Oxygenate-induced structural evolution of high-entropy electrocatalysts for multifunctional alcohol electrooxidation integrated with hydrogen production

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(30)

Published: July 16, 2024

High-entropy compounds have been emerging as promising candidates for electrolysis, yet their controllable electrosynthesis strategy remains a formidable challenge because of the ambiguous ionic interaction and codeposition mechanism. Herein, we report oxygenates directionally induced electrodeposition to construct high-entropy materials with amorphous features, on which structural evolution from phosphide oxide is confirmed by introducing vanadate, thus realizing simultaneous optimization composition structure. The representative P-CoNiMnWVO x shows excellent bifunctional catalytic performance toward alkaline hydrogen reaction ethanol oxidation (EOR), small potentials −168 mV 1.38 V at 100 mA cm −2 , respectively. In situ spectroscopy illustrates that electrochemical reconstruction induces abundant Co–O species main active EOR follows conversion pathway C 2 product. Theoretical calculations reveal optimized electronic structure adsorption free energy intermediates thereby resulting in facilitated kinetic process. A membrane-free electrolyzer delivers both high Faradaic efficiencies acetate H over 95% superior stability at100 during 120 h electrolysis. addition, unique advantages endow multifunctional activity realize multipathway formate-coupled production.

Language: Английский

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High Entropy Oxides: Mapping the Landscape from Fundamentals to Future Vistas

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(8), P. 3694 - 3718

Published: July 5, 2024

High-entropy materials (HEMs) are typically crystalline, phase-pure and configurationally disordered that contain at least five elements evenly blended into a solid-solution framework. The discovery of high-entropy alloys (HEAs) oxides (HEOs) disrupted traditional notions in science, providing avenues for the exploration new materials, property optimization, pursuit advanced applications. While there has been significant research on HEAs, creative breakthroughs HEOs still being revealed. This focus review aims developing structured framework expressing concept HEM, with special emphasis crystal structure functional properties HEOs. Insights recent synthetic advances, foster prospective outcomes their current applications electrocatalysis, battery, comprehensively discussed. Further, it sheds light existing constraints HEOs, highlights adoption theoretical experimental tools to tackle challenges, while delineates potential directions energy application.

Language: Английский

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Synthesis Strategies for High Entropy Nanoparticles

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

Published: Oct. 30, 2024

Abstract Nanoparticles (NPs) of high entropy materials (HEMs) have attracted significant attention due to their versatility and wide range applications. HEM NPs can be synthesized by fragmenting bulk HEMs or disintegrating recrystallizing them. Alternatively, directly producing in NP form from atomic/ionic/molecular precursors presents a challenge. A widely adopted strategy involves thermodynamically driving formation leveraging the entropic contribution but incorporating strategies limit growth at elevated temperatures used for maximizing entropy. second approach is kinetically drive promoting rapid reactions homogeneous reactant mixtures using highly diluted precursor dissolutions. Additionally, experimental evidence suggests that enthalpy plays role processes moderate temperatures, with energy cost generating additional surfaces interfaces nanoscale stabilizing phase. This review critically assesses various synthesis developed preparation, highlighting key illustrative examples offering insights into underlying mechanisms. Such are critical fine‐tuning conditions achieve specific outcomes, ultimately enabling effective optimized generations these advanced both current emerging applications across scientific technological fields.

Language: Английский

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Plasma‐Induced Geometry Engineering in High‐Entropy Oxide Composites for Superior Electromagnetic Absorption

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

Published: Feb. 13, 2025

Abstract The dielectric and magnetic coexistence behavior of high entropy oxides (HEOs) injects infinite dynamism in promoting electromagnetic wave (EMW) absorption, but precisely constructing their regular geometries at the nanoscale remains challenging. Herein, controlled preparation reduced graphite oxide loaded (CoFeNiCuMn)O with various by a rapid plasma process is reported. Modifying only metal content precursor can effectively influence morphology properties resulting derivatives, achieving well‐matched impedance ensuring outstanding absorption performance. results show that truncated octahedral HEO/RGO composite exhibits strongest absorbing capacity, minimum reflection loss −57 dB 14.1 GHz corresponding effective bandwidth covering 4.13 GHz. Moreover, constitutive relationship between multi‐element synergies microwave characteristics systematically explored, mechanism proposed. Delayed wireless charging time simulated values RCS less than −10 dBm 2 whole detection angles further demonstrate its dissipation capability practical application scenarios. This study not enriches variety lightweight efficient materials also guides for new configuration design HEOs.

Language: Английский

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The effect of particle size on structural and catalysts for oxygen evolution reaction of (CoFeNiMnCr)3O4 prepared by controlled synthesis with polyvinylpyrrolidone (PVP)

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 680, P. 818 - 831

Published: Nov. 12, 2024

Language: Английский

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La(FeCuMnMgTi)O₃ High-Entropy Oxide Nanoparticles as Highly Efficient Catalysts for Solvent-Free Aerobic Oxidation of Benzyl Alcohol

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(30), P. 7577 - 7583

Published: July 18, 2024

In this work, a solid-state method for the synthesis of perovskite La(FeCuMnMgTi)O3 high-entropy oxide (HEO) nanoparticles is detailed. Additionally, high performance these as catalysts in aerobic and solvent-free oxidation benzyl alcohol demonstrated. The structural features HEO are studied by X-ray diffraction high-resolution transmission electron microscopy. demonstrate excellent conversion rates selectivity benzaldehyde, reaching 10.6% 52.8% after reaction only 4 h ≤75.6% 24 h. addition, as-prepared catalyst displays robust stability oxidation. Density functional theory calculations that adsorption energy benzaldehyde on surface lower than benzoic acid. This, turn, hinders gradual to acid retains main product.

Language: Английский

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Cold Gas Dynamic Additive Spraying of Al-Matrix Composites Coatings Reinforced by High-Entropy Oxides

Transactions of the Indian Institute of Metals, Journal Year: 2025, Volume and Issue: 78(3)

Published: Jan. 24, 2025

Language: Английский

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Electrocatalytic Reduction of CO₂ to Long-Chain Hydrocarbons on (FeCoNiCu)₃O₄ Medium Entropy Oxide Nanoparticles

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 4196 - 4204

Published: April 20, 2025

Electrocatalytic CO2 reduction reaction (CO2RR) to valuable multicarbon (C2+) fuels and chemicals presents a promising strategy mitigate atmospheric accumulation promote the closure of carbon cycle. However, significant challenges persist in achieving both high product selectivity sustained stability CO2RR. In this study, catalytic performance (Fe,Co,Ni,Cu)3O4 medium entropy oxide (MEO) nanoparticles anchored on reduced graphene (rGO) was evaluated for The MEO-rGO catalyst exhibited remarkable activity, cathodic current density -0.5 A cm-2 at -1.7 V, significantly outperforming bare nickel foam (-0.15 cm-2). Additionally, demonstrated total Faradaic efficiency (FE) 60.3% C2+ products, comprising 30.6% C5H12O 29.7% C5H10O. This exceptional toward long-chain hydrocarbons is attributed enhanced C-C coupling surface, facilitated by energy barriers. Density functional theory (DFT) calculations further revealed that adsorption MEO surface are energetically favorable processes.

Language: Английский

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Oriented Catalysis through Chaos: High-Entropy Spinels in Heterogeneous Reactions

Chemical Science, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 27, 2024

This review provides an overview of the advances in high entropy spinel oxides diverse catalytic reactions and highlights intrinsic structure–property–performance relationships.

Language: Английский

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High-Entropy Oxides derived Cu catalyst for enhanced dehydrogenation of cyclohexanol coupling with hydrogenation of acetone

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

A reduced Cu 0.75 Zn 0.15 Mg 7.1 Al 1 Sc O 11 -HEO catalyst was highly active and stable for the dehydrogenation of cyclohexanol, conversion cyclohexanol could be evidently enhanced when acetone used as solvent and/or hydrogen acceptor.

Language: Английский

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