Degradation of organic pollutants from water by biochar-assisted advanced oxidation processes: Mechanisms and applications

Journal of Hazardous Materials, Год журнала: 2022, Номер 442, С. 130075 - 130075

Опубликована: Сен. 29, 2022

Язык: Английский

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Recent advances in the applications of encapsulated transition-metal nanoparticles in advanced oxidation processes for degradation of organic pollutants: A critical review

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 342, С. 123401 - 123401

Опубликована: Окт. 18, 2023

Язык: Английский

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CoN₁O₂ Single‐Atom Catalyst for Efficient Peroxymonosulfate Activation and Selective Cobalt(IV)=O Generation

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(27)

Опубликована: Апрель 26, 2023

High-valent metal-oxo (HVMO) species are powerful non-radical reactive that enhance advanced oxidation processes (AOPs) due to their long half-lives and high selectivity towards recalcitrant water pollutants with electron-donating groups. However, high-valent cobalt-oxo (CoIV =O) generation is challenging in peroxymonosulfate (PMS)-based AOPs because the 3d-orbital occupancy of cobalt would disfavor its binding a terminal oxygen ligand. Herein, we propose strategy construct isolated Co sites unique N1 O2 coordination on Mn3 O4 surface. The asymmetric configuration able accept electrons from 3d-orbital, resulting significant electronic delocalization at for promoted PMS adsorption, dissociation subsequent CoIV =O species. CoN1 /Mn3 exhibits intrinsic activity activation sulfamethoxazole (SMX) degradation, highly outperforming counterpart CoO3 configuration, carbon-based single-atom catalysts CoN4 commercial oxides. effectively oxidize target contaminants via atom transfer produce low-toxicity intermediates. These findings could advance mechanistic understanding molecular level guide rational design efficient environmental catalysts.

Язык: Английский

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Antibiotics in global rivers

National Science Open, Год журнала: 2022, Номер 1(2), С. 20220029 - 20220029

Опубликована: Авг. 10, 2022

Antibiotics have received extensive attention due to their sophisticated effects on human health and ecosystems. However, there is an extreme scarcity of information composition, content, geographic distribution, risk riverine antibiotics at a large spatial scale. Based systematic review over 600 pieces literature (1999–2021), we established global dataset containing more than 90,000 records covering 169 metabolites in surface water sediment across 76 countries. The occurrence prioritized largely depended socioeconomic developmental levels, the current “hotspots” polluted rivers were found mostly less developed countries or emerging economies (e.g., some Africa, South America, Asia). By developing screening protocol for risk-based prioritization antibiotics, advanced rank list guiding formulation region-specific strategies, which highlighted importance whole life cycle management maintenance world’s rivers.

Язык: Английский

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Thiadiazole-Based Covalent Organic Frameworks with a Donor–Acceptor Structure: Modulating Intermolecular Charge Transfer for Efficient Photocatalytic Degradation of Typical Emerging Contaminants

Environmental Science & Technology, Год журнала: 2022, Номер 56(22), С. 16303 - 16314

Опубликована: Окт. 28, 2022

As novel metal-free photocatalysts, covalent organic frameworks (COFs) have great potential to decontaminate pollutants in water. Fast charge recombination COFs yet inhibits their photocatalytic performance. We found that the intramolecular transfer within could be modulated via constructing a donor-acceptor (D-A) structure, leading improved performance of toward pollutant degradation. By integrating electron donor units (1,3,4-thiadiazole or 1,2,4-thiadiazole ring) and acceptor (quinone), two (COF-TD1 COF-TD2) with robust D-A characteristics were fabricated as visible-light-driven photocatalysts paracetamol. With readily excited electrons 1,3,4-thiadiazole rings, COF-TD1 exhibited efficient electron-hole separation through push-pull electronic effect, resulting superior paracetamol photodegradation (>98% degradation 60 min) than COF-TD2 (∼60% 120 min). efficiently photodegrade complicated water matrices even river water, lake sewage wastewater. Diclofenac, bisphenol A, naproxen, tetracycline hydrochloride also effectively degraded by COF-TD1. Efficient scaled-up reactor achieved either powder form immobilized onto glass slide (to further ease recovery reuse) under natural sunlight irradiation. Overall, this study provided an effective strategy for designing excellent COF-based degrade emerging contaminants.

Язык: Английский

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Nanoconfinement-triggered oligomerization pathway for efficient removal of phenolic pollutants via a Fenton-like reaction

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Янв. 31, 2024

Abstract Heterogeneous Fenton reaction represents one of the most reliable technologies to ensure water safety, but is currently challenged by sluggish Fe(III) reduction, excessive input chemicals for organic mineralization, and undesirable carbon emission. Current endeavors improve catalytic performance are mostly focused on how accelerate while pollutant degradation step habitually overlooked. Here, we report a nanoconfinement strategy using graphene aerogel (GA) support UiO-66-NH 2 -(Zr) binding atomic Fe(III), which alters transfer route during phenol removal from kinetically favored ring-opening thermodynamically oligomerization route. GA favors reduction enriching reductive intermediates allows much faster than unconfined analog (by 208 times in terms first-order rate constant) highly efficient total carbon, i.e., 92.2 ± 3.7% versus 3.6 0.3% 60 min. Moreover, this reduces oxidant consumption more 95% emission 77.9%, compared mineralization homogeneous Fe 2+ +H O system. Our findings may upgrade regulatory toolkit reactions provide an alternative aqueous pollutants.

Язык: Английский

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Ferrate(VI)/Periodate System: Synergistic and Rapid Oxidation of Micropollutants via Periodate/Iodate-Modulated Fe(IV)/Fe(V) Intermediates

Environmental Science & Technology, Год журнала: 2023, Номер 57(17), С. 7051 - 7062

Опубликована: Апрель 19, 2023

The presence of organic micropollutants in water sources worldwide has created a need for the development effective and selective oxidation methods complex matrices. This study is first report combination ferrate(VI) (Fe(VI)) periodate (PI) synergistic, rapid, elimination multiple micropollutants. combined system was found to outperform other Fe(VI)/oxidant systems (e.g., H2O2, peroxydisulfate, peroxymonosulfate) rapid decontamination. Scavenging, probing, electron spin resonance experiments showed that high-valent Fe(IV)/Fe(V) intermediates, rather than hydroxyl radicals, superoxide singlet oxygen, iodyl played dominant role process. Further, generation evidenced directly by 57Fe Mössbauer spectroscopic test. Surprisingly, reactivity PI toward Fe(VI) low (0.8223 M-1 s-1) at pH 8.0, implying not acting as an activator. Besides, only iodine sink PI, iodate also enhanced micropollutant abatement oxidation. Further proved and/or might function ligands, causing utilization efficiency intermediates pollutant outcompete their auto-decomposition. Finally, oxidized products plausible transformation pathways three different single Fe(VI)/PI were characterized elucidated. Overall, this proposed novel strategy (i.e., system) could efficiently eliminate clarified unexpected interactions between PI/iodate accelerated

Язык: Английский

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Antimicrobial Transformation Products in the Aquatic Environment: Global Occurrence, Ecotoxicological Risks, and Potential of Antibiotic Resistance

Environmental Science & Technology, Год журнала: 2023, Номер 57(26), С. 9474 - 9494

Опубликована: Июнь 19, 2023

The global spread of antimicrobial resistance (AMR) is concerning for the health humans, animals, and environment in a One Health perspective. Assessments AMR associated environmental hazards mostly focus on parent compounds, while largely overlooking their transformation products (TPs). This review lists TPs identified surface water environments examines potential promotion, ecological risk, as well human using silico models. Our also summarizes key compartments TPs, related pathways reaching waters methodologies studying fate TPs. 56 covered by were prioritized via scoring ranking various risk hazard parameters. Most data occurrences to date have been reported Europe, little known about antibiotic Africa, Central South America, Asia, Oceania. Occurrence antiviral other antibacterial are even scarcer. We propose evaluation structural similarity between compounds TP assessment. predicted 13 especially tetracyclines macrolides. estimated ecotoxicological effect concentrations from experimental chemical bacteria, algae fleas, scaled potency differences quantitative structure–activity relationships (QSARs) baseline toxicity scaling factor similarity. Inclusion mixtures with increased quotient over threshold one 7 24 antimicrobials included this analysis, only had above one. Thirteen which 6 macrolide posed at least three tested species. There 12/21 that likely exhibit similar or higher level mutagenicity/carcinogenicity, respectively, than compound, tetracycline often showing mutagenicity. carcinogenicity belonged sulfonamides. be mobile but not bioaccumulative, 14 persistent. six highest-priority originated family antivirals. review, particular our concern, can support authorities planning intervention strategies source mitigation toward sustainable future.

Язык: Английский

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Animal production predominantly contributes to antibiotic profiles in the Yangtze River

Water Research, Год журнала: 2023, Номер 242, С. 120214 - 120214

Опубликована: Июнь 10, 2023

Язык: Английский

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Redox-Active Polymers as Robust Electron-Shuttle Co-Catalysts for Fast Fe³⁺/Fe²⁺ Circulation and Green Fenton Oxidation

Environmental Science & Technology, Год журнала: 2023, Номер 57(8), С. 3334 - 3344

Опубликована: Фев. 3, 2023

Accelerating the rate-limiting Fe3+/Fe2+ circulation in Fenton reactions through addition of reducing agents (or co-catalysts) stands out as one most promising technologies for rapid water decontamination. However, conventional such hydroxylamine and metal sulfides are greatly restricted by three intractable challenges: (1) self-quenching effects, (2) heavy dissolution, (3) irreversible capacity decline. To this end, we, first time, introduced redox-active polymers electron shuttles to expedite cycle promote H2O2 activation. The reduction Fe3+ mainly took place at active N–H or O–H bonds a proton-coupled transfer process. As carriers, H atoms solid phase could effectively inhibit radical quenching, avoid maintain long-term via facile regeneration. Experimental density functional theory (DFT) calculation results indicated that activity different shows volcano curve trend function energy barrier, highest occupied molecular orbital–lowest unoccupied orbital (HOMO–LUMO) gap, vertical ionization potential. Thanks appropriate redox ability, polyaniline outperforms other (e.g., poypyrrole, hydroquinone resin, poly(2,6-diaminopyridine), hexaazatrinaphthalene framework) with iron up 5.5 mmol/g, which corresponds state transformation from leucoemeraldine emeraldine. Moreover, proposed system exhibited high pollutant removal efficiency flow-through reactor 8000 bed volumes without an obvious decline performance. Overall, work established green sustainable oxidation system, offers great potential practical organic wastewater remediation.

Язык: Английский

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