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, Journal Year: 2024, Volume and Issue: 36(44)

Published: Sept. 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

Language: Английский

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In Situ Amorphization of Electrocatalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 26, 2024

Abstract Electrocatalysis represents an efficient and eco‐friendly approach to energy conversion, enabling the sustainable synthesis of valuable chemicals fuels. The deliberate engineering electrocatalysts is crucial improving efficacy scalability electrocatalysis. Notably, occurrence in situ amorphization within has been observed during various electrochemical processes, influencing conversion efficiency catalytic mechanism understanding. Of note, dynamic transformation catalysts into amorphous structures complex, often leading configurations. Therefore, revealing this process understanding function species are pivotal for elucidating structure‐activity relationship electrocatalysts, which will direct creation highly catalysts. This review examines mechanisms behind structure formation, summarizes characterization methods detecting species, discusses strategies controlling (pre)catalyst properties conditions that influence amorphization. It also emphasizes importance spontaneously formed oxidation reduction reactions. Finally, it addresses challenges electrocatalysts. aiming guide efficient, selective, stable reactions, inspire future advancements field.

Language: Английский

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Multiphase lattice engineering of bimetallic phosphide-embedded tungsten-based phosphide/oxide nanorods on carbon cloth: A synergistic and stable electrocatalyst for overall water splitting

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: unknown, P. 155832 - 155832

Published: Sept. 1, 2024

Language: Английский

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Accelerated proton-coupled electron transfer kinetics of iron phthalocyanine for oxygen reduction via heteropoly blue clusters

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125080 - 125080

Published: Jan. 1, 2025

Language: Английский

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The polarization loss induced by interfacial charge redistribution using Ar plasma treatment in Ni@C composites for superior microwave absorption performance

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160489 - 160489

Published: Feb. 1, 2025

Language: Английский

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Unveiling a Cooperative Mechanism for the Alkaline Hydrogen Evolution Reaction: Role of Built‐in Electric Field

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

Abstract The work function has a significant influence on surface charge distribution, particularly when built‐in electric field (BIEF) is present. Recent research focused leveraging BIEFs at the interface of different electronic environments to improve hydrogen production. Therefore, analyzing and correlating parameters such as function, BIEF, Gibbs free energy crucial for understanding reaction mechanism. Herein, p‐n heterojunction CuO‐CuWO 4 created form moderate space‐charge region interface. (∆G) in depletion regime displays behavior that contrasts with bulk region, facilitating evolution (HER). Along interface, ∆G indicates high adsorption affinity protons toward CuO phase desorption CuWO phase. catalyst effectively fine‐tunes its value relative coverage exhibits negative cooperative effect. shows up 80% coverage, maintains proton (−1.05 eV), which gradually decreases −0.05 eV 100% coverage. surpassed commercial Pt/C, demonstrating higher efficiency achieving current density 10 mA cm − 2 an overpotential just 21 mV.

Language: Английский

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Metal-free nitrogen-doped carbon-based electrocatalysts for oxygen reduction reaction in microbial fuel cells: Advances, challenges, and future directions

Nano Energy, Journal Year: 2024, Volume and Issue: 134, P. 110537 - 110537

Published: Dec. 3, 2024

Language: Английский

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Electronic Structure Modulation Induced by the Synergy of Cobalt Low-Nuclearity Clusters and Mononuclear Sites for Efficient Oxygen Electrocatalysis

ACS Nano, Journal Year: 2024, Volume and Issue: 19(1), P. 1600 - 1610

Published: Dec. 27, 2024

The development of high-performance bifunctional single-atom catalysts for use in applications, such as zinc–air batteries, is greatly impeded by mild oxygen reduction and evolution reactions (ORR OER). Herein, we report a electrocatalyst designed to overcome these limitations. catalyst consists well-dispersed low-nuclearity Co clusters adjacent single atoms over nitrogen-doped carbon matrix (CoSA+C/NC). precisely tailored asymmetric electronic structures are achieved with strong interactions between species. optimize the adsorption/desorption strength oxygenated intermediates on single-atomic sites endow exceptional activity under alkaline conditions half-wave potential (E1/2) 0.91 V an overpotential (η) 340 mV at 10 mA cm–2. In addition, battery assembled CoSA+C/NC achieves high power density 284.1 mW cm–2 long operational lifespan 400 h, superior those benchmark Pt/C + RuO2. Experimental findings theoretical analysis reveal that enhanced stems from synergistic sites. Consequently, overbinding *OH suppressed accelerated removal. This work establishes design principle advanced electrocatalysts multiphase metal species bearing interactions.

Language: Английский

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Construction of S/Cl-NiCo LDH@NiCo2O4 Heterojunction for Enhanced Charge Storage and Decoupled Water Electrolysis

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: unknown, P. 178419 - 178419

Published: Dec. 1, 2024

Language: Английский

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Approaching Charge Compensation Limit for Promoting Magnetoresistance in 2D Nonlayered MoO₂ via Surface Hydrogen Passivation

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 20, 2025

Abstract Large non‐saturated magnetoresistances of semimetals are dominated by charge compensation due to their unique electronic structure. However, the dramatic magnetoresistance deteriorations often observed in low‐dimensional system resulting from high‐density surface defects, where suppression scattering or concentration unbalance with highly maintained is still challenging. Herein, a hydrogen annealing strategy developed for defects passivation 2D MoO 2 nanoflakes. Systematical characterization H‐MoO nanoflakes reveals formation chemical bonds that reduce defect density and slightly change Fermi level unchanged bulk structures. An obviously enhanced 9.2% demonstrated compared Ar‐MoO 3.9% at 10 K 9 T. The analysis nonlinearity Hall resistivity unravels electrons holes approaches more balanced equilibrium, which attributed self‐doping effects rather than reduced carrier mobility. research not only provides universal on nonlayered approaching limit preserved but also underscores significance tuning structures materials.

Language: Английский

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