Water Research, Journal Year: 2024, Volume and Issue: 268, P. 122545 - 122545
Published: Sept. 30, 2024
Language: Английский
Water Research, Journal Year: 2024, Volume and Issue: 268, P. 122545 - 122545
Published: Sept. 30, 2024
Language: Английский
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
Citations
115Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 344, P. 123643 - 123643
Published: Dec. 21, 2023
Language: Английский
Citations
58Environmental 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
Citations
46Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: Sept. 5, 2024
Language: Английский
Citations
42Small, 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
Citations
28Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 355, P. 124157 - 124157
Published: May 9, 2024
Language: Английский
Citations
24Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124385 - 124385
Published: July 9, 2024
Language: Английский
Citations
24Angewandte 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
Citations
23Proceedings 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
Citations
23Cell 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
Citations
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