Singlet Oxygen Quantum Yields in Environmental Waters

Chemical Reviews, Год журнала: 2021, Номер 121(7), С. 4100 - 4146

Опубликована: Март 8, 2021

Singlet oxygen (1O2) is a reactive species produced in sunlit waters via energy transfer from the triplet states of natural sensitizers. There has been an increasing interest measuring apparent 1O2 quantum yields (ΦΔ) aquatic and atmospheric organic matter samples, driven part by fact that this parameter can be used for environmental fate modeling contaminants to advance our understanding dissolved photophysics. However, lack reproducibility across research groups publications remains challenge significantly limits usability literature data. In first review, we critically evaluate experimental techniques have determine ΦΔ values matter, identify quantify sources errors potentially explain large variability literature, provide general recommendations future studies. second part, qualitative overview known trends as function type, isolation extraction procedures, bulk water chemistry parameters, molecular spectroscopic features, chemical treatments, wavelength, season, location. This review supplemented with comprehensive database samples.

Язык: Английский

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Dissolved Organic Matter Promotes the Aging Process of Polystyrene Microplastics under Dark and Ultraviolet Light Conditions: The Crucial Role of Reactive Oxygen Species

Environmental Science & Technology, Год журнала: 2022, Номер 56(14), С. 10149 - 10160

Опубликована: Июль 6, 2022

Microplastics (MPs) interact frequently with dissolved organic matter (DOM) commonly found in the environment, but information on aging behavior of MPs under participation DOM is still lacking. Thus, polystyrene microplastic (PSMP) process was systematically studied by electron paramagnetic resonance spectroscopy, high-performance liquid chromatography, Fourier transform infrared (FTIR) and two-dimensional correlation spectroscopy analyses dark ultraviolet (UV) light conditions. to promote transfer generate reactive oxygen species (ROS) conditions PSMPs, while generating ROS UV more susceptible photoelectrons accelerated PSMPs. However, among four types, fulvic acid (FA) has a significant promoting effect PSMPs than humic acid, which can be attributed stronger conversion ability FA semiquinone radicals. Density functional theory calculations are used describe difference different structures plastics DOM. This study provides necessary theoretical basis for migration groundwater deep surface water.

Язык: Английский

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The Role of Dissolved Organic Matter Composition in Determining Photochemical Reactivity at the Molecular Level

Environmental Science & Technology, Год журнала: 2019, Номер 53(20), С. 11725 - 11734

Опубликована: Сен. 11, 2019

Dissolved organic matter (DOM) composition influences its ability to form photochemically produced reactive intermediates (PPRI). While relationships have been established between bulk DOM properties and triplet (3DOM) singlet oxygen (1O2) quantum yields, contradictory evidence exists for hydroxyl radical (•OH) hydroxylating species. Furthermore, little is known about these at the molecular level. We evaluated photochemical reactivity of water samples from a wastewater treatment plant St. Louis River in Minnesota Wisconsin, U.S.A. Bulk characterization using ultraviolet-visible spectroscopy demonstrates that color apparent size decrease downstream, while analysis Fourier-transform ion cyclotron resonance mass spectrometry reveals saturation chemodiversity highest near Lake Superior. 3DOM yield coefficients 1O2 yields increase downstream correlate strongly with saturated formulas. Similar results are observed carbon-normalized photodegradation rate constants atorvastatin, carbamazepine, venlafaxine, which react primarily 1O2. In contrast, •OH lowest less saturated, more oxygenated DOM, suggesting not major precursor. Mixed DEET, reacts multiple PPRI. Molecular-level compositional data reveal insights into differing formation pathways individual PPRI, but information specific contaminants needed predict their fate.

Язык: Английский

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Characteristics of microplastic polymer-derived dissolved organic matter and its potential as a disinfection byproduct precursor

Water Research, Год журнала: 2020, Номер 175, С. 115678 - 115678

Опубликована: Март 4, 2020

Язык: Английский

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Triplet-State Photochemistry of Dissolved Organic Matter: Triplet-State Energy Distribution and Surface Electric Charge Conditions

Environmental Science & Technology, Год журнала: 2019, Номер 53(5), С. 2482 - 2490

Опубликована: Фев. 13, 2019

Excited triplet states of chromophoric dissolved organic matter (3CDOM*) are highly reactive species in sunlit surface waters and play a critical role oxygen (ROS) formation pollutant attenuation. In the present study, series chemical probes, including sorbic acid, alcohol, amine, trimethylphenol, furfuryl were employed to quantitatively determine 3CDOM* 1O2 various matters. Using high concentration alcohol as high-energy quencher, can be first distinguished (>250 kJ mol–1) low-energy (<250 mol–1). The terrestrial-origin natural (NOM) was found mainly consist states, while predominant autochthonous-origin NOM effluent/wastewater (EfOM/WWOM). quantum yields electron transfer yield coefficients (fTMP) generated from remained constant all tested External phenolic compound showed quenching effects on triplet-state tended have higher efficiency for aromatic ketone which main states. comparison with NOM, EfOM/WWOM presented lower reaction rate constants amines these differences likely due dissimilar electric charge conditions. Understanding photochemistry CDOM is essential providing useful insights into their photochemical aquatic systems.

Язык: Английский

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Humic Acid and Fulvic Acid Hinder Long-Term Weathering of Microplastics in Lake Water

Environmental Science & Technology, Год журнала: 2021, Номер 55(23), С. 15810 - 15820

Опубликована: Ноя. 10, 2021

We investigated the photoaging of polypropylene (PP) microplastics (MPs) in lake water. The results showed that PP MPs was significantly inhibited water compared with ultrapure after 12 d ultraviolet (UV) irradiation, and humic acid fulvic acid, rather than carbonate (CO32–), nitrate (NO3–), or chloride (Cl–) ions, were identified as primary contributors to observed inhibition. Mechanisms for roles (Suwannee River acid) (Pony Lake reducing rates photodegradation acted both reactive oxygen species (ROS) scavengers (e.g., •OH) (dominant contribution) optical light filters. As ROS scavengers, decreased capacity formation •OH O2•– by under irradiation. In addition, chromophores competed photons through light-shielding effect, thereby causing less fragmentation particles changes other properties (melting temperature, contact angle, surface zeta potential). proposed mechanisms inhibition will aid our efforts assess duration aging alterations MP during long-term weathering natural waters.

Язык: Английский

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Recent advances on microplastic aging: Identification, mechanism, influence factors, and additives release

The Science of The Total Environment, Год журнала: 2023, Номер 889, С. 164035 - 164035

Опубликована: Май 18, 2023

Язык: Английский

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The aging behaviors and release of microplastics: A review

Gondwana Research, Год журнала: 2021, Номер 108, С. 60 - 71

Опубликована: Ноя. 10, 2021

Язык: Английский

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Comparing Photoactivities of Dissolved Organic Matter Released from Rice Straw-Pyrolyzed Biochar and Composted Rice Straw

Environmental Science & Technology, Год журнала: 2022, Номер 56(4), С. 2803 - 2815

Опубликована: Янв. 28, 2022

Here, we systematically compared the photoactivity and photobleaching behavior between dissolved black carbon (DBC) from rice straw biochar leached organic (LDOC) compost using complementary techniques. The Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis showed that DBC was dominated by polycyclic aromatic (55.1%) tannin-like molecules (24.1%), while LDOC lignin-like (58.9%) (19.7%). Under simulated sunlight conditions, had much higher apparent quantum yields for 3DOM* 1O2 but lower •OH than LDOC. After a 168 h irradiation, total number of formulas identified FT-ICR MS decreased 40.1% with concurrent increases in O/C H/C ratios also decreases double bond equivalence minus oxygen (DBE – O) average molecular weight gel permeation chromatography. However, despite large UVA254 DOC, only 12.0% nearly unchanged ratio, DBE O values, distribution, benzenepolycarboxylic condensation (BACon) index regardless percentage condensed (ConAC %). Compared LDOC, photolysis less oxidative destructive mainly via breakup small portion highly rings, probably accompanied photodecarboxylation.

Язык: Английский

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Dissolved Organic Matter Photoreactivity Is Determined by Its Optical Properties, Redox Activity, and Molecular Composition

Environmental Science & Technology, Год журнала: 2023, Номер 57(16), С. 6703 - 6711

Опубликована: Апрель 11, 2023

Predicting the formation of photochemically produced reactive intermediates (PPRI) during irradiation dissolved organic matter (DOM) has remained challenging given complex nature this material and differences in PPRI mechanisms. We investigate role DOM composition photoreactivity using 48 samples that span range freshwater systems wastewater. relate quantum yields for excited triplet-state (fTMP), singlet oxygen (Φ1O2), hydroxylating species (Φ•OH) to determined spectroscopy, Fourier-transform ion cyclotron resonance mass spectrometry, electron-donating capacity (EDC). fTMP Φ1O2 follow similar trends are correlated with bulk properties derived from UV–vis spectra EDC. In contrast, no individual property can be used predict Φ•OH. At molecular level, subset is positively both Φ•OH EDC distinct formulas related Φ1O2, demonstrating •OH 1O2 formed different fractions. Multiple linear regressions each parameters multiple techniques, complementary methods ideal characterizing because technique only a DOM.

Язык: Английский

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