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1.
Water Res ; 266: 122355, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39226743

RESUMEN

In recent decades, global aquaculture has expanded rapidly, raising concerns about coastal environmental degradation due to unregulated or poorly regulated discharge of aquaculture tailwater. Despite the crucial role of dissolved organic matter (DOM) in biogeochemical processes and aquatic biodiversity, the influence of aquaculture type on the molecular characteristics of DOM remains largely unexplored. Herein, this study investigated the variations in chemical and spectroscopic properties as well as molecular characteristics and composition of DOM across different aquaculture types including crustacean, fish and shellfish. Our findings revealed notable differences in DOM quantities among different aquaculture types, with crustacean and fish aquaculture water containing higher DOM amount compared to shellfish aquaculture water. This disparity can be attributed to the more frequent formulated feeds of crustacean and fish in contrast to shellfish aquaculture. Furthermore, distinct differences were also observed in the characteristics and composition of DOM among the different aquaculture waters. Specifically, DOM in shellfish aquaculture water exhibited a higher abundance of unsaturated and reduced molecules as well as increased aromaticity compared to the other two aquaculture waters. Conversely, DOM from fish aquaculture water showed a greater contribution from terrestrial origin characterized by elevated levels of plant-based components such as lignin-like and tannin-like compounds. Interestingly, DOM from shellfish aquaculture water contained lower levels of microbial-derived components such as lipid-like and protein-like compounds, likely due to reduced microorganism populations resulting from lower nutrients availability and higher salinity. Overall, these significant variations in characteristics and composition of DOM underscore the potential impacts of aquaculture type on the DOM biogeochemical cycle and the environmental quality in aquatic ecosystems.

2.
Water Environ Res ; 96(9): e11125, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39258546

RESUMEN

This study aims to identify continuous water quality changes and identify fluorescence properties from urban rivers to marine zones. Various types of natural and anthropogenic sources derived dissolved organic matter (DOM) have been identified in this study. These include soil-derived DOM, plant remnants, and soluble particles produced when organic material partially decomposes and is released by microorganisms, such as bacteria, algae, and plants. DOM was characterized using a three-dimensional excitation-emission matrix (3DEEM), parallel factor analysis (PARAFAC), and water quality parameters from the Buriganga River, Dhaka to Patenga Seaport, Chittagong, along with the Shitalakshya River, a small portion of the Padma River, and the Meghna River. To better understand the data analysis, the study area was divided into three central regions: urban industrial rivers, industrial estuarine rivers, and marine zones. In the urban industrial river, 3DEEM and PARAFAC identified five fluorophores (peaks: A, C, M, T, and Tuv) with five components: detergent-like, fulvic-like, tryptophan or protein-like, fulvic-like (C-type), and protein-like, which might originate from the industrial activities and sewage pollution. In the industrial estuarine river zone, three fluorophores have been identified (peaks: A, C, Tuv) with two known components, namely, fulvic acid (A-type) and fulvic acid (C-type), with an unknown photoproduct at Ex/Em = 295/368 (peak Tuv). Components in the industrial river zone may originate from terrestrial sources, indicating vegetation along the river. In the marine zone, four fluorophores have been identified (peaks: Tuv, A, T, C) with two components, that is, protein- or tryptophan-like and humic acid-like from coral origin. The intensities of both fulvic-like and protein-like substances were high in urban industrial river water owing to industrial activity and sewage pollution. SUVA254 suggests high aromaticity in all three regions, whereas the optical properties suggest that terrestrial and microbial components are present in the urban industrial and estuarine rivers. This further indicates that urban industrial river water quality is highly polluted. The lowest degradation potential index (DPI) in the marine zone might result from the presence of the highest number of dissolved solids in the water, and the highest DPI of industrial estuarine rivers explains the comparatively high presence of terrestrial-derived humic (A)- and humic (C)-like components in the ratio to the unknown photoproduct of mid-wavelength. PRACTITIONER POINTS: This study's uniqueness is a 220-km cruise from an urban river to a coastal seaport to analyze fluorescence properties. The study found that most water parameters were within the DoE standards, except for DO, which was consistently low. 3DEEM-PARAFAC identified five fluorophores linked to detergent, fulvic, and protein-like substances from sewage and industrial sources. Our study concludes that microbial and terrestrial sources dominate dissolved organic matter in urban, estuarine, and marine regions.


Asunto(s)
Monitoreo del Ambiente , Ríos , Calidad del Agua , Ríos/química , Compuestos Orgánicos/análisis , Contaminantes Químicos del Agua/análisis , Fluorescencia , Ciudades
3.
Environ Sci Pollut Res Int ; 31(39): 52253-52266, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-39145910

RESUMEN

Dissolved organic matter (DOM) in landfill leachate impacts the toxicity, bioavailability, and migration of heavy metals. The present study investigated the complexation of heavy metals (Cu2+ and Pb2+) with DOM from two landfill leachate samples, representing an old landfill site containing incineration residues and incombustible waste. The logarithms of the stability constant (log KM) and percentage of complexed fluorophores were calculated using both the Ryan-Weber non-linear model and the modified Stern-Volmer model, yielding good agreement. The log KM values (at pH = 6.0 ± 0.1) calculated using both methods for the two sampling points were 5.02-5.13 and 4.85-5.11 for Cu2+-DOM complexation, and 5.01-5.13 and 4.46-4.87 for Pb2+-DOM complexation, respectively. Log KM was slightly higher for binding of DOM with Cu2+ than Pb2+, and the quenching degree was stronger for complexation with Cu2+ (28.5-30.6% and 38.0-45.9%) than Pb2+ (6.5-7.1% and 10.0-15.4%) in both leachate samples. While log KM values were similar, differences in the contributions of functional groups and molecular composition led to varying degrees of quenching. This study reveals the potential for heavy metal binding by DOM in landfill leachate with a unique solid waste composition and emphasizes variations in fluorescence quenching between Cu2+ and Pb2+ despite similar log KM levels. These findings may be useful for assessing heavy metal behavior in landfill leachate and its impacts on the surrounding environment.


Asunto(s)
Metales Pesados , Instalaciones de Eliminación de Residuos , Contaminantes Químicos del Agua , Cobre/química , Monitoreo del Ambiente/métodos , Fluorescencia , Japón , Plomo/química , Metales Pesados/química , Contaminantes Químicos del Agua/química
4.
Sci Total Environ ; 951: 175768, 2024 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-39191325

RESUMEN

The river course is a transitional area connecting the source and receiving water bodies. The dissolved organic matter (DOM) in the river course is an important factor affecting the aquatic environment and ecological health. However, there are shortcomings in studying the differences and quantitative contributions of river DOM in different seasons and sources. In this study, ultraviolet-visible (UV-vis) and three-dimensional fluorescence spectra were used to characterize the optical properties, analyze the spatiotemporal changes, and establish the quantitative relationship between environmental factors and DOM in the inflow rivers of Baiyangdian Lake. The results showed that the relative DOM concentrations in summer and autumn were significantly higher than those in the other seasons (P < 0.001) and that the DOM source (SR < 1) was mainly exogenous. The fluorescence abundance of protein-like substances (C1 + C2 + C3) was the highest in spring, whereas that of humus C4 was the highest in autumn. Moreover, the inflow rivers exhibited strong autogenetic characteristics (BIX > 1) throughout the year. Self-organizing maps (SOM) indicated that the main driving factors of water quality were NO3--N in spring, autumn, and winter and DO, pH, and chemical oxygen demand (COD) in summer. Random forest analysis showed that the fluorescent components (C1-C4) were closely related to the migration and transformation of nitrogen, and pH and nitrogen were the main predictors of each component. The Mantel test and structural equation model (SEM) showed that temperature and NO3--N significantly influenced the DOM concentration, components, and molecular properties in different seasons. Moreover, the river source also affected the distribution mechanism of DOM in the water body. Our study comprehensively analyzed the response of DOM in inflow rivers in different seasons and water sources, providing a basis for further understanding the driving mechanisms of water quality.

5.
Environ Geochem Health ; 46(9): 350, 2024 Jul 29.
Artículo en Inglés | MEDLINE | ID: mdl-39073511

RESUMEN

Dissolved organic matter (DOM), a pivotal component in the global carbon cycle, plays a crucial role in maintaining the productivity and functionality of aquatic ecosystems. However, the driving factors of variations in the properties of riverine DOM in tropical islands still remain unclear. In this study, the spatiotemporal response of the optical characteristics of riverine DOM to seasonality and land use on Hainan Island in southern China was investigated. Our results revealed that DOM in the rivers of Hainan Island exhibited a relatively high proportion of fulvic acid and demonstrated strong terrestrial sources. The optical properties of DOM exhibited significant variations both seasonally and spatially. Land use exerted a dominant influence on riverine DOM. Specifically, during the wet season, riverine DOM exhibited larger molecular weight, increased chromophoric DOM (CDOM) abundance, and higher Fmax compared to the dry season. Furthermore, riverine DOM influenced by grassland and farmland showed higher CDOM abundance, Fmax, and humification degree in contrast to those impacted by forest and urban. Random forest and correlation analysis results indicated that grassland and farmland enhanced the Fmax of DOM by increasing levels of TP, NO3--N, Chl a, and NH4+-N in the dry season. However, during the wet season, the increased Fmax of DOM induced by grassland and farmland relied on the increments of Chl a and TP concentrations. This study improves our understanding of the spatiotemporal fluctuations of DOM in the rivers of Hainan Island, highlighting the effects of season and land use on DOM. It offers valuable support for improving water quality and contributes to enhancing human comprehension of the global carbon cycle.


Asunto(s)
Monitoreo del Ambiente , Ríos , Estaciones del Año , Ríos/química , China , Monitoreo del Ambiente/métodos , Islas , Clima Tropical , Análisis Espacio-Temporal , Sustancias Húmicas/análisis , Agricultura , Compuestos Orgánicos/análisis , Benzopiranos/análisis
6.
Sci Total Environ ; 947: 174469, 2024 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-38972419

RESUMEN

Understanding the transformation process of dissolved organic matter (DOM) in the sewer is imperative for comprehending material circulation and energy flow within the sewer. The machine learning (ML) model provides a feasible way to comprehend and simulate the DOM transformation process in the sewer. In contrast, the model accuracy is limited by data restriction. In this study, a novel framework by integrating generative adversarial network algorithm-machine learning models (GAN-ML) was established to overcome the drawbacks caused by the data restriction in the simulation of the DOM transformation process, and humification index (HIX) was selected as the output variable to evaluate the model performance. Results indicate that the GAN algorithm's virtual dataset could generally enhance the simulation performance of regression models, deep learning models, and ensemble models for the DOM transformation process. The highest prediction accuracy on HIX (R2 of 0.5389 and RMSE of 0.0273) was achieved by the adaptive boosting model which belongs to ensemble models trained by the virtual dataset of 1000 samples. Interpretability analysis revealed that dissolved oxygen (DO) and pH emerge as critical factors warranting attention for the future development of management strategies to regulate the DOM transformation process in sewers. The integrated framework proposed a potential approach for the comprehensive understanding and high-precision simulation of the DOM transformation process, paving the way for advancing sewer management strategy under data restriction.

7.
Water Res ; 262: 122053, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-39059199

RESUMEN

Biofiltration is a low-cost, low-energy technology that employs a biologically activated bed of porous medium to reduce the biodegradable fraction of the dissolved organic matter (DOM) pool in source water, resulting in the production of drinking water. Microbial communities at different bed depths within the biofilter play crucial roles in the degradation and removal of dissolved organic carbon (DOC), ultimately impacting its performance. However, the relationships between the composition of microbial communities inhabiting different biofilter depths and their utilisation of various DOC fractions remain poorly understood. To address this knowledge gap, we conducted an experimental study where microbial communities from the upper (i.e., top 10 cm) and lower (i.e., bottom 10 cm) sections of a 30-cm long laboratory-scale biofilter were recovered. These communities were then individually incubated for 10 days using the same source water as the biofilter influent. Our study revealed that the bottom microbial community exhibited lower diversity yet had a co-occurrence network with a higher degree of interconnections among its members compared to the top microbial community. Moreover, we established a direct correlation between the composition and network structure of the microbial communities and their ability to utilise various DOM compounds within a DOM pool. Interestingly, although the bottom microbial community had only 20 % of the total cell abundance compared to the top community at the beginning of the incubation, it utilised and hence removed approximately 60 % more total DOC from the DOM pool than the top community. While both communities rapidly utilised labile carbon fractions, such as low-molecular-weight neutrals, the utilisation of more refractory carbon fractions, like high-molecular-weight humic substances with an average molecular weight of more than ca. 1451 g/mol, was exclusive to the bottom microbial community. By employing techniques that capture microbial diversity (i.e., flow cytometry and 16S rRNA amplicon sequencing) and considering the complexities of DOM (i.e., LCOCD), our study provides novel insights into how microbial community structure could influence the microbial-mediated processes of engineering significance in drinking water production. Finally, our findings could offer the opportunity to improve biofilter performances via engineering interventions that shape the compositions of biofilter microbial communities and enhance their utilisation and removal of DOM, most notably the more classically humified and refractory DOM compound groups.


Asunto(s)
Agua Potable , Filtración , Purificación del Agua , Agua Potable/microbiología , Purificación del Agua/métodos , Compuestos Orgánicos , ARN Ribosómico 16S , Bacterias , Microbiología del Agua
8.
Environ Sci Technol ; 58(28): 12697-12707, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-38956762

RESUMEN

Transforming dissolved organic matter (DOM) is a crucial approach to alleviating the formation of disinfection byproducts (DBPs) in water treatment. Although catalytic ozonation effectively transforms DOM, increases in DBP formation potential are often observed due to the accumulation of aldehydes, ketones, and nitro compound intermediates during DOM transformation. In this study, we propose a novel strategy for the sequential oxidation of DOM, effectively reducing the levels of accumulation of these intermediates. This is achieved through the development of a catalyst with a tailored surface and nanoconfined active sites for catalytic ozonation. The catalyst features a unique confinement structure, wherein Mn-N4 moieties are uniformly anchored on the catalyst surface and within nanopores (5-20 Å). This design enables the degradation of the large molecular weight fraction of DOM on the catalyst surface, while the transformed smaller molecular weight fraction enters the nanopores and undergoes rapid degradation due to the confinement effect. The generation of *Oad as the dominant reactive species is essential for effectively reducing these ozone refractory intermediates. This resulted in over 70% removal of carbonaceous and nitrogenous DBP precursors as well as brominated DBP precursors. This study highlights the importance of the nanoscale sequential reactor design and provides new insights into eliminating DBP precursors by the catalytic ozonation process.


Asunto(s)
Desinfección , Ozono , Purificación del Agua , Ozono/química , Catálisis , Purificación del Agua/métodos , Contaminantes Químicos del Agua/química
9.
Environ Technol ; : 1-19, 2024 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-38940267

RESUMEN

In this study, we experimentally investigate the production and characterization of CaCO3 particles through the carbonation process of Ca(OH)2 and evaluate their potential application in removing organic matter. The CaCO3 particles were characterized using BET, SEM-EDX, FT-IR, particle size, and XRD techniques. Adsorption of organic matter was studied using synthetic solutions and samples from two surface water sources. Experiments were conducted at room temperature with adsorbent dosages ranging from 1.3 to 21.5 g/L, initial dissolved organic carbon concentrations between 2.5 and 20 mg/L (initial loading: 0.1-14.6 mgDOC/gCaCO3), and a contact time of at least 5 minutes. We observed a removal efficiency of 70-80% for DOC and 90-95% for UV254 at a low concentration of organic matter (humic acids, 2.5 mgDOC/L). At a concentration of 5.0 mg DOC/L, we achieved (i) 70-90% DOC removal for humic acid, (ii) 50-65% DOC removal for one surface water sample with SUVA254 of 2.4 L/mg·m, and (iii) 20-35% DOC removal for another surface water sample with SUVA254 of 4.3 L/mg·m. Furthermore, we investigated the performance of the prepared particles in repeated usage for organics removal. In conclusion, our findings propose areas for future research including optimizing particle cycling within the reaction environment, exploring particle utilization in reactors such as an up-flow particle bed, and assessing potential applications in a membrane contactor. The environmentally friendly and non-toxic nature of CaCO3 particles emphasizes their significance in future research and applications.

10.
Membranes (Basel) ; 14(6)2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38921492

RESUMEN

The removal of dissolved organic matter (DOM) from seawater before the reverse osmosis (RO) processes is crucial for alleviating organic fouling of RO membranes. However, research is still insufficiently developed in the comparison of the effectiveness of integrating coagulation with ultrafiltration (UF) or sand filtration (SF) in the pretreatment stage of seawater reverse osmosis (SWRO) for the removal of DOM. In this study, we investigated the effect of pretreatment technologies on RO fouling caused by DOM in seawater, including the integration of coagulation and sand filtration (C-S pretreatment) and the integration of coagulation and ultrafiltration (C-U pretreatment). Both integrated pretreatments achieved comparable DOM removal rates (70.2% for C-U and 69.6% for C-S), and C-S exhibited enhanced removal of UV-absorbing compounds. Although C-U was more proficient in reducing the silt density index (below 2) compared to C-S (above 3) and improved the elimination of humic acid-like organics, it left a higher proportion of tyrosine-protein-like organics, soluble microbial by-product-like organics, and finer organics in the effluent, leading to the formation of a dense cake layer on RO membrane and a higher flux decline. Therefore, suitable technologies should be selected according to specific water conditions to efficiently mitigate RO membrane fouling.

11.
J Environ Manage ; 363: 121387, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38850914

RESUMEN

The persistence of dissolved organic matter (DOM) plays a crucial role in the cycling and distribution of carbon and nutrients. Nonetheless, our understanding of how environmental alterations affect the persistence of sedimentary DOM remains incomplete. Excitation Emission Fluorescence Matrix-Parallel Factor Analysis (EEM-PARAFAC) was used to examine the fluorescence and compositional characteristics of hydrophilic and hydrophobic DOM (separated using XAD-8 resin) within sediments from twelve lakes and reservoirs. Fluorescence analysis indicated that DOM persistence is dependent on the proportions of the three components derived from PARAFAC. The Mantel test showed that climatic factors had the most significant impact on DOM persistence (Mantel's r = 0.46-0.54, Mantel's p = 0.001-0.007), while anthropogenic (Mantel's r = 0.24-0.32, Mantel's p = 0.03-0.05) and hydrological factors (Mantel's r = 0.03-0.22, Mantel's p = 0.06-0.40) had a somewhat lesser influence. Environmental changes resulted in a consistent decline in DOM persistence from Northeast to Southwest China, accompanied by an increase in gross primary productivity (GPP). Reduced DOM persistence due to climate, hydrological, and anthropogenic factors may lead to elevated concentrations of total phosphorus (TP), contributing to deteriorating water quality and events such as algal blooms. The decline in water quality due to reduced DOM persistence in lakes with high GPP can exacerbate the transition from carbon sinks to carbon sources. Consequently, the persistence of sedimentary DOM significantly influences nutrient and carbon cycling in lakes. Investigating DOM persistence in lakes across diverse geographic locations offers a new perspective on lake eutrophication and carbon emissions. Furthermore, it is crucial to develop targeted recommendations for lake restoration and management.


Asunto(s)
Ciclo del Carbono , Sedimentos Geológicos , Lagos , Sedimentos Geológicos/química , Sedimentos Geológicos/análisis , Lagos/química , Carbono/análisis , Fósforo/análisis , China , Monitoreo del Ambiente
12.
Sci Total Environ ; 943: 173776, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-38862046

RESUMEN

High­arsenic groundwater is influenced by a combination of processes: reductive dissolution of iron minerals and formation of secondary minerals, metal complexation and redox reactions of organic matter (OM), and formation of more migratory thioarsenate, which together can lead to significant increases in arsenic concentration in groundwater. This study was conducted in a typical sulfur- and arsenic-rich groundwater site within the Datong Basin to explore the conditions of thioarsenate formation and its influence on arsenic enrichment in groundwater using HPLC-ICPMS, hydrogeochemical modeling, and fluorescence spectroscopy. The shallow aquifer exhibited a highly reducing environment, marked by elevated sulfide levels, low concentrations of Fe(II), and the highest proportion of thioarsenate. In the middle aquifer, an optimal ∑S/∑As led to the presence of significant quantities of thioarsenate. In contrast, the deep aquifer exhibited low sulfide and high Fe(II) concentration, with arsenic primarily originating from dissolved iron minerals. Redox fluctuations in the sediment driven by sulfur­iron minerals generated reduced sulfur, thereby facilitating thioarsenate formation. OM played a crucial role as an electron donor for microbial activities, promoting iron and sulfate reduction processes and creating conditions conducive to thioarsenate formation in reduced and high­sulfur environments. Understanding the process of thioarsenate formation and the influencing factors is of paramount importance for comprehending the migration and redistribution of arsenic in groundwater systems.

13.
J Hazard Mater ; 472: 134565, 2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38743974

RESUMEN

Biochar shows great potential in soil cadmium pollution treatment, however, the effect and mechanisms of biochar on cadmium passivation (CP) during the long-term process of soil from flooding to natural air-drying are not clear. In this study, a 300-day experiment was conducted to keep the flooded water level constant for the first 100 days and then dried naturally. Mechanisms of CP by lignin biochar (LBC) were analyzed through chemical analysis, FTIR-2D-COS, EEMs-PARAFAC, ultraviolet spectroscopy characterizations, and microbial community distribution of soil. Results showed that application of LBC results in rapid CP ratio in soil within 35 days, mainly in the residual and Fe-Mn bound states (total 72.80%). CP ratio further increased to 90.89% with water evaporation. The CP mechanisms include precipitation, electrostatic effect, humus complexation, and microbial remediation by promoting the propagation of fungi such as Penicillium and Trichoderma. Evaporation of water promoted the colonization of aerobic microorganisms and then increased the degree of soil humification and aromatization, thereby enhancing the cadmium passivation. Simultaneously, the biochar could reduce the relative abundance of plant pathogens in soil from 1.8% to 0.03% and the freshness index (ß/α) from 0.64 to 0.16, favoring crop growth and promoting carbon sequestration and emission reduction.


Asunto(s)
Cadmio , Carbón Orgánico , Lignina , Microbiología del Suelo , Contaminantes del Suelo , Carbón Orgánico/química , Cadmio/química , Contaminantes del Suelo/química , Lignina/química , Inundaciones , Suelo/química , Desecación
14.
Water Res ; 258: 121806, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38796911

RESUMEN

This work investigates the validation and application of a competitive model approach for full-scale wastewater treatment plants (WWTP) with external recirculation of partially loaded powdered activated carbon (PAC) for removal of organic micropollutants (OMP). It is based on the ideal adsorbed solution theory (IAST) for multisolute mixtures combined with calibration of fictive organic components and correction of single-solute model parameters for OMP by use of the tracer model (TRM). Adsorption kinetics are represented by a pseudo first order reaction (PFO) and compared to mass transfer calculated with the homogenous surface diffusion model (HSDM). Model validation with operational data from two different WWTPs showed a strong dependency of model results on the batch sample quality used for model calibration. In contrast, the kinetic approach is of less importance for predicting full-scale OMP removal with long PAC sludge retention times. Further model application demonstrated that external PAC recirculation significantly improves the OMP removal with regard to both adsorption capacity and compensation of competitive effects of Dissolved Organic Carbon (DOC).


Asunto(s)
Carbón Orgánico , Eliminación de Residuos Líquidos , Aguas Residuales , Contaminantes Químicos del Agua , Adsorción , Contaminantes Químicos del Agua/química , Eliminación de Residuos Líquidos/métodos , Carbón Orgánico/química , Aguas Residuales/química , Purificación del Agua/métodos , Cinética , Modelos Teóricos , Carbono/química
15.
J Environ Sci (China) ; 144: 67-75, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38802239

RESUMEN

Freeze-induced acceleration of I- oxidation and the consequent iodination of dissolved organic matter (DOM) contribute to the formation of organoiodine compounds (OICs) in cold regions. The formed OICs may be a potentially important source of risk and are very closely with the environment and human health. Herein, we investigated the acceleration effects of the freeze process on I- oxidation and the formation of OICs. In comparison to reactive iodine species (RIS) formed in aqueous solutions, I- oxidation and RIS formation were greatly enhanced in frozen solution and were affected by pH, and the content of I- and O2. Freeze-thaw process further promoted I- oxidation and the concentration of RIS reached 45.7 µmol/L after 6 freeze-thaw cycles. The consequent products of DOM iodination were greatly promoted in terms of both concentration and number. The total content of OICs ranged from 0.02 to 2.83 µmol/L under various conditions. About 183-1197 OICs were detected by Fourier transform ion cyclotron resonance mass spectrometry, and more than 96.2% contained one or two iodine atoms. Most OICs had aromatic structures and were formed via substitution and addition reactions. Our findings reveal an important formation pathway for OICs and shed light on the biogeochemical cycling of iodine in the natural aquatic environment.


Asunto(s)
Congelación , Yoduros , Oxidación-Reducción , Contaminantes Químicos del Agua , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/análisis , Yoduros/química , Halogenación , Yodo/química
16.
J Hazard Mater ; 471: 134418, 2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38688225

RESUMEN

The emergence of mining projects for rare earth elements (REEs) in response to rising global demand and geopolitical factors introduces environmental concerns, such as the suspected release of anthropogenic REEs to aquatic systems and the coexistence of radionuclides (U, Th). Northern regions confront heightened challenges from limited research and accelerated climate change. Drivers of REEs in surface waters (including George and Koroc rivers, their tributaries, and thermokarst lakes) were studied (2017-2023) in subarctic Canada within a climate transition zone, near a prospective REE mine. Dissolved REEs (<0.45 µm) correlated positively with Al, Fe, Th, U, Cl- and DOC. A novel relationship with water temperature demonstrated an approximate 10-fold decrease in REE concentrations over the environmental gradient (2-20 ℃), suggesting complex implications for REE speciation under climate pressures. Optical analyses further predicted REEs were mobilized by humic-rich, terrestrial DOC, with correlations presenting a possible co-transport with Al, Fe and Th. Relationships for redox-sensitive Ce anomalies (Ce/Ce* = 0.18-1.2) with multi-valent trace metals (Al, Fe, Ti) and DOC were suggestive of a preferential adsorption of Ce by inorganic colloids in low-DOC systems. Findings emphasized the potential for changes in REE geochemistry with ongoing northern surface warming and vegetation shifts.

17.
Mar Pollut Bull ; 202: 116307, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38564820

RESUMEN

This study utilizes ultraviolet and fluorescence spectroscopic indices of dissolved organic matter (DOM) from sediments, combined with machine learning (ML) models, to develop an optimized predictive model for estimating sediment total organic carbon (TOC) and identifying adjacent land-use types in coastal sediments from the Yellow and Bohai Seas. Our results indicate that ML models surpass traditional regression techniques in estimating TOC and classifying land-use types. Penalized Least Squares Regression (PLR) and Cubist models show exceptional TOC estimation capabilities, with PLR exhibiting the lowest training error and Cubist achieving a correlation coefficient 0.79. In land-use classification, Support Vector Machines achieved 85.6 % accuracy in training and 92.2 % in testing. Maximum fluorescence intensity and ultraviolet absorbance at 254 nm were crucial factors influencing TOC variations in coastal sediments. This study underscores the efficacy of ML models utilizing DOM optical indices for near real-time estimation of marine sediment TOC and land-use classification.


Asunto(s)
Carbono , Monitoreo del Ambiente , Sedimentos Geológicos , Aprendizaje Automático , Sedimentos Geológicos/química , Carbono/análisis , Monitoreo del Ambiente/métodos
18.
Environ Sci Ecotechnol ; 21: 100392, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38434492

RESUMEN

Activated carbon is employed for the adsorption of organic micropollutants (OMPs) from water, typically present in concentrations ranging from ng L-1 to µg L-1. However, the efficacy of OMP removal is considerably deteriorated due to competitive adsorption from background dissolved organic matter (DOM), present at substantially higher concentrations in mg L-1. Interpreting the characteristics of competitive DOM is crucial in predicting OMP adsorption efficiencies across diverse natural waters. Molecular weight (MW), aromaticity, and polarity influence DOM competitiveness. Although the aromaticity-related metrics, such as UV254, of low MW DOM were proposed to correlate with DOM competitiveness, the method suffers from limitations in understanding the interplay of polarity and aromaticity in determining DOM competitiveness. Here, we elucidate the intricate influence of aromaticity and polarity in low MW DOM competition, spanning from a fraction level to a compound level, by employing direct sample injection liquid chromatography coupled with ultrahigh-resolution Fourier-transform ion cyclotron resonance mass spectrometry. Anion exchange resin pre-treatment eliminated 93% of UV254-active DOM, predominantly aromatic and polar DOM, and only minimally alleviated DOM competition. Molecular characterization revealed that nonpolar molecular formulas (constituting 26% PAC-adsorbable DOM) with medium aromaticity contributed more to the DOM competitiveness. Isomer-level analysis indicated that the competitiveness of highly aromatic LMW DOM compounds was strongly counterbalanced by increased polarity. Strong aromaticity-derived π-π interaction cannot facilitate the competitive adsorption of hydrophilic DOM compounds. Our results underscore the constraints of depending solely on aromaticity-based approaches as the exclusive interpretive measure for DOM competitiveness. In a broader context, this study demonstrates an effect-oriented DOM analysis, elucidating counterbalancing interactions of DOM molecular properties from fraction to compound level.

19.
Sci Total Environ ; 926: 171845, 2024 May 20.
Artículo en Inglés | MEDLINE | ID: mdl-38521269

RESUMEN

Biochar, which including pyrochar (PBC) and hydrochar (HBC), has been tested as a soil enhancer to improve saline soils. However, the effects of PBC and HBC application on ammonia (NH3) volatilization and dissolved organic matter (DOM) in saline paddy soils are poorly understood. In this research, marsh moss-derived PBC and HBC biochar types were applied to paddy saline soils at 0.5 % (w/w) and 1.5 % (w/w) rates to assess their impact on soil NH3 volatilization and DOM using a soil column experiment. The results revealed that soil NH3 volatilization significantly increased by 56.1 % in the treatment with 1.5 % (w/w) HBC compared to the control without PBC or HBC. Conversely, PBC and the lower application rate of HBC led to decrease in NH3 volatilization ranging from 2.4 % to 12.1 %. Floodwater EC is a dominant factor in NH3 emission. Furthermore, the fluorescence intensities of the four fractions (all humic substances) were found to be significantly higher in the 1.5 % (w/w) HBC treatment applied compared to the other treatments, as indicated by parallel factor analysis modeling. This study highlights the potential for soil NH3 losses and DOM leaching in saline paddy soils due to the high application rate of HBC. These findings offer valuable insights into the effects of PBC and HBC on rice paddy saline soil ecosystems.

20.
Water Res ; 255: 121534, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38555785

RESUMEN

Organics, as widespread pollutants in high-strength ammonia wastewater, typically exert adverse effects on the performance of partial nitrification-anammox (PNA) systems. However, the in-depth knowledge on how microbial consortia respond to these disturbances remains limited. In this study, we unveiled the evolution of complex organic matter flow and its impact on the metabolic hierarchy and adaptation of microbial consortia, employing multi-omics approaches, i.e., 16S amplicon sequencing, metagenomics, and metabolomics. In a two-stage PNA system sequentially treating synthetic wastewater and incineration leachate over 230 days, partial nitrification stayed stable (nitrite accumulation > 97%) while anammox efficiency dropped (nitrogen removal decreased from 86% to 78%). The phenomenon was revealed to be correlated with the evolution of dissolved organic matter (DOM) and xenobiotic organic compounds (XOCs). In the PN stage, ammonia-oxidizing bacteria (AOB) exhibited excellent adaptability through active metabolic regulation after treating leachate. Numerous heterotrophs proliferated to utilize DOM and XOCs, triggering a "boom" state evident in the glycerophospholipid metabolism. However, in the anammox stage, the competition between carbon fixation and central carbon metabolism within autotrophs and heterotrophs became evident. Increased biosynthesis costs inhibited the central metabolism (specific anammox activity decreased by 66%) and the Wood-Ljungdahl pathway of anammox bacteria (AnAOB) in the presence of recalcitrant organics. Additionally, the degradation of organics was limited, exhibiting a "bust" state. This study revealed the metabolic adaption and susceptibility of AOB and AnAOB in response to organics from the leachate, demonstrating the applicability of the two-stage configuration for treating high-strength wastewater containing abundant and diverse organics.

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