A Multi‐Site Synergistic Effect in High‐Entropy Alloy for Efficient Hydrogen Evolution

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 4, 2024

Abstract Unraveling the mechanism driven by electronegativity‐dominated electronic configuration is crucial for developing high‐entropy alloys as efficient catalyst hydrogen evolution reaction (HER). In this work, different atoms with diverse electronegativities are explored to regulate electrocatalytic activity of PtFeCoNi@HCS toward HER, resulting in PtFeCoNiCuCr@HCS an overpotential 29 mV at 10 mA cm −2 and enhanced durability surpassing that commercial 20% Pt/C KOH environment. Based on various physicochemical electrochemical techniques well density functional theory calculations, a multi‐site synergistic effect within material elucidated terms both structural composition process. Briefly, Pt Cu serve fundamental elements form face‐centered cubic crystal framework, Cr primarily functions electron donor configuration, Co serves main active site water dissociation, produced species prefer transfer Pt, Fe, sites formation. This work offers in‐depth insight high entropy helpful designing electrocatalysts.

Language: Английский

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Suppression of Structural Heterogeneity in High‐Entropy Intermetallics for Electrocatalytic Upgrading of Waste Plastics

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 29, 2024

Abstract The key to fully realizing the potential of high‐entropy alloys (HEAs) lies in balancing their inherent local chemical disordering with long‐range ordering required for electrochemical applications. Herein, we synthesized a distinctive L1 0 ‐(PtIr)(FeMoBi) intermetallics (HEIs) exhibiting nanoscale order and atomic scale short‐range disorder via lattice compensation strategy mitigate entropy reduction tendency. (PtIr)(FeMoBi) catalyst exhibited remarkable activity selectivity glycollic acid (GA) production electrocatalytic waste polymer‐derived ethylene glycol oxidation reaction (EGOR). With mass 5.2 A mg Pt −1 Faradaic efficiency (FE) GA 95 %, it outperformed most previously reported electrocatalysts selective production. lattice‐compensation effect promotes homogeneity Fe actives sites, facilitating co‐adsorption EG OH reducing energy barriers dehydrogenation OH‐combination processes. This approach effectively avoids formation low‐active sites commonly encountered HEA solid solutions, offering promising avenue exploring complex interplay between catalytic HEI structures.

Language: Английский

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Application of platinum-based high-entropy-alloy nanoparticles for electro-oxidation of formic acid and glycerol

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 82, P. 448 - 455

Published: Aug. 2, 2024

Language: Английский

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High-entropy intermetallics: emerging inorganic materials for designing high-performance catalysts

Chemical Science, Journal Year: 2024, Volume and Issue: 15(32), P. 12644 - 12666

Published: Jan. 1, 2024

High-entropy intermetallics have several advantages over disordered high-entropy alloys, e.g. , greater tunability, multifunctionality, structural/thermal stability, more facile site isolation, and precise control of electronic structures.

Language: Английский

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High-entropy alloy nanomaterials for electrocatalysis

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(87), P. 12615 - 12632

Published: Jan. 1, 2024

Synthetic strategies and electrocatalytic applications of high-entropy alloys.

Language: Английский

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Engineering Topological and Chemical Disorder in Pd Sites for Record‐Breaking Formic Acid Electrocatalytic Oxidation

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 13, 2024

Designing palladium-based formic acid oxidation reaction (FAOR) catalysts to achieve significant breakthroughs in catalytic activity, pathway selectivity, and toxicity resistance is both urgent challenging. Here, these challenges are addressed by pioneering a novel catalyst design that incorporates topological chemical disorder, developing new class of PdCuLaYMnW high-entropy amorphous alloys with porous network (Net-Pd-HEAA) as highly active, selective, stable FAOR electrocatalyst. This Net-Pd-HEAA demonstrates record-breaking performance, achieving the mass specific activities 5.94 A mg

Language: Английский

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Catalytic CO−O coupling on high-entropy alloys: A composition optimization dependent on the reaction assumptions

Journal of Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 115983 - 115983

Published: Jan. 1, 2025

Language: Английский

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Enhanced CO-tolerance of Rh-based catalysts by photo-assisted built-in electric field for efficient formic acid oxidation

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125160 - 125160

Published: Feb. 1, 2025

Language: Английский

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A Radical-Assisted Approach to High-Entropy Alloy Nanoparticle Electrocatalysts under Ambient Conditions

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

Published: Feb. 21, 2025

High-entropy alloy (HEA) nanoparticles are rising as promising catalysts but face challenges in both facile synthesis and correlation of the structure with properties. Herein, utilizing highly reductive carbon-centered isopropyl alcohol radicals generated by UV irradiation, we report a simple yet robust wet chemical method to synthesize HEA under ambient conditions. These isopropanol verified electron paramagnetic resonance spectroscopy impose very large overpotentials reduce diverse metal ions into five seven different elements. Specially, PtPdIrRhAuAgCu on reduced electrochemical graphene oxide (rEGO) support (PtPdIrRhAuAgCu-rEGO) demonstrate superior activity for hydrogen evolution reaction (HER) across entire pH range, small 11, 30, 31 mV deliver current density -10 mA cm-2 1 M KOH, phosphate buffer saline, 0.5 H2SO4, respectively. The excellent HER performance PtPdIrRhAuAgCu-rEGO surpasses that commercial Pt/C most contemporary literature. Density functional theory calculations using random structures mimicking disordering confirm its imply possible between d-band centers nearest atoms face-centered cubic hollow site.

Language: Английский

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Enhancing Oxygen Evolution Electrocatalysis in Heazlewoodite: Unveiling the Critical Role of Entropy Levels and Surface Reconstruction

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

Published: April 7, 2025

Abstract Entropy engineering has proven effective in enhancing catalyst electrochemical properties, particularly for the oxygen evolution reaction (OER). Challenges persist, however, modulating entropy and understanding dynamic reconfiguration of high‐entropy sulfides during OER. In this study, an innovative situ corrosion method is introduced to convert low‐valent nickel on a foam substrate into heazlewoodite (HES/NF), significantly boosting OER performance. By synthesizing series low‐, medium‐, heazlewoodites, intrinsic factors influence surface electrocatalytic activity systematically explored. Employing combination ex characterization techniques, it observed that HES/NF dynamically transforms stable hydroxide oxide (MOOH)‐sulfide composite under conditions. This transition, coupled with lattice distortion, optimizes electrostatic potential distribution, ensuring superior catalytic preventing sulfide deactivation through formation HES‐MOOH species. synergy enables achieve remarkably low overpotentials: 172.0 mV at 100.0 mA cm −2 229.0 extreme current density 300.0 . When paired Pt/C cathode, exhibits rapid kinetics, outstanding stability, exceptional water‐splitting The scalable, cost‐effective approach paves way advanced electrocatalyst design, promising breakthroughs energy storage conversion technologies.

Language: Английский

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