p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(31), С. 21357 - 21366

Опубликована: Июль 25, 2024

With more flexible active sites and intermetal interaction, dual-atom catalysts (DACs) have emerged as a new frontier in various electrocatalytic reactions. Constructing typical p-d orbital hybridization between p-block d-block metal atoms may bring avenues for manipulating the electronic properties thus boosting activities. Herein, we report distinctive heteronuclear dual-metal atom catalyst with asymmetrical FeSn dual embedded on two-dimensional C2N nanosheet (FeSn–C2N), which displays excellent oxygen reduction reaction (ORR) performance half-wave potential of 0.914 V an alkaline electrolyte. Theoretical calculations further unveil powerful stannum ferrum sites, triggers electron delocalization lowers energy barrier *OH protonation, consequently enhancing ORR activity. In addition, FeSn–C2N-based Zn–air battery provides high maximum power density (265.5 mW cm–2) specific capacity (754.6 mA h g–1). Consequently, this work validates immense along perception into logical design DACs.

Язык: Английский

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High-efficient OER/ORR bifunctional electrocatalyst based on single transition-metal anchored Graphynes: Key descriptors under acceptance-backdonation mechanism framework

Applied Surface Science, Год журнала: 2025, Номер unknown, С. 162482 - 162482

Опубликована: Янв. 1, 2025

Язык: Английский

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Engineering TM–N₂@C₁₅N₅S₃H₅-Based Covalent-Organic Frameworks for Enhanced Water-Splitting and Oxygen Reduction Reactions: A Constant Potential and Feature Coevaluation Approach

Langmuir, Год журнала: 2025, Номер unknown

Опубликована: Март 11, 2025

The development of highly active metal-based single-atom catalysts (SACs) is crucial for energy conversion and storage, offering optimized atom utilization high catalytic activity, with bifunctional SACs hydrogen evolution (HER) oxygen evolution/reduction (OER/ORR) reactions providing greater efficiency cost-effectiveness than monofunctional catalysts, making them scientifically economically valuable. By integrating density functional theory machine learning methods, we systematically evaluated the potential TM–N2@C15N5S3H5 monolayers as efficient HER/OER/ORR revealing that 27 TM atoms remain stable on N2@C15N5S3H5 a TM–N2 coordination environment. Rh–N2@C15N5S3H5 outperforms Pt in HER, while drives both HER OER, Ni–N2@C15N5S3H5 catalyzes OER ORR, catalysts. Comparative activity analysis reveals Ni-d orbitals interact O-p orbitals, pairing up electrons from antibonding states into downward bonding thus fitting OH* adsorption enhancing performance. We further examined pH applied effects OER/ORR performance monolayers, show enhanced acidic conditions, excelling ORR under alkaline conditions conditions. Moreover, techniques were to explore correlation between range structural atomic properties.

Язык: Английский

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Black phosphorus nanodots-modified Pt/C electrocatalyst for methanol-tolerant oxygen reduction in direct methanol fuel cells

Rare Metals, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 8, 2024

Язык: Английский

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