p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(31), P. 21357 - 21366

Published: July 25, 2024

With more flexible active sites and intermetal interaction, dual-atom catalysts (DACs) have emerged as a new frontier in various electrocatalytic reactions. Constructing typical p-d orbital hybridization between p-block d-block metal atoms may bring avenues for manipulating the electronic properties thus boosting activities. Herein, we report distinctive heteronuclear dual-metal atom catalyst with asymmetrical FeSn dual embedded on two-dimensional C2N nanosheet (FeSn–C2N), which displays excellent oxygen reduction reaction (ORR) performance half-wave potential of 0.914 V an alkaline electrolyte. Theoretical calculations further unveil powerful stannum ferrum sites, triggers electron delocalization lowers energy barrier *OH protonation, consequently enhancing ORR activity. In addition, FeSn–C2N-based Zn–air battery provides high maximum power density (265.5 mW cm–2) specific capacity (754.6 mA h g–1). Consequently, this work validates immense along perception into logical design DACs.

Language: Английский

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High-density asymmetric iron dual-atom sites for efficient and stable electrochemical water oxidation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 1, 2024

Double-atom catalysts (DACs) have opened distinctive paradigms in the field of rapidly developing atomic catalysis owing to their great potential for promoting catalytic performance various reaction systems. However, increasing loading and extending service life metal active centres represents a considerable challenge efficient utilization DACs. Here, we rationally design asymmetric nitrogen, sulfur-coordinated diatomic iron on highly defective nitrogen-doped carbon nanosheets (denoted A-Fe

Language: Английский

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Precisely designing asymmetrical selenium-based dual-atom sites for efficient oxygen reduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 7, 2025

Owing to their synergistic interactions, dual-atom catalysts (DACs) with well-defined active sites are attracting increasing attention. However, more experimental research and theoretical investigations needed further construct explicit understand the synergy that facilitates multistep catalytic reactions. Herein, we precisely design a series of asymmetric selenium-based comprise heteronuclear SeN2–MN2 (M = Fe, Mn, Co, Ni, Cu, Mo, etc.) for efficient oxygen reduction reaction (ORR). Spectroscopic characterisation calculations revealed selenium atoms can efficiently polarise charge distribution other metal through short-range regulation. In addition, compared Se or Fe single-atom sites, SeFe facilitate in conversion energy barrier from *O *OH via coadsorption intermediates. Among these designed catalysts, selenium-iron achieves superior alkaline ORR performance, half-wave potential 0.926 V vs. reversible hydrogen electrode. SeN2–FeN2-based Zn–air battery has high specific capacity (764.8 mAh g−1) maximum power density (287.2 mW cm−2). This work may provide good perspective designing DACs improve efficiency. Dual-atom precise gaining attention, but studies optimise construction synergy. Here authors report dual- atom reaction.

Language: Английский

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Recent advances in the development of single atom catalysts for oxygen evolution reaction

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 82, P. 1081 - 1100

Published: Aug. 9, 2024

Language: Английский

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Regulation of d‐Orbital Electron in Fe‐N₄ by High‐Entropy Atomic Clusters for Highly Active and Durable Oxygen Reduction Reaction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(46)

Published: June 19, 2024

Abstract Simultaneously improving activity and stability is a crucial yet challenge in the development of metallic single‐atom‐based catalysts. In current work, novel approach introduced to address this issue by combining post‐adsorption secondary pyrolysis techniques create synergistic catalytic system, which single atoms (SAs) Fe sites played NC matrix (Fe─NC) are coupled with high‐entropy atomic clusters (HEACs). Theoretical calculations reveal that incorporation HEACs lead rehybridization 3d orbital configuration Fe‐N 4 , helps balance adsorption/desorption energy oxygenated intermediates. situ spectroscopy further reveals rate‐limiting step OH * desorption on HEAC/Fe─NC oxygen reduction reaction (ORR) more facile compared Fe─NC, implying higher ORR activity. Moreover, effect diffusion activation barriers entropy contributes structural HEAC/Fe─NC, resulting remarkable durability. Consequently, unique catalyst exhibits half‐wave potentials 0.927 0.828 V an aqueous solution KOH (0.1 m ) HClO ), respectively, along excellent The findings propose strategy for modulating electronic structure SAs catalysts enhancing their through strong interactions between HEACs.

Language: Английский

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Tailoring peroxyacetic acid (PAA) activation by sewage sludge derived atomic-Fe clusters/Fe-N4 catalyst via thermally driven spin manipulation

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Language: Английский

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Structural Regulation Strategies of Atomic Cobalt Catalysts for Oxygen Electrocatalysis

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

Published: March 3, 2025

Abstract Oxygen electrocatalysis is a core reaction in renewable energy devices, greatly promoting the transformation and upgrading of structure. Nonetheless, performance conversion devices hindered by large overpotential slow kinetics oxygen electrocatalytic reactions. Recently, single‐atom catalysts (SACs) have emerged as promising contenders field because their exceptional metal atom utilization, distinctive coordination environment, adjustable electronic properties. This review presents latest advancements design Co‐based SACs for electrocatalysis. First, OER ORR mechanisms are introduced. Subsequently, strategies regulating structure summarized three aspects, including centers, support carriers. A particular emphasis given to relationship between properties catalysts. Afterward, applications explored. Ultimately, challenges prospects prospected.

Language: Английский

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Engineering the Active Sites of MOF‐derived Catalysts: From Oxygen Activation to Activate Metal‐Air Batteries^†

Chinese Journal of Chemistry, Journal Year: 2024, Volume and Issue: 42(20), P. 2520 - 2535

Published: June 19, 2024

Comprehensive Summary The electrochemical processes of oxygen reduction reaction (ORR) and evolution (OER) play a crucial role in various energy storage conversion systems. However, the inherently slow kinetics reversible reactions present an urgent demand for development efficient electrocatalysts. Recently, metal‐organic framework (MOF) derivatives have attracted extensive attention electrocatalysis research due to their unique porous structure, abundant active sites, tunable structural properties. Especially, optimization electronic structure sites MOF has been proven as effective strategy enhance catalytic activity. In this review, we provide overview strategies advanced catalysts O—O bond activation reactions, including construction synergistic effects between multiple heterogeneous interfaces, utilization metal support interactions, precise modulation organic ligands surrounding at atomic level. Furthermore, review offers theoretical insights into mechanisms derivatives, well identification sites. Finally, potential challenges prospects are discussed. This contributes understanding advancement Key Scientists

Language: Английский

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Developing new electrocatalysts for oxygen evolution reaction via high throughput experiments and artificial intelligence

npj Computational Materials, Journal Year: 2024, Volume and Issue: 10(1)

Published: Aug. 28, 2024

The development of non-noble metal electrocatalysts for the Oxygen Evolution Reaction (OER) is advancing towards use multi-element materials. To reveal complex correlations OER electrocatalysts, we developed an iterative workflow combining high-throughput experiments and AI-generated content (AIGC) processes. An increased number 909 (compared to 145 in previous literature) universal descriptors inorganic materials science were constructed used as Artificial Neural Network (ANN) input. A large statistical ensembles with each ANN individual ensemble having a reduced integrated new Hierarchical (HNN) algorithm. This algorithm addresses longstanding challenge balancing overwhelming descriptor numbers insufficient datasets traditional approaches problems. As result, combination AIGC experimental validation significantly enhanced prediction accuracy, increase R2 values from 0.7 0.98 Tafel slopes.

Language: Английский

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Double coordination shell modulation of nitrogen-free atomic manganese sites for enhancing oxygen reduction performance

Chemical Science, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Utilizing double coordination shell modulation, we construct a novel nitrogen-free single-atom manganese configuration catalyst on graphene oxide (Mn–S 1 O 4 G), which exhibits excellent ORR and zinc–air battery performances.

Language: Английский

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