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Effect of Solution pH on the Dual Role of Dissolved Organic Matter in Sensitized Pollutant Photooxidation.

ABSTRACT: Dissolved organic matter (DOM) has a dual role in indirect phototransformations of aquatic contaminants by acting both as a photosensitizer and an inhibitor. Herein, the pH dependence of the inhibitory effect of DOM and the underlying mechanisms were studied in more than 400 kinetic irradiation experiments over the pH range of 6-11. Experiments employed various combinations of one of three DOM isolates, one of two model photosensitizers, the model antioxidant phenol, and one of nine target compounds (TCs), comprising several aromatic amines, in particular anilines and sulfonamides, and 4-cyanophenol. Using model photosensitizers without antioxidants, the phototransformation of most TCs increased with increasing pH, even for TCs for which pH did not affect speciation. This trend was attributed to pH-dependent formation yields of TC-derived radicals and their re-formation to the parent TC. Analogous trends were observed with DOM as a photosensitizer. Comparison of model and DOM photosensitizer data sets showed increasing inhibitory effects of DOM on TC phototransformation kinetics with increasing pH. In systems with anilines as a TC and phenol as a model antioxidant, pH trends of the inhibitory effect could be rationalized based on the reduction potential difference (ΔE_red) of phenoxyl/phenol and anilinyl/aniline couples. Our results indicate that the light-induced transformation of aromatic amines in the aquatic environment is governed by the pH-dependent inhibitory effects of antioxidant phenolic moieties of DOM and pH-dependent processes related to the formation of amine oxidation intermediates.

SUBMITTER: Wenk J

PROVIDER: S-EPMC8735754 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Data for dynamics analysis of soil dissolved organic matter. Long term amendment effect.

Project description:The data presented here are related to the research paper entitled "Spectral characteristics of soil dissolved organic matter: long-term effects of exogenous organic matter on soil organic matter and spatial-temporal changes" (Musadji et al., 2020). Fluorescence Excitation-Emission Matrixes and DOC content of 39 suction cup soil solutions are given for a control and an urban green waste compost amended soil sampled in spring and autumn. Principal component analysis (PCA) was used to identify possible spatial-temporal trends and to emphasize the long term effect of organic amendment on soil organic matter quality.

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Project description:We examined the molecular composition of forest soil water during three different seasons at three different sites, using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). We examined oxic soils and tested the hypothesis that pH and season correlate with the molecular composition of dissolved organic matter (DOM). We used molecular formulae and their relative intensity from ESI-FT-ICR-MS for statistical analysis. Applying unconstrained and constrained ordination methods, we observed that pH, dissolved organic carbon (DOC) concentration and season were the main factors correlating with DOM molecular composition. This result is consistent with a previous study where pH was a main driver of the molecular differences between DOM from oxic rivers and anoxic bog systems in the Yenisei River catchment. At a higher pH, the molecular formulae had a lower degree of unsaturation and oxygenation, lower molecular size and a higher abundance of nitrogen-containing compounds. These characteristics suggest a higher abundance of tannin connected to lower pH that possibly inhibited biological decomposition. Higher biological activity at a higher pH might also be related to the higher abundance of nitrogen-containing compounds. Comparing the seasons, we observed a decrease in unsaturation, molecular diversity and the number of nitrogen-containing compounds in the course of the year from March to November. Temperature possibly inhibited biological degradation during winter, which could cause the accumulation of a more diverse compound spectrum until the temperature increased again. Our findings suggest that the molecular composition of DOM in soil pore waters is dynamic and a function of ecosystem activity, pH and temperature.

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Microbes incubated Microplastics-derived dissolved organic matter

Project description:Microbes incubated Microplastics-derived dissolved organic matter Raw sequence reads

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HBH0622 Dissolved Organic Matter

Project description:DOM extraction in oceanic samples was carried out using PPL cartridges.

2022-11-09 | MSV000090678 | MassIVE

Universal molecular structures in natural dissolved organic matter.

Project description:Natural dissolved organic matter (DOM) comprises a broad range of dissolved organic molecules in aquatic systems and is among the most complex molecular mixtures known. Here we show, by comparing detailed structural fingerprints of individual molecular formulae in DOM from a set of four marine and one freshwater environments, that a major component of DOM is molecularly indistinguishable in these diverse samples. Molecular conformity was not only apparent by the co-occurrence of thousands of identical molecular formulae, but also by identical structural features of those isomers that collectively represent a molecular formula. The presence of a large pool of compounds with identical structural features in DOM is likely the result of a cascade of degradation processes or common synthetic pathways that ultimately lead to the formation of a universal background, regardless of origin and history of the organic material. This novel insight impacts our understanding of long-term turnover of DOM as the underlying mechanisms are possibly universal.

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Project description:Solar photoexcitation of chromophoric groups in dissolved organic matter (DOM), when coupled to photoreduction of ubiquitous Fe(III)-oxide nanoparticles, can significantly accelerate DOM degradation in near-surface terrestrial systems, but the mechanisms of these reactions remain elusive. We examined the photolysis of chromophoric soil DOM coated onto hematite nanoplatelets featuring (001) exposed facets using a combination of molecular spectroscopies and density functional theory (DFT) computations. Reactive oxygen species (ROS) probed by electron paramagnetic resonance (EPR) spectroscopy revealed that both singlet oxygen and superoxide are the predominant ROS responsible for DOM degradation. DFT calculations confirmed that Fe(II) on the hematite (001) surface, created by interfacial electron transfer from photoexcited chromophores in DOM, can reduce dioxygen molecules to superoxide radicals (•O2-) through a one-electron transfer process. 1H nuclear magnetic resonance (NMR) and electrospray ionization Fourier-transform ion cyclotron resonance mass spectrometry (ESI-FTICR-MS) spectroscopies show that the association of DOM with hematite enhances the cleavage of aromatic groups during photodegradation. The findings point to a pivotal role for organic matter at the interface that guides specific ROS generation and the subsequent photodegradation process, as well as the prospect of using ROS signatures as a forensic tool to help interpret more complicated field-relevant systems.

| S-EPMC10867828 | biostudies-literature

Photooxidation of atrazine and its influence on disinfection byproducts formation during post-chlorination: effect of solution pH and mechanism.

Project description:Partial photooxidation of micropollutants may lead to various degradation intermediates, obviously affecting disinfection byproducts (DBPs) formation during the post-chlorination process. The photooxidation of atrazine (ATZ) in aqueous solutions with low-pressure mercury UV lamps in UV, UV/H2O2 and UV/TiO2 treatment system and the formation of chlorinated disinfection byproducts (DBPs) during subsequent chlorination processes including dichloroacetic acid (DCAA), trichloroacetic acid (TCAA), 1,1,1-trichloro-2-propanone (TCP), trichloromethane (TCM) and chloropicrin (CHP) were investigated in this study. The effect of solution pH on the oxidation pathway of ATZ in three UV photooxidation treatment process and the impact of photooxidation on the DBPs formations were assessed. Based on UPLC-ESI-MS/MS analyses, identification of main oxidation intermediates was performed and the plausible degradation pathways of ATZ in photooxidation system were proposed, indicating that photooxidation of ATZ in UV/H2O2 and UV/TiO2 process system was significantly pH-dependent processes. Dichloroacetic acid (DCAA), trichloroacetic acid (TCAA), 1,1,1-trichloro-2-propanone (TCP), trichloromethane (TCM) and chloropicrin (CHP) were detected in photooxidized ATZ solutions. Compared to the other three DBPs, TCM and TCP were the main DBPs formed. The DBPs formations were greatly promoted in oxidized ATZ solutions. Solution pH and UV irradiation time exhibited obvious impact on the DBPs formation on the basis of DBP species. The variation tendency of DBPs observed relates to the combustion of ATZ in photooxidation system and the production oxidation intermediates.

| S-EPMC7684306 | biostudies-literature

Dissolved Organic Matter in the Global Ocean: A Primer.

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| S-EPMC7584329 | biostudies-literature

Global effects of agriculture on fluvial dissolved organic matter.

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| S-EPMC4635380 | biostudies-literature

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