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

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 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.

Language: Английский

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Hollow Porous Carbon Nanocubes with High-Loading Accessible Iron Atomic Sites for CO₂ Electroreduction

ACS Applied Nano Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 4, 2025

Single-atom catalysts (SACs) have exhibited enormous potential toward electrocatalytic CO2 reduction (CO2RR). The accessibility of active sites has a significant influence on their catalytic performance, especially in the mass-transport-limited reaction like CO2RR. Therefore, rational design SACs with easily accessible and high-loading atomic is crucial but still remains grand challenge. In this work, thermally removable template strategy combined emulsion-induced interface anisotropic assembly method was developed to prepare iron single-atom catalyst easy high loading amount. For CO2RR, as-synthesized Fe-SACs supported hollow porous carbon nanocube (H–Fe–NC SACs) display selectivity CO. Most importantly, CO partial current density H–Fe–NC at −0.98 V can reach −23.5 mA cm–2, which 2.3 times higher than that solid sphere. matrix efficiently enhances promotes mass transport, thus accelerating kinetics catalysis reaction. It expected carrier engineering provide versatile route improve performance

Language: Английский

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Mo–Mo bond promoted super-high electro-catalytic efficiency of nitrate reduction to ammonia

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 124, P. 242 - 250

Published: April 8, 2025

Language: Английский

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One-pot synthesis of chitin-derived Co–NPs/NC catalysts: Efficient reductive N-formylation of nitro compounds to formamides

Molecular Catalysis, Journal Year: 2024, Volume and Issue: 572, P. 114792 - 114792

Published: Dec. 26, 2024

Language: Английский

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