The vast number of element combinations and the explosive growth composition space pose significant challenges to development high‐entropy alloys (HEAs). Here, we propose a procedural research method aimed at accelerating discovery efficient electrocatalysts for oxygen reduction reaction (ORR) based on Pt‐based quinary HEAs. begins with an library provided by large language model (LLM), combined microscale precursor printing pulse high‐temperature synthesis techniques prepare multi‐element combination HEA array in one step. Through high‐throughput measurement using scanning electrochemical cell microscopy (SECCM), precise identification highly active exploration specific are achieved. Advantageous further validated practical electrocatalytic evaluations. contributions individual sites synergistic effects among elements such HEAs enhancing activity elucidated via density functional theory (DFT) calculations. This integrates experiments, catalyst validation, DFT calculations, providing new pathway materials field energy catalysis.

Language: Английский

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Electrocatalytic properties of ultrathin FeSe2/Ni0·85Se heterostructure hollow nanobelts for oxygen evolution in alkaline water and simulated seawater

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 97, P. 632 - 639

Published: Dec. 4, 2024

Language: Английский

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