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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Recent advances of metal suboxide catalysts for carbon‐neutral energy applications

EcoEnergy, Год журнала: 2024, Номер 2(1), С. 45 - 82

Опубликована: Фев. 22, 2024

Abstract Metal suboxides have emerged as a class of promising candidates for many electrocatalytic applications owing to their enhanced electrical conductivity and chemical activities. In this review, we summarized the recent progress metal suboxides. We firstly introduced discovery suboxides, categories according element tables. Then various synthetic methods been systematically illustrated involving solid‐state synthesis, high‐temperature low‐temperature synthesis plasma‐driven methods, etc. addition, demonstrated in field water, carbon nitrogen cycle‐based energy catalysis technologies electrochemical hydrogen evolution reaction, oxygen reduction dioxide reduction, urea oxidation methanol reaction nitrate Finally, make brief conclusion about developments giving an outlook future research challenges. These insights are expected hold promise developing suboxide catalysts toward practical applications.

Язык: Английский

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Sulfur‐Bridged Asymmetric CuNi Bimetallic Atom Sites for CO₂ Reduction with High Efficiency

Advanced Materials, Год журнала: 2024, Номер 36(33)

Опубликована: Июнь 25, 2024

Abstract Double‐atom catalysts (DACs) with asymmetric coordination are crucial for enhancing the benefits of electrochemical carbon dioxide reduction and advancing sustainable development, however, rational design DACs is still challenging. Herein, this work synthesizes atomically dispersed novel sulfur‐bridged Cu‐S‐Ni sites (named Cu‐S‐Ni/SNC), utilizing biomass wool keratin as precursor. The plentiful disulfide bonds in overcome limitations traditional gas‐phase S ligand etching process enable one‐step formation S‐bridged sites. X‐ray absorption spectroscopy (XAS) confirms existence bimetallic N 2 Cu‐S‐NiN moiety. In H‐cell, Cu‐S‐Ni/SNC shows high CO Faraday efficiency 98.1% at −0.65 V versus RHE. Benefiting from charge tuning effect between metal site bridged sulfur atoms, a large current density 550 mA cm −2 can be achieved −1.00 flow cell. Additionally, situ XAS, attenuated total reflection surface‐enhanced infrared (ATR‐SEIRAS), functional theory (DFT) calculations show Cu main adsorption dual‐regulated by Ni which enhances activation accelerates *COOH intermediates. This kind atom may open new pathways precision preparation performance regulation atomic materials toward energy applications.

Язык: Английский

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Breaking symmetry for better catalysis: insights into single-atom catalyst design

Chemical Society Reviews, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This review examines the strategies of symmetry breaking (charge/coordination/geometric) in single-atom catalysts to regulate active site electronic structures, greatly enhancing catalytic performance.

Язык: Английский

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Achieving Negatively Charged Pt Single Atoms on Amorphous Ni(OH)2 Nanosheets with Promoted Hydrogen Absorption in Hydrogen Evolution

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Май 23, 2024

Single-atom (SA) catalysts with nearly 100% atom utilization have been widely employed in electrolysis for decades, due to the outperforming catalytic activity and selectivity. However, most of reported SA are fixed through strong bonding between dispersed single metallic atoms nonmetallic substrates, which greatly limits controllable regulation electrocatalytic catalysts. In this work, Pt-Ni bonded Pt catalyst adjustable electronic states was successfully constructed a electrochemical reduction on coordination unsaturated amorphous Ni(OH)

Язык: Английский

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Enhanced N₂ Adsorption and Activation by Combining Re Clusters and In Vacancies as Dual Sites for Efficient and Selective Electrochemical NH₃ Synthesis

Nano Letters, Год журнала: 2024, Номер 24(2), С. 748 - 756

Опубликована: Янв. 3, 2024

The electrochemical N2 reduction reaction (NRR) is a green and energy-saving sustainable technology for NH3 production. However, high activity selectivity can hardly be achieved in the same catalyst, which severely restricts development of NRR. In2Se3 with partially occupied p-orbitals suppress H2 evolution (HER), shows excellent presence VIn simultaneously provide active sites confine Re clusters through strong charge transfer. Additionally, well-isolated stabilized on by confinement effect result Re-VIn maximum availability. By combining as dual spontaneous adsorption activation, NRR performance enhanced significantly. As result, Re-In2Se3-VIn/CC catalyst delivers yield rate (26.63 μg h–1 cm–2) FEs (30.8%) at −0.5 V vs RHE.

Язык: Английский

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MXene‐Bimetallic Hybrids via Mixed Molten Salts Etching for Kinetics‐Enhanced and Dendrite‐Free Lithium–Sulfur Batteries

Small, Год журнала: 2024, Номер 20(34)

Опубликована: Апрель 9, 2024

Lithium-sulfur (Li-S) batteries with high theoretical energy density (2600 Wh kg

Язык: Английский

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Lattice Strain and Mott–Schottky Effect of the Charge-Asymmetry Pd₁Fe Single-Atom Alloy Catalyst for Semi-Hydrogenation of Alkynes with High Efficiency

ACS Nano, Год журнала: 2024, Номер 18(20), С. 13286 - 13297

Опубликована: Май 10, 2024

The ideal interface design between the metal and substrate is crucial in determining overall performance of alkyne semihydrogenation reaction. Single-atom alloys (SAAs) with isolated dispersed active centers are media for study reaction effects. Herein, a charge-asymmetry "armor" SAA (named Pd1Fe SAA@PC), which consists alloy core semiconducting P-doped C (PC) shell, rationally designed as an catalyst selective hydrogenation alkynes high efficiency. Multiple spectroscopic analyses density functional theory calculations have demonstrated that SAA@PC dual-regulated by lattice tensile Schottky effects, govern selectivity activity hydrogenation, respectively. (1) PC shell layer applied external traction force causing 1.2% strain inside to increase selectivity. (2) P doping into C-shell realized transition from p-type semiconductor n-type semiconductor, thereby forming unique junction advancing activity. dual regulation effect ensures excellent phenylethylene, achieving conversion rate 99.9% 98.9% at 4 min. These well-defined modulation strategies offer practical approach rational optimization catalysts.

Язык: Английский

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Transient heating synthesis of a highly ordered Ga–Cu intermetallic antiperovskite for efficient ammonia electrosynthesis and ultrastable zinc–nitrate fuel cells

Energy & Environmental Science, Год журнала: 2024, Номер 17(18), С. 6698 - 6706

Опубликована: Янв. 1, 2024

Strong p–d intermetallic hybridization was performed to construct an ordered antiperovskite via transient heating strategy, exhibiting high and stable electrochemical activity in both ammonia synthesis zinc–nitrate battery.

Язык: Английский

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Asymmetric Sn-O-Mn structures enhance Mn eg-O 2p orbital hybridization in MnO2 for efficient hybrid capacitive deionization

Separation and Purification Technology, Год журнала: 2025, Номер unknown, С. 131679 - 131679

Опубликована: Янв. 1, 2025

Язык: Английский

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