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1.
Sci Rep ; 14(1): 8493, 2024 04 11.
Artigo em Inglês | MEDLINE | ID: mdl-38605135

RESUMO

This study involved the production of 20 biochar samples derived from secondary medicinal residues of Snow Lotus Oral Liquid, processed within the temperature range of 200-600 °C. Additionally, four medicinal residues, including dissolved organic matter (DOM), from 24 samples obtained using the shaking method, served as the primary source material. The investigation focused on two key factors: the modifier and preparation temperature. These factors were examined to elucidate the spectral characteristics and chemical properties of the pharmaceutical residues, biochar, and DOM. To analyze the alterations in the spectral attributes of biochar and medicinal residues, we employed near-infrared spectroscopy (NIR) in conjunction with Fourier-infrared one-dimensional and two-dimensional correlation spectroscopy. These findings revealed that modifiers enhanced the aromaticity of biochar, and the influence of preparation temperature on biochar was diminished. This observation indicates the stability of the aromatic functional group structure. Comparative analysis indicated that Na2CO3 had a more pronounced structural effect on biochar, which is consistent with its adsorption properties. Furthermore, we utilized the fluorescence indices from UV-visible spectroscopy and excitation-emission-matrix spectra with the PARAFAC model to elucidate the characteristics of the fluorescence components in the DOM released from the samples. The results demonstrated that the DOM released from biochar primarily originated externally. Aromaticity reduction and increased decay will enhance the ability of the biochar to bind pollutants. Those results confirmed the link between the substantial increase in the adsorption performance of the high-temperature modified charcoal in the previous study and the structural changes in the biochar. We investigated the structural changes of biochar and derivative DOM in the presence of two perturbing factors, modifier and preparation temperature. Suitable modifiers were selected. Preparation for the study of adsorption properties of snow lotus medicinal residues.


Assuntos
Carvão Vegetal , Lotus , Carvão Vegetal/química , Matéria Orgânica Dissolvida , Temperatura , Espectrometria de Fluorescência/métodos , Substâncias Húmicas/análise
2.
Environ Sci Technol ; 58(14): 6204-6214, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38557085

RESUMO

Marine permeable sediments are important sites for organic matter turnover in the coastal ocean. However, little is known about their role in trapping dissolved organic matter (DOM). Here, we examined DOM abundance and molecular compositions (9804 formulas identified) in subtidal permeable sediments along a near- to offshore gradient in the German North Sea. With the salinity increasing from 30.1 to 34.6 PSU, the DOM composition in bottom water shifts from relatively higher abundances of aromatic compounds to more highly unsaturated compounds. In the bulk sediment, DOM leached by ultrapure water (UPW) from the solid phase is 54 ± 20 times more abundant than DOM in porewater, with higher H/C ratios and a more terrigenous signature. With 0.5 M HCl, the amount of leached DOM (enriched in aromatic and oxygen-rich compounds) is doubled compared to UPW, mainly due to the dissolution of poorly crystalline Fe phases (e.g., ferrihydrite and Fe monosulfides). This suggests that poorly crystalline Fe phases promote DOM retention in permeable sediments, preferentially terrigenous, and aromatic fractions. Given the intense filtration of seawater through the permeable sediments, we posit that Fe can serve as an important intermediate storage for terrigenous organic matter and potentially accelerate organic matter burial in the coastal ocean.


Assuntos
Matéria Orgânica Dissolvida , Ferro , Ferro/química , Água do Mar/química , Água , Compostos Orgânicos
3.
Proc Biol Sci ; 291(2020): 20240016, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38565157

RESUMO

An emerging consensus suggests that evolved intraspecific variation can be ecologically important. However, evidence that evolved trait variation within vertebrates can influence fundamental ecosystem-level processes remains sparse. In this study, we sought to assess the potential for evolved variation in the spotted salamander (Ambystoma maculatum) to affect aquatic ecosystem properties. Spotted salamanders exhibit a conspicuous polymorphism in the colour of jelly encasing their eggs-some females produce clear jelly, while others produce white jelly. Although the functional significance of jelly colour variation remains largely speculative, evidence for differences in fecundity and the morphology of larvae suggests that the colour morphs might differ in the strength or identity of ecological effects. Here, we assessed the potential for frequency variation in spotted salamander colour morphs to influence fundamental physiochemical and ecosystem properties-dissolved organic carbon, conductivity, acidity and primary production-with a mesocosm experiment. By manipulating colour morph frequency across a range of larval densities, we were able to demonstrate that larva density and colour morph variation were ecologically relevant: population density reduced dissolved organic carbon and increased primary production while mesocosms stocked with white morph larvae tended to have higher dissolved organic carbon and conductivity. Thus, while an adaptive significance of jelly coloration remains hypothetical, our results show that colour morphs differentially influence key ecosystem properties-dissolved organic carbon and conductivity.


Assuntos
Matéria Orgânica Dissolvida , Ecossistema , Animais , Feminino , Cor , Ambystoma , Larva
4.
J Environ Manage ; 357: 120715, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38579465

RESUMO

The effluents from conventional wastewater treatment plants (WWTP), even if accomplishing quality regulations, substantially differ in their characteristics with those of waters in natural environments. Constructed wetlands (CWs) serve as transitional ecosystems within WWTPs, mitigating these differences and restoring natural features before water is poured into the natural environment. Our study focused on an experimental surface-flow CW naturalizing the WWTP effluent in a semiarid area in Eastern Spain. Despite relatively low pollutant concentrations entering the CW, it effectively further reduced settled organic matter and nitrogen. Dissolved organic matter (DOM) reaching the CW was mainly protein-like, yet optical property changes in the DOM indicated increased humification, aromaticity, and stabilization as it flowed through the CW. Flow cytometry analysis revealed that the CW released less abundant but more active bacterial populations than those received. MiSeq Illumina sequencing highlighted changes in the prokaryotic community composition, with phyla Proteobacteria, Bacteroidetes, Firmicutes, and Actinobacteria dominating the CW outflow. Functional prediction tools (FaproTax and PICRUSt2) demonstrated a shift towards microbial guilds aligned with those of the natural aquatic environments, increased aerobic chemoheterotrophs, photoautotrophs, and metabolic reactions at higher redox potentials. Enhanced capabilities for degrading plant material correlated well with changes in the DOM pool. Our findings emphasize the role of CWs in releasing biochemically stable DOM and functionally suited microbial populations for natural receiving environments. Consequently, we propose CWs as a naturalization nature-based solution (NBS) in water-scarce regions like the Mediterranean, where reclaimed discharged water can significantly contribute to ecosystem's water resources compared to natural flows.


Assuntos
Águas Residuárias , Áreas Alagadas , Ecossistema , Cidadania , Bactérias , Matéria Orgânica Dissolvida , Região do Mediterrâneo , Eliminação de Resíduos Líquidos
5.
Sci Total Environ ; 926: 171857, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38521264

RESUMO

In aquatic ecosystems, dissolved organic matter (DOM) plays a vital role in microbial communities and the biogeochemical cycling of elements. However, little is known about the associations between DOM and microbial communities in lake sediments. This study investigated the composition of water-extractable organic matter and microbial communities in surface sediments of lakes with different salinities on the Qinghai-Tibet Plateau. Ultrahigh-resolution mass spectrometry and high-throughput microbial sequencing techniques were employed to assess the associations between molecular diversity and microbial diversity and the effects of salinity in 19 lakes spanning a salinity range from 0.22 ‰ to 341.87 ‰. Our results show that increasing salinity of lake water led to higher molecular diversity of DOM in surface sediments. High-salinity lakes exhibited distinct DOM characteristics, such as lower aromaticity, smaller molecular weight, and higher oxidation degree, compared to freshwater lakes. The complexity of the microbial network composition of sediments first increased and then decreased with the increase of salinity. Moreover, as salinity increases, the dominant species transitioned from Gammaproteobacteria to Bacteroidia, and this transition was accompanied by a decrease in microbial diversity and an increase in molecular diversity. Microbial factors accounted for 34.68 % of the variation in the molecular composition of DOM. Overall, this study emphasizes the significant effects of salinity on both molecular and microbial diversity in lake sediments. Furthermore, our findings underscore the importance of microbes in controlling the range of organic compounds present in lakes and deepen our knowledge of the biogeochemical cycling of DOM.


Assuntos
Lagos , Microbiota , Lagos/química , Tibet , Matéria Orgânica Dissolvida , Salinidade , Água
6.
Sci Total Environ ; 926: 171864, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38521274

RESUMO

The effect of dissolved organic matter (DOM) on bacterial regrowth in water after disinfection using ultraviolet (UV) light emitting diodes (UVLEDs) is still unclear. Herein, the regrowth and responses of Vibrio parahaemolyticus and Bacillus cereus were investigated after being exposed to UVLEDs at combined wavelengths (265 and 280 nm) in a phosphate-buffered saline consisting of Suwannee River natural organic matter (SRNOM) and Suwannee River fulvic acid (SRFA). Low-molecular-weight (MW) organic compounds, which may form into intermediary photoproducts, and indicate bacterial repair metabolism, were characterized through non-target screening using orbitrap mass spectrometry. This study demonstrates the ability of the UVLEDs-inactivated cells to regrow. After UV exposure, a considerable upregulation of RecA was observed in two strains. With increasing the incubation time, the expression levels of RecA in V. parahaemolyticus increased, which may be attributed to the dark repair mechanism. Coexisting anionic DOM affects both the disinfection and bacterial regrowth processes. The time required for bacterial regrowth after UV exposure reflects the time needed for the individual cells to reactivate, and it differs in the presence or absence of DOM. In the presence of DOM, the cells were less damaged and required less time to grow. The UVLEDs exposure results in the occurrence of low-MW organic compounds, including carnitine or acryl-carnitine with N-acetylmuramic acid, which are associated with bacterial repair metabolism. Overall, the results of this study expand the understanding of the effects of water matrices on bacterial health risks. This can aid in the development of more effective strategies for water disinfection.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Desinfecção , Matéria Orgânica Dissolvida , Água , Rios , Purificação da Água/métodos , Compostos Orgânicos , Bactérias , Carnitina , Poluentes Químicos da Água/química
7.
Sci Total Environ ; 926: 171943, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38527546

RESUMO

Monoculture plantations in China, characterized by the continuous cultivation of a single species, pose challenges to timber accumulation and understory biodiversity, raising concerns about sustainability. This study investigated the impact of continuous monoculture plantings of Chinese fir (Cunninghamia lanceolata [Lamb.] Hook.) on soil properties, dissolved organic matter (DOM), and microorganisms over multiple generations. Soil samples from first to fourth-generation plantations were analyzed for basic chemical properties, DOM composition using Fourier transform ion cyclotron resonance mass spectrometry, and microorganisms via high-throughput sequencing. Results revealed a significant decline in nitrate nitrogen content with successive rotations, accompanied by an increase in easily degradable compounds like carbohydrates, aliphatic/proteins, tannins, Carbon, Hydrogen, Oxygen and Nitrogen- (CHON) and Carbon, Hydrogen, Oxygen and Sulfur- (CHOS) containing compounds. However, the recalcitrant compounds, such as lignin and carboxyl-rich alicyclic molecules (CRAMs), condensed aromatics and Carbon, Hydrogen and Oxygen- (CHO) containing compounds decreased. Microorganism diversity, abundance, and structure decreased with successive plantations, affecting the ecological niche breadth of fungal communities. Bacterial communities were strongly influenced by DOM composition, particularly lignin/CRAMs and tannins. Continuous monoculture led to reduced soil nitrate, lignin/CRAMs, and compromised soil quality, altering chemical properties and DOM composition, influencing microbial community assembly. This shift increased easily degraded DOM, accelerating soil carbon and nitrogen cycling, ultimately reducing soil carbon sequestration. From environmental point of view, the study emphasizes the importance of sustainable soil management practices in continuous monoculture systems. Particularly the findings offer valuable insights for addressing challenges associated with monoculture plantations and promoting long-term ecological sustainability.


Assuntos
Cunninghamia , Microbiota , Matéria Orgânica Dissolvida , Nitratos/análise , Lignina/metabolismo , Taninos/análise , Taninos/metabolismo , Solo/química , Compostos Orgânicos/análise , Compostos de Enxofre/metabolismo , Nitrogênio/análise , Carbono/análise , Hidrogênio/análise , Oxigênio/análise
8.
Sci Total Environ ; 926: 171962, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38537819

RESUMO

Estuaries are important components of the global carbon cycle; exchanging carbon between aquatic, atmospheric, and terrestrial environments, representing important loci for blue carbon storage and greenhouse gas emissions. However, how estuarine gradients affect sinking/suspended particles, and dissolved organic matter dynamic interactions remains unexplored. We fractionated suspended/sinking particles to assess and characterise carbon fate differences. We investigated bacterial colonisation (SYBR Green I) and exopolymer concentrations (TEP/CSP) with microscopy staining techniques. C/H/N and dry weight analysis identified particle composition differences. Meanwhile, nutrient and carbon analysis, and excitation and emission matrix evaluations with a subsequent parallel factor (PARAFAC) analysis characterised dissolved organic matter. The lack of clear salinity driven patterns in our study are presumably due to strong mixing forces and high particle heterogeneity along the estuary, with only density differences between suspended and sinking particles. Elbe estuary particles' organic portion is made up of marine-like (sinking) and terrestrial-like (suspended) signatures. Salinity did not have a significant role in microbial degradation and carbon composition, although brackish estuary portions were more biologically active. Indicative of increased degradation rates, leading to decreased greenhouse gas emissions, which are especially relevant for estuaries, with their disproportionate greenhouse gas emissions. Bacterial colonisation decreased seawards, indicative of decreased degradation, and shifts in microbial community composition and functions. Our findings span diverse strands of research, concerning steady carbon contributions from both marine and terrestrial sources, carbon aromaticity, humification index, and bioavailability. Their integration highlights the importance of the Elbe estuary as a model system, providing robust information for future policy decisions affecting dissolved and particulate matter dynamics within the Elbe Estuary.


Assuntos
Carbono , Gases de Efeito Estufa , Carbono/análise , Matéria Orgânica Dissolvida , Gases de Efeito Estufa/análise , Estuários , Material Particulado/análise , Rios
9.
Sci Total Environ ; 926: 172086, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38556025

RESUMO

Dissolved organic matter (DOM) in rainfall participates in many biogeochemical cycles in aquatic environments and affects biological activities in water bodies. Revealing the characteristics of rainfall DOM could broaden our understanding of the carbon cycle. Therefore, the distribution characteristics and response mechanisms of DOM to microorganisms were investigated in different regions of Hebei. The results indicated that the water quality of the northern region was worse than that of the middle and southern regions. The two protein like components (C1, C2) and one humic like component (C3) were obtained; at high molecular weight (MW), the fluorescence intensity is high in the northern region (0.03 ± 0.02 R.U.), while at low MW, the fluorescence intensity is highest in the southern region (0.50 ± 0.18 R.U.). Furthermore, C2 is significantly positively correlated with C1 (P < 0.01), while C2 is significantly negatively correlated with C3 (P < 0.05) was observed. The spectral index results indicated that rainfall DOM exhibited low humification and highly autochthonous characteristics. The southern region obtained higher richness and diversity of microbial species than northern region (P < 0.05). The community exhibits significant spatiotemporal differences, and the Acinetobacter, Enterobacter, and Massilia, were dominant genus. Redundancy and network analyses showed that the effects of C1, C2, and nitrate on microorganisms increased with decreasing MW, while low MW exhibited a more complex network between DOM and microorganisms than high MW. Meanwhile, C1, C2 had a large total effect on ß-diversity and function through structural equation modeling. The backward trajectory model indicates that the sources of air masses are from the northwest, local area, and sea in the northern, middle, and southern regions, respectively. This study broadened the understanding of the composition of summer rainfall DOM and its interactions with microorganisms during rainfall.


Assuntos
Matéria Orgânica Dissolvida , Rios , Rios/química , Espectrometria de Fluorescência , Qualidade da Água , Compostos Orgânicos/análise , Substâncias Húmicas/análise
10.
Chemosphere ; 355: 141782, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38548083

RESUMO

While anthropogenic pollution is a major threat to aquatic ecosystem health, our knowledge of the presence of xenobiotics in coastal Dissolved Organic Matter (DOM) is still relatively poor. This is especially true for water bodies in the Global South with limited information gained mostly from targeted studies that rely on comparison with authentic standards. In recent years, non-targeted tandem mass spectrometry has emerged as a powerful tool to collectively detect and identify pollutants and biogenic DOM components in the environment, but this approach has yet to be widely utilized for monitoring ecologically important aquatic systems. In this study we compared the DOM composition of Algoa Bay, Eastern Cape, South Africa, and its two estuaries. The Swartkops Estuary is highly urbanized and severely impacted by anthropogenic pollution, while the Sundays Estuary is impacted by commercial agriculture in its catchment. We employed solid-phase extraction followed by liquid chromatography tandem mass spectrometry to annotate more than 200 pharmaceuticals, pesticides, urban xenobiotics, and natural products based on spectral matching. The identification with authentic standards confirmed the presence of methamphetamine, carbamazepine, sulfamethoxazole, N-acetylsulfamethoxazole, imazapyr, caffeine and hexa(methoxymethyl)melamine, and allowed semi-quantitative estimations for annotated xenobiotics. The Swartkops Estuary DOM composition was strongly impacted by features annotated as urban pollutants including pharmaceuticals such as melamines and antiretrovirals. By contrast, the Sundays Estuary exhibited significant enrichment of molecules annotated as agrochemicals widely used in the citrus farming industry, with predicted concentrations for some of them exceeding predicted no-effect concentrations. This study provides new insight into anthropogenic impact on the Algoa Bay system and demonstrates the utility of non-targeted tandem mass spectrometry as a sensitive tool for assessing the health of ecologically important coastal ecosystems and will serve as a valuable foundation for strategizing long-term monitoring efforts.


Assuntos
Matéria Orgânica Dissolvida , Poluentes Ambientais , Ecossistema , Estuários , Baías , Rios/química , Agricultura , Preparações Farmacêuticas
11.
Chemosphere ; 355: 141826, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38552805

RESUMO

Recent studies have increasingly focused on the occurrence of plastic leachate and its impacts on aquatic ecosystems. Nonetheless, the environmental fate of this leachate in the presence of abundant natural organic matter (NOM)-a typical scenario in environments contaminated with plastics-remains underexplored. This study investigates the photo-induced leaching behaviors of dissolved organic matter (DOM) from terrestrial-sourced particles (forest soil and leaf litter) and microplastics (MPs), specifically polystyrene (PS) and polyvinyl chloride (PVC), over a two-week period. We also examined the biodegradability and spectroscopic characteristics of the leached DOM from both sources. Our results reveal that DOM from microplastics (MP-DOM) demonstrates more persistent leaching behavior compared to terrestrial-derived DOM, even with lesser quantities per unit of organic carbon. UV irradiation was found to enhance DOM leaching across all particle types. However, the photo-induced leaching behaviors of fluorescent components varied with the particle type. The MP group exhibited a broader range and higher biodegradability (ranging from 19.7% to 61.6%) compared to the terrestrial-sourced particles (ranging from 3.7% to 16.5%). DOM leached under UV irradiation consistently showed higher biodegradability than that under dark conditions. Furthermore, several fluorescence characteristics of DOM, such as the protein/phenol-like component (%C2), terrestrial humic-like component (%C3), and humification index (HIX)-traditionally used to indicate the biodegradability of natural organic matter-were also effective in assessing MP-DOM (with correlation coefficients R2 = 0.6055 (p = 0.003), R2 = 0.5389 (p = 0.007), and R2 = 0.4640 (p = 0.015), respectively). This study provides new insights into the potential differences in environmental fate between MP-DOM and NOM in aquatic environments heavily contaminated with MPs.


Assuntos
Microplásticos , Plásticos , Matéria Orgânica Dissolvida , Ecossistema , Solo/química , Substâncias Húmicas/análise , Espectrometria de Fluorescência/métodos
12.
Environ Sci Technol ; 58(13): 5856-5865, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38516968

RESUMO

Measuring the quantum yield and reactivity of triplet-state dissolved organic matter (3DOM*) is essential for assessing the impact of DOM on aquatic photochemical processes. However, current 3DOM* quantification methods require multiple fitting steps and rely on steady-state approximations under stringent application criteria, which may introduce certain inaccuracies in the estimation of DOM photoreactivity parameters. Here, we developed a global kinetic model to simulate the reaction kinetics of the hv/DOM system using four DOM types and 2,4,6-trimethylphenol as the probe for 3DOM*. Analyses of residuals and the root-mean-square error validated the exceptional precision of the new model compared to conventional methods. 3DOM* in the global kinetic model consistently displayed a lower quantum yield and higher reactivity than those in local regression models, indicating that the generation and reactivity of 3DOM* have often been overestimated and underestimated, respectively. The global kinetic model derives parameters by simultaneously fitting probe degradation kinetics under different conditions and considers the temporally increasing concentrations of the involved reactive species. It minimizes error propagation and offers insights into the interactions of different species, thereby providing advantages in accuracy, robustness, and interpretability. This study significantly advances the understanding of 3DOM* behavior and provides a valuable kinetic model for aquatic photochemistry research.


Assuntos
Matéria Orgânica Dissolvida , Processos Fotoquímicos , Fotoquímica , Fotólise
13.
Sci Total Environ ; 925: 171745, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38508257

RESUMO

Forests are significant carbon reservoirs, with approximately one-third of this carbon stored in the soil. Forest thinning, a prevalent management technique, is designed to enhance timber production, preserve biodiversity, and maintain ecosystem functions. Through its influence on biotic and abiotic factors, thinning can profoundly alter soil carbon storage. Yet, the full implications of thinning on forest soil carbon reservoirs and the mechanisms underpinning these changes remain elusive. In this study, we undertook a two-year monitoring initiative, tracking changes in soil extracellular enzyme activities (EEAs), microbial communities, and other abiotic parameters across four thinning intensities within a temperate pine forest. Our results show a marked increase in soil carbon stock following thinning. However, thinning also led to decreased dissolved organic carbon (DOC) content and a reduced DOC to soil organic carbon (SOC) ratio, pointing toward a decline in soil carbon lability. Additionally, fourier transform infrared spectroscopy (FTIR) analysis revealed an augmented relative abundance of aromatic compounds after thinning. There was also a pronounced increase in absolute EEAs (per gram of dry soil) post-thinning, implying nutrient limitations for soil microbes. Concurrently, the composition of bacterial and fungal communities shifted toward oligotrophic dominance post thinning. Specific EEAs (per gram of soil organic matter) exhibit a significant reduction following thinning, indicating a deceleration in organic matter decomposition rates. In essence, our findings reveal that thinning transitions soil toward an oligotrophic state, dampening organic matter decomposition, and thus bolstering the soil carbon storage potential of forest. This study provides enhanced insights into the nuanced relationship between thinning practices and forest soil carbon dynamics, serving as a robust foundation for enlightened forest management strategies.


Assuntos
Microbiota , Solo , Solo/química , Carbono , Florestas , Compostos Orgânicos , Microbiologia do Solo , Matéria Orgânica Dissolvida
15.
Environ Sci Technol ; 58(10): 4637-4647, 2024 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-38427796

RESUMO

Marine dissolved organic matter (DOM) is an important component of the global carbon cycle, yet its intricate composition and the sea salt matrix pose major challenges for chemical analysis. We introduce a direct injection, reversed-phase liquid chromatography ultrahigh resolution mass spectrometry approach to analyze marine DOM without the need for solid-phase extraction. Effective separation of salt and DOM is achieved with a large chromatographic column and an extended isocratic aqueous step. Postcolumn dilution of the sample flow with buffer-free solvents and implementing a counter gradient reduced salt buildup in the ion source and resulted in excellent repeatability. With this method, over 5,500 unique molecular formulas were detected from just 5.5 nmol carbon in 100 µL of filtered Arctic Ocean seawater. We observed a highly linear detector response for variable sample carbon concentrations and a high robustness against the salt matrix. Compared to solid-phase extracted DOM, our direct injection method demonstrated superior sensitivity for heteroatom-containing DOM. The direct analysis of seawater offers fast and simple sample preparation and avoids fractionation introduced by extraction. The method facilitates studies in environments, where only minimal sample volume is available e.g. in marine sediment pore water, ice cores, or permafrost soil solution. The small volume requirement also supports higher spatial (e.g., in soils) or temporal sample resolution (e.g., in culture experiments). Chromatographic separation adds further chemical information to molecular formulas, enhancing our understanding of marine biogeochemistry, chemodiversity, and ecological processes.


Assuntos
Matéria Orgânica Dissolvida , Água , Espectrometria de Massas/métodos , Água/química , Água Doce/química , Cloreto de Sódio , Carbono
16.
Huan Jing Ke Xue ; 45(3): 1539-1552, 2024 Mar 08.
Artigo em Chinês | MEDLINE | ID: mdl-38471868

RESUMO

The global occurrences of lake eutrophication have led to algal bloom and the subsequent algal decomposition, releasing high amounts of algae-derived dissolved organic matter (DOM) into the lake water. Algae-derived DOM could regulate the quantity and composition of DOM in lake water and further impact the biogeochemical cycles of multiple elements. In this study, the dynamic changes in the quantity and quality of DOM during algal decomposition under different eutrophic scenarios (e.g., from oligotrophication to severe eutrophication) were monitored, and the corresponding environmental effects (e.g., microbial responses and greenhouse gas emissions) caused by algal decomposition were further explored. The results showed that algal decomposition significantly increased the DOM levels, bioavailability, and intensities of fluorescent components in the water. The total DOM levels gradually decreased, whereas the average molecular weight increased along the decomposition process. Furthermore, unsaturated hydrocarbon and aliphatic compounds were preferentially utilized by microorganisms during algal decomposition, and some refractory molecules (e.g., lignin, condensed hydrocarbons, and tannin with high O/C values) were synchronously generated, as evidenced by the results from ultra-high-resolution mass spectrometry. The dominant bacterial species during algal decomposition shifted from Proteobacteria (46%) to Bacteroidetes (42%). In addition, algae addition resulted in 1.2-5 times the emissions of CO2 and CH4 from water, and the emission rates could be well predicted by the optical index of a254 in water. This study provides comprehensive perspectives for understanding the environmental behaviors of aquatic DOM and further paves the ways for the mitigation of lake eutrophication.


Assuntos
Matéria Orgânica Dissolvida , Lagos , Lagos/química , Espectrometria de Massas , Bactérias , Água/análise , Eutrofização , China
17.
Environ Pollut ; 346: 123657, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38428787

RESUMO

Straw amendment significantly enhances mercury (Hg) methylation and subsequent methylmercury (MeHg) bioaccumulation in Hg-contaminated paddy fields by releasing dissolved organic matter (DOM). This study comprehensively investigates the regulatory mechanisms of DOM and its different molecular weights derived from sulfur-rich rape straw (RaDOM) and composted rape straw (CRaDOM) applied in the rice-filling stage on soil MeHg production and subsequent bioaccumulation in rice grains. The results indicated that the amendment of RaDOM and CRaDOM significantly reduced soil MeHg content by 42.40-62.42%. This reduction can be attributed to several factors, including the suppression of Hg-methylating bacteria in soil, the supply of sulfate from RaDOM and CRaDOM, and the increase in the humification, molecular weight, and humic-like fractions of soil DOM. Additionally, adding RaDOM increased the MeHg bioaccumulation factor in roots by 27.55% while inhibiting MeHg transportation by 12.24% and ultimately reducing MeHg content in grains by 21.24% compared to the control group. Similarly, CRaDOM enhanced MeHg accumulation by 25.19%, suppressed MeHg transportation by 39.65%, and reduced MeHg levels in the grains by 27.94%. The assimilation of sulfate derived from RaDOM and CRaDOM into glutathione may be responsible for the increased retention of MeHg in the roots. Over the three days, there was a significant decrease in soil MeHg content as the molecular weight of RaDOM increased; conversely, altering the molecular weight of CRaDOM demonstrated an inverse trend. However, this pattern was not observed after 12 days. Applying sulfur-rich rape DOM can help mitigate MeHg accumulation in paddy fields by regulating the quality of soil DOM, sulfur cycling, and Hg-methylating bacteria.


Assuntos
Brassica rapa , Mercúrio , Compostos de Metilmercúrio , Oryza , Poluentes do Solo , Mercúrio/análise , Solo , Matéria Orgânica Dissolvida , Poluentes do Solo/análise , Sulfatos , Metilação
18.
Ecotoxicol Environ Saf ; 274: 116237, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38503104

RESUMO

Dissolved organic matter (DOM) is a crucial component of natural sediments that alters Cd sequestration. Nevertheless, how different types of DOM fuel Cd mobilization in Mn-rich sediments has not been elucidated. In the present study, four typical DOM, fluvic acid (FA), bovine serum albumin (BSA), sodium alginate (SA), and sodium dodecyl benzene sulfonate (SDBS), were used to amend Cd-contaminated sediment to study their effects on Cd/Mn biotransformation and microbial community response. The results demonstrated that different DOM drive microbial community shifts and enhance microbially mediated Mn oxide (MnO) reduction and Cd release. The amendment of terrestrial- and anthropogenic-derived DOM (FA and SDBS) mainly contributed to enriching Mn-reducing bacteria phylum Proteobacteria, and its abundance increased by 38.16-74.47 % and 56.41-73.98 %, respectively. Meanwhile, microbial-derived DOM (BSA and SA) mainly stimulated the abundances of metal(loid)-resistant bacteria phylum Firmicutes. Accompanied by microbial community structure, diversity, and co-occurrence network shifts, the DOM concentration and oxidation-reduction potential changed, resulting in enhanced Cd mobilization. Importantly, FA stimulated Cd release most remarkably, probably because of the decreased cooperative interactions between bacterial populations, stronger reduction of MnOs, and higher aromaticity and hydrophobicity of the sediment DOM after amendment. This study linked DOM types to functional microbial communities, and explored the potential roles of different DOM types in Cd biotransformation in lake sediments.


Assuntos
Cádmio , Manganês , Cádmio/metabolismo , Manganês/metabolismo , Matéria Orgânica Dissolvida , Bactérias/metabolismo , Firmicutes
19.
Nat Commun ; 15(1): 2640, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38531850

RESUMO

Climate change induced shifts in treeline position, both towards higher altitudes and latitudes induce changes in soil organic matter. Eventually, soil organic matter is transported to alpine and subarctic lakes with yet unknown consequences for dissolved organic matter (DOM) diversity and processing. Here, we experimentally investigate the consequences of treeline shifts by amending subarctic and temperate alpine lake water with soil-derived DOM from above and below the treeline. We use ultra-high resolution mass spectrometry (FT-ICR MS) to track molecular DOM diversity (i.e., chemodiversity), estimate DOM decay and measure bacterial growth efficiency. In both lakes, soil-derived DOM from below the treeline increases lake DOM chemodiversity mainly through the enrichment with polyphenolic and highly unsaturated compounds. These compositional changes are associated with reductions in bulk and compound-level DOM reactivity and reduced bacterial growth efficiency. Our results suggest that treeline advancement has the potential to enrich a large number of lake ecosystems with less biodegradable DOM, affecting bacterial community function and potentially altering the biogeochemical cycling of carbon in lakes at high latitudes and altitudes.


Assuntos
Matéria Orgânica Dissolvida , Lagos , Lagos/química , Ecossistema , Altitude , Solo/química
20.
Environ Int ; 185: 108518, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38430584

RESUMO

Dissolved organic matter (DOM) constitutes the most active fraction in global carbon pools, with estuarine sediments serving as significant repositories, where DOM is susceptible to dynamic transformations. Anthropogenic nitrogen (N) and sulfur (S) inputs further complicate DOM by creating N-bearing DOM (DON) and S-bearing DOM (DOS). This study delves into the spatial gradients and transformation mechanisms of DOM, DON, and DOS in Pearl River Estuary (PRE) sediments, China, using combined techniques of UV-visible spectroscopy, Excitation-emission matrix (EEM) fluorescence spectroscopy, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), and microbial high-throughput sequencing. Results uncovered a distinct spatial gradient in DOM concentration, aromaticity (SUVA254), hydrophobicity (SUVA260), the content of substituent groups including carboxyl, carbonyl, hydroxyl and ester groups (A253/A203) of chromophoric DOM (CDOM), and the abundances of tyrosine/tryptophan-like protein and humic-like substances in fluorophoric DOM (FDOM). These all decreased from upper to lower PRE, accompanied by a decrease in O3S and O5S components, indicating seaward reduction in the contribution of terrestrial OM, especially anthropogenic inputs. Additionally, sediments exhibited a reduction in molecular diversity (number of formulas) of DOM, DON, and DOS from upper to lower PRE, with molecules tending towards a lower nominal oxidation state of carbon (NOSC) and higher bio-reactivity (MLBL), molecular weight (m/z) and saturation (H/C). While molecular composition of DOM remained similar in PRE sediments, the relative abundance of lignin-like substances decreased, with a concurrent increase in protein-like and lipid-like substances in DON and DOS from upper to lower PRE. Mechanistic analysis identified the joint influence of terrestrial OM, anthropogenic N/S inputs, and microbial processes in shaping the spatial gradients of DOM, DON, and DOS in PRE estuarine sediments. This study contributes valuable insights into the intricate spatial gradients and transformations of DOM, DON, and DOS within human-impacted estuarine sediments.


Assuntos
Matéria Orgânica Dissolvida , Rios , Humanos , Rios/química , Espectrometria de Massas , Estuários , Carbono
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