Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: April 9, 2024

The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the reduction reaction (ORR) kinetics. Herein, a new approach for boosting inherent ORR activity atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. as-prepared catalyst delivers excellent half-wave potentials 0.78 0.90 V in acidic alkaline solutions, respectively. decent can also be validated from high-performance rechargeable Zn-air battery. experiments density functional theory calculations reveal that electron spin-state monodispersed active transferred low spin (LS, t

Language: Английский

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Optimizing electronic synergy of atomically dispersed dual-metal Ni–N₄ and Fe–N₄ sites with adjacent Fe nanoclusters for high-efficiency oxygen electrocatalysis

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(2), P. 704 - 716

Published: Dec. 7, 2023

The electronic synergy of Fe nanoclusters and Ni/Fe–N 4 single-atomic sites optimizes the adsorption/desorption oxygenated intermediates reduces energy barrier oxygen electrocatalysis, boosting Zn–air batteries performance.

Language: Английский

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Development of Synergistically Efficient Ni–Co Pair Catalytic Sites for Enhanced Polysulfide Conversion in Lithium–Sulfur Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(37)

Published: March 29, 2024

Abstract The performance of Lithium–sulfur (Li–S) batteries is constrained by the migration lithium polysulfide (LiPS), slow conversion LiPS, and significant reaction barrier encountered during precipitation/dissolution Li 2 S throughout discharge/charge cycle. In this contribution, study presents Ni–Co dual‐atom catalytic sites on hollow nitrogen‐doped carbon (NiCoNC). Theoretical calculations experimental data reveal that catalysts (DACs) accelerate kinetic LiPSs facilitate formation/decomposition discharging charging, which minimizes LiPS migration. Consequently, utilization S/NiCoNC cathodes manifests a substantial initial capacity 1348.5 mAh g −1 at 0.1 C, exceptional cycling stability with an average degradation rate 0.028% per cycle over 900 cycles 0.5 noteworthy capability 626 C. Electrodes higher sulfur loading 4.5 mg cm −2 low electrolyte/sulfur ratio 8 µL exhibit specific capacities up to 1236 as well retention 494.2 after 200 0.2 This effectively showcases potential DACs for cathodes, thereby enhancing overall Li–S batteries.

Language: Английский

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Optimizing the binding of the *OOH intermediate via axially coordinated Co-N5 motif for efficient electrocatalytic H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 338, P. 123078 - 123078

Published: July 7, 2023

Language: Английский

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Surface Engineered Single‐atom Systems for Energy Conversion

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 10, 2024

Abstract Single‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs still early stages of conversion, problems like agglomeration low conversion efficiency hampering their practical applications. Substantial research focus on support modifications, which vital SAC stability due intimate relationship between atoms support. In this review, category supports variety surface engineering strategies employed SA systems summarized, including site (heteroatom doping, vacancy introducing, groups grafting, coordination tunning) structure (size/morphology control, cocatalyst deposition, facet engineering, crystallinity control). Also, merits single‐atom systematically introduced. Highlights comprehensive summary discussions utilization surface‐engineered diversified applications photocatalysis, electrocatalysis, thermocatalysis, devices. At end potential obstacles using field discussed. This review aims guide rational design manipulation target‐specific capitalizing characteristic benefits engineering.

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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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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Cobalt phthalocyanine promoted copper catalysts toward enhanced electro reduction of CO2 to C2: Synergistic catalysis or tandem catalysis?

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 92, P. 499 - 507

Published: Jan. 18, 2024

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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Cascade Synthesis of Fe‐N2‐Fe Dual‐Atom Catalysts for Superior Oxygen Catalysis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 3, 2024

Dual-atom catalysts (DACs) have been proposed to break the limitation of single-atom (SACs) in synergistic activation multiple molecules and intermediates, offering an additional degree freedom for catalytic regulation. However, it remains a challenge synthesize DACs with high uniformity, atomic accuracy, satisfactory loadings. Herein, we report facile cascade synthetic strategy DAC via precise electrostatic interaction control neighboring vacancy construction. We synthesized well-defined, uniformly dispersed dual Fe sites which were connected by two nitrogen bonds (denoted as Fe-N

Language: Английский

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