Engineering the Lewis Acidity of Fe Single-Atom Sites via Atomic-Level Tuning of Spatial Coordination Configuration for Enhanced Oxygen Reduction DOI

Qingyun Qu,

Yu Mao,

Shufang Ji

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 16, 2025

Nitrogen-doped carbon-supported Fe catalysts (Fe-N-C) with Fe-N4 active sites hold great promise for the oxygen reduction reaction (ORR). However, fine-tuning structure of to enhance their performance remains a grand challenge. Herein, we report an innovative design strategy promote ORR activity and kinetics by engineering Lewis acidity, which is achieved tuning spatial coordination geometry. Theoretical calculations indicated that Fe1-N4SO2 (with axial –SO2 group bonded Fe) offered favorable acidity ORR, leading optimized adsorption energies key intermediates. To implement this strategy, developed molecular-cage-encapsulated synthesize single-atom site catalyst (SAC) sites. In agreement theory, Fe1-N4SO2/NC demonstrated outstanding in both alkaline (E1/2 = 0.910 V 0.1 M KOH) acidic media 0.772 HClO4), surpassing commercial Pt/C traditional SACs Fe1-N4 or planar S-coordinated Fe1-N4-S Moreover, newly showed application potential quasi-solid-state Zn–air batteries, delivering superior across wide temperature range.

Язык: Английский

Engineering the Lewis Acidity of Fe Single-Atom Sites via Atomic-Level Tuning of Spatial Coordination Configuration for Enhanced Oxygen Reduction DOI

Qingyun Qu,

Yu Mao,

Shufang Ji

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 16, 2025

Nitrogen-doped carbon-supported Fe catalysts (Fe-N-C) with Fe-N4 active sites hold great promise for the oxygen reduction reaction (ORR). However, fine-tuning structure of to enhance their performance remains a grand challenge. Herein, we report an innovative design strategy promote ORR activity and kinetics by engineering Lewis acidity, which is achieved tuning spatial coordination geometry. Theoretical calculations indicated that Fe1-N4SO2 (with axial –SO2 group bonded Fe) offered favorable acidity ORR, leading optimized adsorption energies key intermediates. To implement this strategy, developed molecular-cage-encapsulated synthesize single-atom site catalyst (SAC) sites. In agreement theory, Fe1-N4SO2/NC demonstrated outstanding in both alkaline (E1/2 = 0.910 V 0.1 M KOH) acidic media 0.772 HClO4), surpassing commercial Pt/C traditional SACs Fe1-N4 or planar S-coordinated Fe1-N4-S Moreover, newly showed application potential quasi-solid-state Zn–air batteries, delivering superior across wide temperature range.

Язык: Английский

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