Maneuver of the d-orbital spin polarization of Fe single atomic sites via a near-range axial ligand effect for boosting oxygen reduction reaction

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125007 - 125007

Опубликована: Янв. 1, 2025

Язык: Английский

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Engineering the Lewis Acidity of Fe Single-Atom Sites via Atomic-Level Tuning of Spatial Coordination Configuration for Enhanced Oxygen Reduction

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 16, 2025

Nitrogen-doped carbon-supported Fe catalysts (Fe-N-C) with Fe-N4 active sites hold great promise for the oxygen reduction reaction (ORR). However, fine-tuning structure of to enhance their performance remains a grand challenge. Herein, we report an innovative design strategy promote ORR activity and kinetics by engineering Lewis acidity, which is achieved tuning spatial coordination geometry. Theoretical calculations indicated that Fe1-N4SO2 (with axial –SO2 group bonded Fe) offered favorable acidity ORR, leading optimized adsorption energies key intermediates. To implement this strategy, developed molecular-cage-encapsulated synthesize single-atom site catalyst (SAC) sites. In agreement theory, Fe1-N4SO2/NC demonstrated outstanding in both alkaline (E1/2 = 0.910 V 0.1 M KOH) acidic media 0.772 HClO4), surpassing commercial Pt/C traditional SACs Fe1-N4 or planar S-coordinated Fe1-N4-S Moreover, newly showed application potential quasi-solid-state Zn–air batteries, delivering superior across wide temperature range.

Язык: Английский

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Probing the synergistic effect of metal–organic framework derived Co-Nx rich interwoven hierarchical porous carbon tube encapsulated dual redox active nanoalloy for high-performance Zn-air battery and supercapacitor applications

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 683, С. 818 - 832

Опубликована: Дек. 18, 2024

Язык: Английский

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Molecular Nanojunction Catalyst for Oxygen Evolution Reaction

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 26, 2025

Abstract Achieving close integration and strong electronic communication between molecular catalysts conductive substrates is crucial for developing the stability catalytic activity of nanomaterials. However, constructing heterostructure catalyst usually need complex demanding synthesis processes. Herein, a facile universal “molecular nanojunction” strategy developed to prepare with high by improving coplanarity nanojunction facilitating efficient electron transfer. The density function theory (DFT) calculations in situ characterization indicate that reduces excessive * OH adsorption accelerates deprotonation process, thereby promoting oxygen generation. shows better evolution reaction (OER) performance than most reported catalysts. What's more, are applied alkaline anion exchange membrane (AEM) electrolysis cells, exhibiting excellent performance.

Язык: Английский

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Functional additives for proton exchange membrane fuel cells

EnergyChem, Год журнала: 2025, Номер unknown, С. 100144 - 100144

Опубликована: Янв. 1, 2025

Язык: Английский

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Turn the Harm into A Benefit: Axial Cl Adsorption on Curved Fe‐N₄ Single Sites for Boosted Oxygen Reduction Reaction in Seawater

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 26, 2025

Abstract Seawater electrocatalysis is urgently needed for various energy storage and conversion systems. However, the adsorption of chloride ions (Cl − ) to active sites can degrade oxygen reduction reaction (ORR) activity stability, thus reducing catalytic performance. In this paper, a curved FeN 4 single atomic structure designed by utilizing curvature engineering, which turns harmful Cl into benefit on Fe site that changes rate determining step ORR reduces overall barrier according density functional theory (DFT) calculation. Experimental studies reveal prepared highly‐curved single‐atom iron catalyst (HC‐Fe SA exhibits excellent in different electrolytes, with half‐wave potentials 0.90 V 0.1 M KOH, simulated seawater, 0.75 natural respectively. This work opens up an avenue synthesis high‐performance seawater‐based catalysts through regulating local curvature.

Язык: Английский

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Constructing Pentagonal Topological Defects in Carbon Aerogels for Flexible Zinc‐Air Batteries

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 16, 2025

Abstract In the context of energy conversion, design and synthesis high‐performance metal‐free carbon electrocatalysts for oxygen reduction reaction (ORR) is crucial. Herein, a one‐step nitrogen doping/extraction strategy proposed to fabricate 3D nitrogen‐doped aerogels (NCA‐Cl) with rich pentagonal topological defects. The NCA‐Cl electrocatalyst exhibits superb ORR activity, displaying half‐wave potential 0.89 V vs RHE 0.74 under alkaline (0.1 m KOH) acidic HClO 4 ) media, respectively, thanks balanced * OOH intermediate adsorption desorption induced by defects dopants. aqueous zinc‐air battery (ZAB) equipped cathode delivers peak power density 206.6 mW cm −2 , specific capacity 810.6 mAh g −1 durability 400 h, flexible ZAB also performed convincingly. This work provides an effective formation enhancement electrocatalytic activity carbon‐based catalysts.

Язык: Английский

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Fundamental Mechanistic Insights on the Peripherally Substituted Iron Phthalocyanine Selectively Catalyzing the Sulfur Redox Reactions

Energy storage materials, Год журнала: 2025, Номер unknown, С. 104157 - 104157

Опубликована: Март 1, 2025

Язык: Английский

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Unsaturation degree of Fe single atom site manipulates polysulfide behavior in sodium-sulfur batteries

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

Опубликована: Март 21, 2025

Sodium | |sulfur batteries hold great promise for grid-scale energy storage, yet their performance is hindered by the shuttling and sluggish redox of sulfur species. Herein, we report a strategic design hosts modified with coordinatively unsaturated iron single-atom (Fe‒Nx) sodium batteries. Utilizing theoretical calculations, geometric descriptor γ (lNa‒S/lFe‒N) electronic φ (eg /t2g) simultaneously correlated unsaturation degree Fe‒Nx site are proposed. A negative correlation between adsorption strength polysulfides, along positive decomposition capability Na2S established. The Fe‒N1 sites, minimum maximum values, identified as optimal functional species optimizing polysulfides behaviors. utilizing /S electrodes deliver improved utilization (81.4% at 167.5 mA g‒1), sustained rate (1003.0 mAh g‒1 1675 stable cycling (83.5% retention over 450 cycles 3350 g‒1). Moreover, Fe‒N1/S enable pouch cells to 77.4% (1296.9 g‒1) 0.1 g‒1. Our work offers strategy designing high-activity, fast validates practical potential Sodium-sulfur S authors propose descriptors concomitantly coordinative Fe single atoms engineer highly active robust electrode Na-S

Язык: Английский

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Carbon nanotube supported iron phthalocyanine providing efficient electron transfer pathway for water decontamination

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125303 - 125303

Опубликована: Март 1, 2025

Язык: Английский

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