Boosting High‐Valent Fe═O Formation via Fe Electron Localization in Asymmetric FeMo Dual‐Atom Catalyst for Fenton‐Like Reaction

Small, Год журнала: 2025, Номер unknown

Опубликована: Май 27, 2025

Abstract High‐valent Fe═O species, recognized as pivotal reactive oxygen intermediates in the catalyst‐activated peroxymonosulfate (PMS) oxidation system, play a dominant role contaminant degradation. However, inherent correlation between Fe 3d electronic structure of heterogeneous catalysts and generation efficiency high‐valent remains unclear, limiting rational design high‐performance catalysts. To end, Fe–Mo dual‐atom (FeMoNC) with N 3 Fe‐O‐MoN 2 configurations are constructed, which exhibit exceptional sulfadiazine (SDZ) degradation activity (k = 0.92 min −1 ). This performance surpasses that monometallic FeNC (1.67 times), attributed to optimized species. Combined XPS/XAS analysis DFT calculations reveal electron transfer from Mo upshifts d‐band center by 0.144 eV, facilitates O γ ‐O β bond cleavage PMS (energy barrier reduced 31%) stabilizes The modifications further confirm promoted formation. work elucidates origin heteronuclear catalysts, providing universal strategy for manipulating 3d‐electron enhance metal‐oxo chemistry advanced processes.

Язык: Английский

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Unveiling the Mystery of Precision Catalysis: Dual‐Atom Catalysts Stealing the Spotlight

Small, Год журнала: 2024, Номер unknown

Опубликована: Дек. 26, 2024

In the era of atomic manufacturing, precise manipulation structures to engineer highly active catalytic sites has become a central focus in catalysis research. Dual-atom catalysts (DACs) have garnered significant attention for their superior activity, selectivity, and stability compared single-atom (SACs). However, comprehensive review that integrates geometric electronic factors influencing DAC performance remains limited. This systematically explores structure DAC, addressing key macroscopic parameters, such as spatial arrangements interatomic distances, well microscopic factors, including local coordination environments structures. Additionally, metal-support interactions (MSI) long-range (LSI) are comprehensively analyzed, which play pivotal yet underexplored role governing behavior. integration tailored functional groups is further discussed fine-tune properties, thereby optimizing intermediate adsorption, enhancing reaction kinetics, expanding multifunctionality various electrochemical environments. offers novel insights into rational design by elucidating intricate mechanisms underlying DACs' exceptional performance. Ultimately, DACs positioned critical players precision catalysis, highlighting potential drive breakthroughs across broad spectrum applications.

Язык: Английский

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Regulating the Cu2Se-SnO nanosheet heterostructure interface for efficient CO2 conversion to tunable syngas ratios

Journal of Alloys and Compounds, Год журнала: 2024, Номер 985, С. 174108 - 174108

Опубликована: Март 7, 2024

Язык: Английский

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Atomically Integration of O-Bridged Co-Fe Hetero-Pairs as Tandem Photocatalyst Towards Highly Efficient Hydroxyl Radicals Production

Опубликована: Янв. 1, 2024

Photocatalytic Fenton-coupled oxygen reduction reaction (ORR) is a promising strategy for •OH production. Single-atom catalysts (SACs), featuring high atom utilization, exhibit superior catalytic activity. However, it remains challenge to synchronously achieve efficient catalysis of both steps on one active site. Herein, novel Co-Fe hetero-atom pair tandem photocatalyst was precisely constructed by pre-designing the structure covalent organic frameworks (COFs) and introduction strategies sites. Thanks synergism neighboring atoms, Co-Fe-COF presents highly hydroxyl radicals production following process O2+H2O→H2O2→•OH. Additionally, immobilization pairs pore walls COF can boost enrichment contaminants, thus increasing utilization •OH. Theoretical simulations reveal proximity electronic effect O-bridged not only thermodynamically promotes formation OOH*, but also dynamically activates self-healing cycle Fe(II)/Fe(III). This work provides routine designing high-performance catalysts.

Язык: Английский

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P-tuned FeN2 binuclear sites for boosted CO2 electro-reduction

Journal of Energy Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Окт. 1, 2024

Язык: Английский

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