Constructing Asymmetrical Coordination Microenvironment with Phosphorus‐Incorporated Nitrogen‐Doped Carbon to Boost Bifunctional Oxygen Electrocatalytic Activity

Advanced Functional Materials, Год журнала: 2024, Номер 34(18)

Опубликована: Янв. 17, 2024

Abstract Carbon‐based metal‐free electrocatalysts have been recognized as inexpensive alternatives to afford excellent activity in oxygen reduction/evolution reactions (ORR/OER). Nevertheless, precisely identifying the local active sites and tailoring corresponding electronic properties enhance reaction kinetics remain challenging. Herein, a facile strategy create electrocatalyst comprised of mesoporous nitrogen‐doped carbon matrix with phosphorus incorporation (NPC) is described. The as‐prepared NPC‐950 demonstrates superior ORR under alkaline acidic conditions half‐wave potentials 0.88 0.72 V, respectively, comparable commercial Pt/C (0.85 0.76 V) overwhelmingly other N‐doped catalyst materials. In addition, remarkable promotion OER observed. Notably, zinc–air battery equipped this NCP‐950 exhibits exceptional performance peak power density, specific capacity, long‐term operation durability. Theoretical calculations uncover that NC material results effective charge density redistribution, thus modulating achieve optimum adsorption desorption intermediates. work provides deep understanding heteroatom‐doped materials highlights importance modulation bifunctional electrocatalytic activity.

Язык: Английский

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Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Фев. 28, 2024

Abstract The development of facile tailoring approach to adjust the intrinsic activity and stability atomically-precise metal nanoclusters catalysts is great interest but remians challenging. Herein, well-defined Au 8 modified by single-atom sites are rationally synthesized via a co-eletropolymerization strategy, in which uniformly dispersed nanocluster co-entrenched on poly-carbazole matrix. Systematic characterization theoretical modeling reveal that functionalizing single-atoms enable altering electronic structures clusters, amplifies their electrocatalytic reduction CO 2 ~18.07 fold compared isolated clusters. rearrangements structure not only strengthen adsorption key intermediates *COOH, also establish favorable reaction pathway for reaction. Moreover, this strategy fixing cross-linked polymer networks efficiently deduce performance deactivation caused agglomeration during catalytic process. This work contribute explore improvement

Язык: Английский

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Construction of Fe Nanoclusters/Nanoparticles to Engineer FeN₄ Sites on Multichannel Porous Carbon Fibers for Boosting Oxygen Reduction Reaction

Advanced Functional Materials, Год журнала: 2024, Номер 34(23)

Опубликована: Янв. 15, 2024

Abstract Fe–N–C catalysts are emerging as promising alternatives to Pt‐based for the oxygen reduction reaction (ORR), while they still suffer from sluggish kinetics due discontented binding affinity between Fe‐N 4 sites and oxygen‐containing intermediates, unsatisfactory stability. Herein, a flexible multichannel carbon fiber membrane immobilized with atomically dispersed neighboring Fe nanoclusters/nanoparticles (FeN ‐Fe NCP @MCF) is synthesized. The optimized geometric electronic structures of atomic brought by adjacent hierarchically porous structure matrix endow FeN @MCF outstanding ORR activity stability, considerably outperforming its counterpart only commercial Pt/C catalyst. Liquid solid‐state zinc–air batteries employing both exhibit durability. Theoretical calculation reveals that nanoclusters can trigger remarkable electron redistribution modulate hybridization central 3 d O 2 p orbitals, facilitating activation molecules optimizing adsorption capacity intermediates on sites, thus accelerating kinetic. This work offers an effective approach constructing coupling have single atoms coexisting efficient catalysis.

Язык: Английский

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Precisely constructing charge-asymmetric dual-atom Fe sites supported on hollow porous carbon spheres for efficient oxygen reduction

Energy & Environmental Science, Год журнала: 2024, Номер 17(13), С. 4646 - 4657

Опубликована: Янв. 1, 2024

Transition group metal catalysts showing atomic dispersion are on the rise as affordable electrocatalysts for oxygen reduction reaction (ORR) in fuel cell batteries, but their activity acidic media remains constrained.

Язык: Английский

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Boosting ORR/OER bifunctional electrocatalysis by promoting electronic redistribution of Fe-N-C on CoFe-FeNC for ultra-long rechargeable Zn-air batteries

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 359, С. 124485 - 124485

Опубликована: Авг. 8, 2024

Язык: Английский

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Boosted electrocatalytic activity and durability of Cu Fe/N C by modulating the interfacial composition and electronic structure for efficient oxygen reduction reaction

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 677, С. 771 - 780

Опубликована: Авг. 5, 2024

Язык: Английский

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Precise synthesis of dual atom sites for electrocatalysis

Nano Research, Год журнала: 2024, Номер unknown

Опубликована: Сен. 17, 2024

Язык: Английский

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Termination-acidity tailoring of molybdenum carbides for alkaline hydrogen evolution reaction

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 6, 2025

Transition-metal carbides have been advocated as the promising alternatives to noble-metal platinum-based catalysts in electrocatalytic hydrogen evolution reaction over half a century. However, effectiveness of transition-metal catalyzing high-pH electrolyte is severely compromised due lowered proton activity and intractable alkaline-leaching issue centers. Herein, on basis validation molybdenum-carbide model-catalyst system by taking advantage surface science techniques, Mo2C micro-size spheres terminated Al3+ doped MoO2 layer exhibit notable performance alkaline with near-zero onset-potential, low overpotential (40 mV) at typical current density 10 mA/cm2, small Tafel slope (45 mV/dec), well long-term stability for continuous production 200 h. Advanced morphology spectroscopy characterizations demonstrate that local -Al-OH-Mo- structures within Al-MoO2 terminations serve strong Brønsted acid sites accelerate deprotonation kinetics HER process. Our work paves an interesting termination-acidity-tailoring strategy explore cost-effective towards water electrolysis beyond. Exploring low-cost, efficient replace platinum crucial generation. Here, authors report termination-acidity boosts molybdenum carbides, achieving sustaining generation

Язык: Английский

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Single-atom sites combined with metal nano-aggregates for efficient electrocatalysis

Energy & Environmental Science, Год журнала: 2023, Номер 16(12), С. 5663 - 5687

Опубликована: Янв. 1, 2023

This review summarizes recent progress and prospects of catalysts containing metal single-atom (M 1 ) nano-aggregates (MNAs, particles or clusters), which promise to combine the merits SACs MNA-based for efficient electrocatalysis.

Язык: Английский

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Regulating Atomically‐Precise Pt Sites for Boosting Light‐Driven Dry Reforming of Methane

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(46)

Опубликована: Авг. 12, 2024

Abstract Light‐driven dry reforming of methane is a promising and mild route to convert two greenhouse gas into valuable syngas. However, developing facile strategy atomically‐precise regulate the active sites realize balanced stable syngas production still challenging. Herein, we developed spatial confinement approach precisely control over platinum species on TiO 2 surfaces, from single atoms nanoclusters. The configuration comprising sub‐nanoclusters engenders pronounced electronic metal‐support interactions, with resultant interfacial states prompting surface charge rearrangement. unique geometric properties these atom‐cluster assemblies facilitate effective activation CH 4 CO , accelerating intermediate coupling minimizing side reactions. Our catalyst exhibits an outstanding generation rate 34.41 mol g Pt −1 h superior durability, displaying high apparent quantum yield 9.1 % at 365 nm turnover frequency 1289 . This work provides insightful understanding for exploring more multi‐molecule systems atomic scale.

Язык: Английский

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