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2.
Environ Sci Technol ; 57(40): 15004-15013, 2023 10 10.
Artigo em Inglês | MEDLINE | ID: mdl-37782146

RESUMO

Growing evidence indicates that rivers are hotspots of greenhouse gas (GHG) emissions and play multiple roles in the global carbon budget. However, the roles of terrestrial carbon from land use in river GHG emissions remain largely unknown. We studied the microbial composition, dissolved organic matter (DOM) properties, and GHG emission responses to different landcovers in rivers (n = 100). The bacterial community was mainly constrained by land-use intensity, whereas the fungal community was mainly controlled by DOM chemical composition (e.g., terrestrial DOM with high photoreactivity). Anthropogenic stressors (e.g., land-use intensity, gross regional domestic product, and total population) were the main factors affecting chromophoric DOM (CDOM). DOM biodegradability exhibited a positive correlation with CDOM and contributed to microbial activity for DOM transformation. Variations in CO2 and CH4 emissions were governed by the biodegradation or photomineralization of dissolved organic carbon derived from autotrophic DOM and were indirectly affected by land use via changes in DOM properties and water chemistry. Because the GHG emissions of rivers offset some of the climatic benefits of terrestrial carbon (or ocean) sinks, intensified urban land use inevitably alters carbon cycling and changes the regional microclimate.


Assuntos
Matéria Orgânica Dissolvida , Gases de Efeito Estufa , Rios , Carbono , Matéria Orgânica Dissolvida/análise , Gases de Efeito Estufa/análise , Rios/química , China
3.
Environ Pollut ; 334: 122116, 2023 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-37394053

RESUMO

Tire tread particles (TTP) are environmentally prevalent microplastics and generate toxic aqueous leachate. We determined the total carbon and nitrogen leachate concentrations and chemical profiles from micron (∼32 µm) and centimeter (∼1 cm) TTP leachate over 12 days. Dissolved organic carbon (DOC) and total dissolved nitrogen (TDN) were used to measure the concentration of leached compounds. Nontargeted chemical analysis by comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC×GC/TOF-MS) was used to compare the chemical profiles of leachates. After leaching for 12 days, DOC was 4.0 times higher in the micron TTP leachate than in the centimeter TTP leachate, and TDN was 2.6 times higher. The total GC×GC/TOF-MS chromatographic feature peak area was 2.9 times greater in the micron TTP leachate than the centimeter TTP leachate, and similarly, the total relative abundance of 54 tentatively identified compounds was 3.3 times greater. We identified frequently measured tire-related chemicals, such as 6PPD, N-cyclohexyl-N'-phenylurea (CPU), and hexa(methoxymethyl)melamine (HMMM), but nearly 50% of detected chemicals were not previously reported in tire literature or lacked toxicity information. Overall, the results demonstrate that smaller TTP have a greater potential to leach chemicals into aquatic systems, but a significant portion of these chemicals are not well-studied and require further risk assessment.


Assuntos
Matéria Orgânica Dissolvida , Fenilenodiaminas , Plásticos , Poluentes Químicos da Água , Matéria Orgânica Dissolvida/análise , Matéria Orgânica Dissolvida/química , Matéria Orgânica Dissolvida/classificação , Cromatografia Gasosa-Espectrometria de Massas , Plásticos/análise , Plásticos/química , Plásticos/classificação , Tamanho da Partícula , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/química , Poluentes Químicos da Água/classificação , Fenilenodiaminas/análise , Fenilenodiaminas/química , Fenilenodiaminas/classificação , Medição de Risco
4.
Environ Sci Technol ; 57(11): 4668-4678, 2023 03 21.
Artigo em Inglês | MEDLINE | ID: mdl-36892554

RESUMO

Alpine river and lake systems on the Tibetan Plateau are highly sensitive indicators and amplifiers of global climate change and important components of the carbon cycle. Dissolved organic matter (DOM) encompasses organic carbon in aquatic systems, yet knowledge about DOM variation throughout the river-lake aquatic continuum within alpine regions is limited. We used optical spectroscopy, ultrahigh-resolution mass spectrometry (Fourier transform ion cyclotron resonance mass spectrometry), and stable water isotopic measurements to evaluate linkages between DOM composition and hydrological connection. We investigated glacial influences on DOM composition throughout the watershed of Selin Co, including upstream glacier-fed rivers and downstream-linked lakes. We found that the dissolved organic carbon concentration increased, whereas specific ultraviolet absorbance (SUVA254) decreased along the river-lake continuum. Relative to rivers, the downstream lakes had low relative abundances of polyphenolic and condensed aromatic compounds and humic-like substances but increased relative abundances of aliphatics and protein-like compounds. SUVA254 decreased while protein-like components increased with enriched stable water isotope δ2H-H2O, indicating that DOM aromaticity declined while autochthonous production increased along the flow paths. Glacier meltwater contributed to elevated relative abundances of aliphatic and protein-like compounds in headwater streams, while increased relative abundances of aromatics and humic-like DOM were found in glacier-fed lakes than downstream lakes. We conclude that changes in hydrological conditions, including glacier melt driven by a warming climate, will significantly alter DOM composition and potentially their biogeochemical function in surface waters on the Tibetan Plateau.


Assuntos
Matéria Orgânica Dissolvida , Hidrologia , Lagos , Matéria Orgânica Dissolvida/análise , Lagos/análise , Lagos/química , Tibet , Movimentos da Água , Rios , Congelamento , Espectrometria de Massas , Hidrogênio , Isótopos de Oxigênio , Volatilização
5.
Chemosphere ; 323: 138285, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36868424

RESUMO

Anion exchange resin is responsible for removing harmful anionic contaminants in drinking water treatment, but it may become a significant source of precursors for disinfection byproducts (DBPs) by shedding material during application without proper pretreatment. Batch contact experiments were performed to investigate the dissolution of magnetic anion exchange resins and their contribution to organics and DBPs. Dissolved organic carbon (DOC) and dissolved organic nitrogen (DON) released from the resin were highly correlated with the dissolution conditions (contact time and pH), in which 0.7 mg/L DOC and 0.18 mg/L DON were distributed at exposure time of 2 h and pH 7. The formation potential of four DBPs in the shedding fraction was also revealed that trichloromethane (TCM), dichloroacetonitrile (DCAN), nitrosodimethylamine (NDMA), and dichloroacetamide (DCAcAm) concentrations could reach 21.4, 5.1, 12.1 µg/L, and 69.6 ng/L, respectively. Furthermore, the hydrophobic DOC that preferred to detach from the resin mainly originated from the residues of crosslinkers (divinylbenzene) and porogenic agents (straight-chain alkanes) detected by LC-OCD and GC-MS. Nevertheless, pre-cleaning inhibited the leaching of the resin, among which acid-base and ethanol treatments significantly lowered the concentration of leached organics, and formation potential of DBPs (TCM, DCAN, and DCAcAm) below 5 µg/L and NDMA dropped to 10 ng/L.


Assuntos
Resinas de Troca Aniônica , Técnicas de Química Analítica , Purificação da Água , Resinas de Troca Aniônica/química , Purificação da Água/instrumentação , Matéria Orgânica Dissolvida/análise , Matéria Orgânica Dissolvida/química , Clorofórmio/análise , Clorofórmio/química , Dimetilnitrosamina/análise , Dimetilnitrosamina/química , Concentração de Íons de Hidrogênio , Microscopia Eletrônica de Varredura , Técnicas de Química Analítica/instrumentação , Técnicas de Química Analítica/métodos
6.
Artigo em Inglês | MEDLINE | ID: mdl-35954582

RESUMO

Dissolved organic matter (DOM) is a central component in the biogeochemical cycles of marine and terrestrial carbon pools, and its structural features greatly impact the function and behavior of ecosystems. In this study, the Wanggang River, which is a seagoing river that passes through Yancheng City, was selected as the research object. Three-dimensional (3D) fluorescence spectral data and UV−visible spectral data were used for component identification and source analysis of DOM based on the PARAFAC model. The results showed that the DOM content of the Wanggang River during the dry season was significantly higher than during the wet season; the DOM content increased gradually from the upper to lower reaches; the proportion of terrigenous components was higher during the wet season than during the dry. UV−Vis spectral data a280 and a355 indicated that the relative concentrations of protein-like components in the DOM of the Wanggang River were higher than those of humic-like components, and the ratio of aromatic substances in the DOM of the Wanggang River water was higher during the wet season. The DOM in the Wanggang River was dominated by protein-like components (>60%), and the protein-like components were dominated by tryptophan proteins (>40%). This study showed that the temporal and spatial distributions of DOM in rivers can be accurately determined using 3D fluorescence spectroscopy combined with the PARAFAC model. This provides useful insight into the biogeochemical process of DOM in rivers of coastal areas.


Assuntos
Matéria Orgânica Dissolvida , Rios , China , Matéria Orgânica Dissolvida/análise , Ecossistema , Reprodutibilidade dos Testes , Rios/química , Análise Espaço-Temporal , Espectrometria de Fluorescência/métodos
7.
Proc Natl Acad Sci U S A ; 119(5)2022 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-35101918

RESUMO

Metabolites exuded by primary producers comprise a significant fraction of marine dissolved organic matter, a poorly characterized, heterogenous mixture that dictates microbial metabolism and biogeochemical cycling. We present a foundational untargeted molecular analysis of exudates released by coral reef primary producers using liquid chromatography-tandem mass spectrometry to examine compounds produced by two coral species and three types of algae (macroalgae, turfing microalgae, and crustose coralline algae [CCA]) from Mo'orea, French Polynesia. Of 10,568 distinct ion features recovered from reef and mesocosm waters, 1,667 were exuded by producers; the majority (86%) were organism specific, reflecting a clear divide between coral and algal exometabolomes. These data allowed us to examine two tenets of coral reef ecology at the molecular level. First, stoichiometric analyses show a significantly reduced nominal carbon oxidation state of algal exometabolites than coral exometabolites, illustrating one ecological mechanism by which algal phase shifts engender fundamental changes in the biogeochemistry of reef biomes. Second, coral and algal exometabolomes were differentially enriched in organic macronutrients, revealing a mechanism for reef nutrient-recycling. Coral exometabolomes were enriched in diverse sources of nitrogen and phosphorus, including tyrosine derivatives, oleoyl-taurines, and acyl carnitines. Exometabolites of CCA and turf algae were significantly enriched in nitrogen with distinct signals from polyketide macrolactams and alkaloids, respectively. Macroalgal exometabolomes were dominated by nonnitrogenous compounds, including diverse prenol lipids and steroids. This study provides molecular-level insights into biogeochemical cycling on coral reefs and illustrates how changing benthic cover on reefs influences reef water chemistry with implications for microbial metabolism.


Assuntos
Antozoários/metabolismo , Matéria Orgânica Dissolvida/análise , Alga Marinha/metabolismo , Animais , Antozoários/genética , Antozoários/crescimento & desenvolvimento , Carbono/metabolismo , Recifes de Corais , Ecossistema , Biologia Marinha/métodos , Metabolômica/métodos , Nitrogênio/metabolismo , Nutrientes , Fósforo/metabolismo , Polinésia , Água do Mar/química , Alga Marinha/genética , Alga Marinha/crescimento & desenvolvimento
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