Fe/Cu diatomic sites dispersed on nitrogen-doped mesoporous carbon for the boosted oxygen reduction reaction in Mg-air and Zn-air batteries

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124450 - 124450

Published: July 27, 2024

Language: 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, Journal Year: 2024, Volume and Issue: 34(23)

Published: Jan. 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.

Language: Английский

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Revealing the Active Sites in Atomically Dispersed Multi‐Metal–Nitrogen–Carbon Catalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: Jan. 30, 2024

Abstract Atomically dispersed metal‐nitrogen‐carbon catalysts have been extensively explored for various sustainable energy‐related reactions. From a material perspective, these are likely to consist of combination single‐atom, dual‐atom and possibly even multi‐atom sites. However, pinpointing their true active sites has remained challenging task. In this study, model catalyst is introduced, Co/CoMn‐NC, featuring both Co single‐atom CoMn on nitrogen‐doped carbon substrate. By employing X‐ray adsorption spectroscopy density functional theory calculations, the atomic configuration Co/CoMn‐NC determined. Density calculations also used unequivocally identify Co‐atom within motif as predominate site toward oxygen reduction reaction (ORR), which further confirmed by in situ Raman spectroscopy. The cooperative interactions between can finely tune d‐band center ameliorate desorption behaviors intermediates, thereby facilitating ORR kinetic. Overall, study introduces systematic strategy elucidate structure superiority system provides new insights into atomically multi‐metal sites, showcasing that enhanced catalytic performance extends beyond unified diatomic or monatomic

Language: Английский

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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Feb. 29, 2024

Abstract The exploration of sustainable energy utilization requires the implementation advanced electrochemical devices for efficient conversion and storage, which are enabled by usage cost-effective, high-performance electrocatalysts. Currently, heterogeneous atomically dispersed catalysts considered as potential candidates a wide range applications. Compared to conventional catalysts, metal atoms in carbon-based have more unsaturated coordination sites, quantum size effect, strong metal–support interactions, resulting exceptional catalytic activity. Of these, dual-atomic (DACs) attracted extensive attention due additional synergistic effect between two adjacent atoms. DACs advantages full active site exposure, high selectivity, theoretical 100% atom utilization, ability break scaling relationship adsorption free on sites. In this review, we summarize recent research advancement DACs, includes (1) comprehensive understanding synergy atomic pairs; (2) synthesis DACs; (3) characterization methods, especially aberration-corrected scanning transmission electron microscopy synchrotron spectroscopy; (4) energy-related last part focuses great catalysis small molecules, such oxygen reduction reaction, CO 2 hydrogen evolution N reaction. future challenges opportunities also raised prospective section.

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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Research progress of Zn-air batteries suitable for extreme temperatures

Energy storage materials, Journal Year: 2024, Volume and Issue: 69, P. 103429 - 103429

Published: April 23, 2024

Language: 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, Journal Year: 2024, Volume and Issue: 17(13), P. 4646 - 4657

Published: Jan. 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.

Language: 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, Journal Year: 2024, Volume and Issue: 359, P. 124485 - 124485

Published: Aug. 8, 2024

Language: Английский

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Salt Effect Engineering Single Fe‐N₂P₂‐Cl Sites on Interlinked Porous Carbon Nanosheets for Superior Oxygen Reduction Reaction and Zn‐Air Batteries

Advanced Science, Journal Year: 2024, Volume and Issue: 11(12)

Published: Jan. 15, 2024

Abstract Developing efficient metal‐nitrogen‐carbon (M‐N‐C) single‐atom catalysts for oxygen reduction reaction (ORR) is significant the widespread implementation of Zn‐air batteries, while synergic design matrix microstructure and coordination environment metal centers remains challenges. Herein, a novel salt effect‐induced strategy proposed to engineer N P coordinated atomically dispersed Fe atoms with extra‐axial Cl on interlinked porous carbon nanosheets, achieving superior catalyst (denoted as Fe‐NP‐Cl‐C) ORR batteries. The hierarchical nanosheet architecture can provide rapid mass/electron transfer channels facilitate exposure active sites. Experiments density functional theory (DFT) calculations reveal distinctive Fe‐N 2 ‐Cl sites afford significantly reduced energy barriers promoted kinetics ORR. Consequently, Fe‐NP‐Cl‐C exhibits distinguished performance half‐wave potential (E 1/2 ) 0.92 V excellent stability. Remarkably, assembled battery based delivers an extremely high peak power 260 mW cm −2 large specific capacity 812 mA h g −1 , outperforming commercial Pt/C most reported congeneric catalysts. This study offers new perspective structural optimization engineering electrocatalysis conversion devices.

Language: Английский

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Tailoring First Coordination Sphere of Dual‐Metal Atom Sites Boosts Oxygen Reduction and Evolution Activities

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(28)

Published: Feb. 24, 2024

Abstract It is important to tune the coordination configuration of dual‐atom catalyst (DAC), especially in first sphere, render high intrinsic catalytic activities for oxygen reduction/evolution reactions (ORR/OER). Herein, a type atomically dispersed and boron‐coordinated DAC structure, namely, FeN 4 B‐NiN B dual sites, reported. In this incorporation boron into sphere /NiN atomic sites regulates its geometry electronic structure by forming “Fe‐B‐N” “Ni‐B‐N” bridges. The exhibits much enhanced ORR OER property compared ‐NiN counterparts. Density functional theory calculations reveal that boron‐induced charge transfer asymmetric distributions central Fe/Ni atoms optimize adsorption desorption behavior ORR/OER intermediates reduce activation energy potential‐determining step. Zinc‐air batteries employing cathode exhibit maximum power density (236.9 mW cm −2 ) stable cyclability up 1100 h. result illustrates pivotal role first‐coordination DACs tuning electrochemical conversion storage activities.

Language: Английский

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