Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

Advanced Materials, Год журнала: 2024, Номер 36(38)

Опубликована: Июль 31, 2024

Abstract Aqueous zinc–iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost‐effectiveness, and scalability. However, the inadequate redox kinetics severe shuttling effect of polyiodide ions impede commercial viability. Herein, several Zn‐MOF‐derived porous carbon materials designed, further preparation iron–doped (Fe–N–C, M9) with varied Fe doping contents is optimized based on a facile self‐assembly/carbonization approach. M9, atomic coordinated nitrogen atoms, employed as an efficient cathode host AZIBs. Functional modifications hosts involving species levels investigated. The adsorption tests, in situ Raman spectroscopy, UV–vis results demonstrate capability charge‐discharge mechanism iodine species. Furthermore, experimental findings theoretical analyses have proven that conversion enhanced through physicochemical confinement effect. This study offers basic principles strategic design single‐atom dispersed high‐performance Flexible soft–pack battery wearable microbattery applications also implications future long‐life aqueous designs.

Язык: Английский

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Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc‐Air Batteries

Advanced Materials, Год журнала: 2024, Номер 36(44)

Опубликована: Сен. 16, 2024

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity stability is a crucial, yet challenging step to achieving conversion. Here, an approach address this issue: synthesis atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over porous, defect‐containing nitrogen‐doped carbon support, described. Through incorporation phosphorus atom into the second coordination sphere iron, durability boundaries catalyst pushed unprecedented level alkaline environments, such as those found zinc‐air battery. The rationale delicately incorporate P heteroatoms defects close central metal sites (FeN 4 ‐OH) order break local symmetry electronic distribution. This enables suitable binding strength oxygenated intermediates. In situ characterizations theoretical studies demonstrate that these synergetic interactions responsible for stability. These intrinsic advantages /NCP enable potential gap mere 0.65 V power density 263.8 mW cm −2 when incorporated findings underscore importance design principles access high‐performance green

Язык: Английский

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Spin Engineering of Fe─N─C by Axial Ligand Modulation for Enhanced Bifunctional Oxygen Catalysis

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 17, 2024

Abstract Iron‐based single‐atom catalysts (Fe─N─C) exhibit excellent oxygen reduction activity but struggle with bifunctional performance due to their poor evolution activity. Although the Fe spin state is found be closely associated enhanced activity, controllably regulating remains a challenge. Here, controllable regulation of directly achieved through competitive coordination between chlorine and pyridine nitrogen in axial direction Fe─N 4 . The regulated from high intermediate by modulation ligands weak‐field ligand strong‐field pyridinic nitrogen, which leads N─FeN small potential gap (Δ E = 0.68 V). Theoretical calculations indicate that turning accompanied an binding strength sites *OH leading significant decrease OER barrier. Moreover, exhibits sufficient durability for reaction (ORR) (over 50 h), (OER) 200 assembled zinc–air battery 1000 h). Here novel approach proposed designing efficient based on profound insights into Fe─N─C catalysis.

Язык: Английский

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Tailoring the Electron Delocalization in S-LM1-xO-Snx by d Orbital Coupling for Efficient Resistance of Toxic By-Products in Catalytic Combustion of (Cl)-VOCs

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125036 - 125036

Опубликована: Янв. 1, 2025

Язык: Английский

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The Role of Long‐Range Interactions Between High‐Entropy Single‐Atoms in Catalyzing Sulfur Conversion Reactions

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract Sulfur conversion reactions are the foundation of lithium–sulfur batteries but usually possess sluggish kinetics during practical battery operation. Herein, a high‐entropy single‐atom catalyst (HESAC) is synthesized for this process. In contrast to conventional dual‐atom catalysts that form metal–metal bonds, center metal atoms in HESAC not bonded exhibit long‐range interactions at sub‐nanometer distance (<9 Å). The synergistic effect between and entropy changes enables regulation d‐ π‐ electron states. This alteration electronic structure improves adsorption conductivity intermediate polysulfides, thereby accelerating their kinetics. Consequently, leads significant enhancement specific capacities by ≈40% high rates compared catalysts. resulting with demonstrates remarkable areal capacity 3.4 mAh cm −2 10 C. These findings provide valuable insights into design principle atom electrochemical reactions.

Язык: Английский

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Covalent Organic Frameworks with Fe/Co Single-Atom Nanozyme for Alendronate Sodium Detection

ACS Applied Nano Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 11, 2025

Constructing nanozyme-based single atoms with exposed metal-Nx catalytic sites for alendronate sodium (ALDS) tablet quality control is a complex and uncommon task. Herein, we presented an innovative colorimetric assay to detect ALDS utilizing carbon-supported Fe/Co dual-atom nanozymes (Fe/CoSA-NCs) derived from precursor of porphyrin covalent organic frameworks (COFs). The Fe/CoSA-NC nanozymes, featuring Fe–N5 active site electronic interactions between Fe Co, exhibited enhanced peroxidase-like activity. Experimental findings theoretical calculations elucidated that the superior activity Fe/CoSA-NCs stemmed synergistic effect dual atoms, which boosted substrate adsorption reduced reaction barrier. When integrated Fe/CoSA-NCs, could be inhibited due ALDS-Fe3+ coordination. Leveraging this mechanism, rapid selective method was developed detecting ALDS. sensor showed detection limit 0.96 μM in phosphate buffer, surpassing traditional techniques terms efficiency, accuracy, simplicity. Moreover, system successfully utilized pharmaceutical determine urine samples. This work opens powerful avenue developing efficient COFs expands potential applications nanozyme clinical pharmacy.

Язык: Английский

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Engineering Bipolar Doping in a Janus Dual-Atom Catalyst for Photo-Enhanced Rechargeable Zn-Air Battery

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Март 28, 2025

Abstract Harnessing solar energy to enhance the rechargeable zinc–air batteries (RZABs) performance is a promising avenue toward sustainable storage and conversion. Simultaneously enhancing light-absorption capacity carrier separation efficiency in nanomaterials, as well improving electrical conductivity configuration for electrocatalysis, presents formidable challenge due inherent trade-offs interdependencies. Here, we have developed Janus dual-atom catalyst (JDAC) with bifunctional centers efficient charge electrocatalytic through bipolar doping strategy. The situ X-ray absorption near-edge structure Raman spectroscopy analyses demonstrated that Ni Fe JDAC not only function effective sites oxygen evolution reaction reduction reaction, respectively, but also serve hole electron enrichment sites, effectively suppressing photoelectron recombination while photocurrent generation. As result, assembled JDAC-based light-assisted RZABs exhibited extraordinary stability at large current densities. This work delivers pivotal insight design catalysts efficiently convert into electric chemical energy.

Язык: Английский

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Metal-organic-framework-derived dual-atom catalysts: from synthesis to electrocatalytic applications

Materials Science and Engineering R Reports, Год журнала: 2024, Номер 162, С. 100886 - 100886

Опубликована: Ноя. 23, 2024

Язык: Английский

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Biological Neural Network‐Inspired Micro/Nano‐Fibrous Carbon Aerogel for Coupling Fe Atomic Clusters With Fe‐N₄ Single Atoms to Enhance Oxygen Reduction Reaction

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 5, 2025

Nitrogen-coordinated metal single atoms catalysts, especially with M-N4 configuration confined within the carbon matrix, emerge as a frontier of electrocatalytic research for enhancing sluggish kinetics oxygen reduction reaction (ORR). Nevertheless, due to highly planar D4h symmetry in M-N4, their adsorption behavior toward intermediates is limited, undesirably elevating energy barriers associated ORR. Moreover, structural engineering substrate also poses significant challenges. Herein, inspired by biological neural network (BNN), reticular nervous system high-speed signal processing and transmitting, comprehensive biomimetic strategy proposed tailoring Fe-N4 (Fe SAs) coupled Fe atomic clusters ACs) active sites, which are anchored onto chitosan microfibers/nanofibers-based aerogel (CMNCA-FeSA+AC) continuous conductive channels an oriented porous architecture. Theoretical analysis reveals synergistic effect SAs ACs optimizing electronic structures expediting The ingenious will shed light on topology optimization efficient electrocatalysts advanced electrochemical conversion devices.

Язык: Английский

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Synergistic effect of Cu and Fe on chitosan-glutamic acid hydrogel for green synthesis of N doped carbon with CuFe dual atomic clusters for Zn-air batteries

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 161938 - 161938

Опубликована: Март 1, 2025

Язык: Английский

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