Coupled Surface-Confinement Effect and Pore Engineering in a Single-Fe-Atom Catalyst for Ultrafast Fenton-like Reaction with High-Valent Iron-Oxo Complex Oxidation

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(41), P. 15667 - 15679

Published: Oct. 6, 2023

The nanoconfinement effect in Fenton-like reactions shows great potential environmental remediation, but the construction of confinement structure and corresponding mechanism are rarely elucidated systematically. Herein, we proposed a novel peroxymonosulfate (PMS) activation system employing single Fe atom supported on mesoporous N-doped carbon (FeSA-MNC, specific surface area = 1520.9 m2/g), which could accelerate catalytic oxidation process via surface-confinement effect. degradation activity confined was remarkably increased by 34.6 times compared to its analogue unconfined system. generation almost 100% high-valent iron-oxo species identified 18O isotope-labeled experiments, quenching tests, probe methods. density functional theory illustrated that narrows gap between d-band center Fermi level atom, strengthens charge transfer rate at reaction interface reduces free energy barrier for PMS activation. exhibited excellent pollutant efficiency, robust resistance coexisting matter, adaptation wide pH range (3.0-11.0) various temperature environments (5-40 °C). Finally, FeSA-MNC/PMS achieve sulfamethoxazole removal without significant performance decline after 10,000-bed volumes. This work provides insights into chemistry guides design superior systems remediation.

Language: Английский

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Rational modulation of Fe single-atom electronic structure in a Fe-N2B4 configuration for preferential 1O2 generation in Fenton-like reactions

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 344, P. 123643 - 123643

Published: Dec. 21, 2023

Language: Английский

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Active Center Size-Dependent Fenton-Like Chemistry for Sustainable Water Decontamination

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(50), P. 21416 - 21427

Published: Dec. 8, 2023

Accurately controlling catalytic activity and mechanism as well identifying structure–activity–selectivity correlations in Fenton-like chemistry is essential for designing high-performance catalysts sustainable water decontamination. Herein, active center size-dependent with single cobalt atoms (CoSA), atomic clusters (CoAC), nanoparticles (CoNP) were fabricated to realize the changeover of peroxymonosulfate (PMS)-based chemistry. Catalytic durability vary change metal sizes. Besides, reducing size from significantly modulates contributions radical nonradical mechanisms, thus achieving selective/nonselective degradation. Density functional theory calculations reveal evolutions mechanisms systems over different Gibbs free energies reactive oxygen species generation. Single-atom site contact PMS preferred induce while dissociates generates radicals on nanoparticles. Differences originating reaction endow developed selectivity mineralization treating actual hospital wastewater column reactors. This work brings an in-depth understanding effects guides design intelligent fulfill demand specific scenes purification.

Language: Английский

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Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination

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

Published: Sept. 5, 2024

Language: Английский

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Advancements in Electrocatalytic Nitrogen Reduction: A Comprehensive Review of Single‐Atom Catalysts for Sustainable Ammonia Synthesis

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 22, 2024

Abstract Electrocatalytic nitrogen reduction technology seamlessly aligns with the principles of environmentally friendly chemical production. In this paper, a comprehensive review recent advancements in electrocatalytic NH 3 synthesis utilizing single‐atom catalysts (SACs) is offered. Into research and applications three categories SACs: noble metals (Ru, Au, Rh, Ag), transition (Fe, Mo, Cr, Co, Sn, Y, Nb), nonmetallic (B) context ammonia delved. In‐depth insights into material preparation methods, coordination patterns, characteristics reaction (NRR) are provided. The systematic comparison capabilities various SAC types offers framework for their integration NRR. Additionally, challenges, potential solutions, future prospects incorporating SACs endeavors discussed.

Language: Английский

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The structure-performance relationships in active center size-dependent Fenton-like catalysis: From nanoparticles to single atoms

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 355, P. 124157 - 124157

Published: May 9, 2024

Language: Английский

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Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124385 - 124385

Published: July 9, 2024

Language: Английский

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Atomically Dispersed p‐Block Aluminum‐Based Catalysts for Oxygen Reduction Reaction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(20)

Published: March 13, 2024

The main group metals are commonly perceived as catalytically inert in the context of oxygen reduction reactions (ORR) due to delocalized valence orbitals. Regulating local environment and structure metal center coordinated by nitrogen ligands (M-N

Language: Английский

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The “4 + 1” strategy fabrication of iron single-atom catalysts with selective high-valent iron-oxo species generation

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(23)

Published: May 30, 2024

Single-atom catalysts (SACs) with atomic dispersion active sites have exhibited huge potentials in peroxymonosulfate (PMS)-based Fenton-like chemistry water purification. However, four-N coordination metal (MN 4 ) moieties often suffer from such problems as low selectivity and narrow workable pH. How to construct SACs a controllable strategy optimized electronic structures is of great challenge. Herein, an innovative (i.e., the “4 + 1” fabrication) was devised precisely modulate first-shell coordinated microenvironment FeN SAC using additional N (SA-FeN 5 ). This leads almost 100% selective formation high-valent iron-oxo [Fe(IV)═O] (steady-state concentration: 2.00 × 10 −8 M) SA-FeN /PMS system. In-depth theoretical calculations unveil that configuration optimizes electron distribution monatomic Fe sites, which thus fosters PMS adsorption reduces energy barrier for Fe(IV)═O generation. then attached polyvinylidene difluoride membrane continuous flow device, showing long-term abatement microcontaminant. work furnishes general effective activation metal-oxo species generation by high N-coordination number regulation SACs, would provide guidance rational design superior environmental

Language: Английский

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Gambling of homogeneous and heterogeneous Fenton in wastewater treatment

Cell Reports Physical Science, Journal Year: 2024, Volume and Issue: 5(5), P. 101966 - 101966

Published: May 1, 2024

Employing Fenton technology for efficiently removing pollutants in water stands as a significant method. Within the domain of traditional techniques, there exist both homogeneous and heterogeneous systems. Homogeneous systems tackle iron sludge concerns through incorporation co-catalysts, whereas adeptly manipulate surface microenvironments adjust active sites, enabling pollutant degradation across wide range pH. Each system boasts distinct advantages limitations. This perspective critically examines existing challenges associated solutions reactions comprehensive analysis typical case studies. The focus is on evaluating industrial potential these systems, forecasting future developmental trends, fostering more robust sustainable advancement within context carbon peaking neutrality goals.

Language: Английский

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