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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Sulfur Vacancies in Pyrite Trigger the Path to Nonradical Singlet Oxygen and Spontaneous Sulfamethoxazole Degradation: Unveiling the Hidden Potential in Sediments

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(15), P. 6753 - 6762

Published: March 25, 2024

Pharmaceutical residues in sediments are concerning as ubiquitous emerging contaminants. Pyrite is the most abundant sulfide minerals estuarine and coastal sediments, making it a major sink for pharmaceutical pollutants such sulfamethoxazole (SMX). However, research on adsorption redox behaviors of SMX pyrite surface limited. Here, we investigated impact nonphotochemical process fate coexisting SMX. Remarkably, sulfur vacancies (SVs) promoted generation nonradical species (hydrogen peroxide, H2O2 singlet oxygen, 1O2), thereby exhibiting prominent degradation performance under darkness. Nonradical 1O2 contributed approximately 73.1% total degradation. The SVs with high surrounding electron density showed an advanced affinity adsorbing O2 then initiated reactions sediment electron-storing geobattery pyrite, resulting extensive through two-electron oxygen reduction pathway. Surface Fe(III) (hydro)oxides facilitated decomposition to generation. Distinct products were observed all samples concentrations ranging from 1.96 2.94 μM, while ranged 4.63 × 10–15 8.93 M. This dark-redox pathway outperformed traditional photochemical routes pollutant degradation, broadening possibilities use sediments. Our study highlighted SV-triggered yet previously overlooked source species, which offered fresh insights into geochemical processes dynamics regions frequent oscillations sulfur-rich

Language: Английский

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Enhanced photocatalytic degradation of sulfamethoxazole using MIL-101(Fe) supported Mo single-atom with oxygen vacancies under visible light activation of peroxymonosulfate

Process Safety and Environmental Protection, Journal Year: 2025, Volume and Issue: 195, P. 106778 - 106778

Published: Jan. 10, 2025

Language: Английский

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Singlet oxygen in environmental catalysis: Mechanisms, applications and future directions

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 529, P. 216439 - 216439

Published: Jan. 16, 2025

Language: Английский

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Regulating PMS affinity by intimate interface to generate coupled radicals and non-radicals in efficiently antibiotics degradation

Separation and Purification Technology, Journal Year: 2025, Volume and Issue: unknown, P. 131419 - 131419

Published: Jan. 1, 2025

Language: Английский

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Iron Single-Atom Catalyst Actuates PMS/O₃ Activation Process: Nonradical Generation Path for Synergistic Multiperoxides

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

Published: Jan. 13, 2025

Singlet oxygen (1O2) is an excellent reactive species in advanced oxidation processes for water purification due to its environmental suitability and selectivity. However, generation conversion mechanisms remain unclear. Herein, we have constructed a high-yield system 1O2 by introducing ozone (O3) into iron single-atom catalyst/peroxymonosulfate (PMS) system. The steady-state concentration of the was increased 53.2% at O3 below 0.5 mg/L. formation from high-valent iron-oxo (FeIV═O) revealed electron paramagnetic resonance analysis, where FeIV═O found probe experiment via activation PMS on sites. developed situ singlet fluorescence imaging technique observed that addition has promoted process 1O2. Density functional theory calculations further demonstrated low energy barrier key intermediate OO* this process. These findings help understand mechanism production molecular level guide design efficient reaction systems purification.

Language: Английский

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Single‐Atom Catalysts Originated from Metal–Organic Frameworks for Sulfate Radical‐Based Advanced Oxidation Processes: Critical Insights into Mechanisms

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(6)

Published: Oct. 22, 2023

Abstract The widely discussed single‐atom catalysts (SACs) are regarded as a kind of attractive material for sulfate radical‐based advanced oxidation processes (SR‐AOPs) owing to their maximum atomic utilization efficiency and outstanding stability. Currently, metal–organic frameworks (MOFs) have appeared prospective precursors building SACs due extensive chelating sites, functional adjustability, structural tunability. However, there few critical systematic reviews about the application MOF‐derived in SR‐AOPs, especially in‐depth analysis mechanisms. Therefore, this review seeks offer thorough summary development SR‐AOPs. First, unique advantages MOFs derivative thoroughly. Afterward, current synthesis strategies elaborated categorically unveil formation process single atoms coordination environments. Notably, roles different reaction sites including generation reactive species mediating electron transfer further analyzed explain mechanisms comprehensively. Thereafter, characterization techniques theoretical calculations studies also highlighted. Eventually, insights into present challenges future developments proposed, which expected enhance catalytic

Language: Английский

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Efficient 1O2 production from H2O2 over lattice distortion controlled spinel ferrites

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 343, P. 123468 - 123468

Published: Nov. 5, 2023

Language: Английский

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Prussian Blue Analogues and Their Derivatives: From Elaborate Microstructure Design to Boosted Fenton-Like Application

Accounts of Materials Research, Journal Year: 2024, Volume and Issue: 5(5), P. 585 - 599

Published: April 9, 2024

ConspectusHeterogeneous Fenton-like reaction is a promising process for refractory wastewater treatment. Among the various heterogeneous catalysts, Prussian blue (PB) and analogues (PBAs) show great potential hydrogen peroxide persulfate activation owing to their low toxicity, simple preparation, high activity. To further improve catalytic activity of PBAs derivatives (PBDs), many efforts have been made overcome instability crystal structure develop feasible methodologies prepare PBAs/PBDs with diverse morphologies compositions. In this Account, our recent achievements on novel synthetic strategies obtain controlled morphologies, geometric sites, electronic structures were systematically summarized. The physicochemical properties contribution in advanced oxidation processes (AOPs) also discussed.First, we focus developing synthesis technology (such as "copolymer-co-morphology" conception) controllable morphology. By regulating chelating agents, surfactants, metal ions, preparation conditions constructing heterojunction, stability was significantly improved during redox reaction. Notably, inherit characteristics PBAs, topological transformation strategy applied fabricate oxides similar those through thermal calcination under an aerobic atmosphere. Subsequently, has extensively single-atom nitrides, zerovalent metals via treatment inert/reducing atmospheres. These provide guidance devising materials superior cycling tests not only reactions but other systems. addition property optimization, relationship between deliberately designed first explored depth using 57Fe Mössbauer spectroscopy. Moreover, benefiting from these efficient techniques conscientious explorations, research elucidated important descriptors intrinsic pathways revealed significant effect external energy (ultraviolet visible light) PBAs/PBDs-dominant findings inspiration application additional energy. Finally, challenges development prospects AOPs are comprehensively discussed. Overall, Account provides comprehensive insights into fabrication strategies, properties, local structures, correlation mechanisms analysis paves way future catalysis fields.

Language: Английский

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Mn doped nitrogen containing carbon activating peroxymonosulfate for enhancing sulfadiazine degradation via single oxygen pathway: Performance and mechanism

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 352, P. 128196 - 128196

Published: May 29, 2024

Language: Английский

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