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1.
Water Res ; 264: 122130, 2024 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-39146847

RESUMEN

Nutrient pollution has become an important issue to solve in stormwater runoff due to the fast population growth and urbanization that impacts water quality and triggers harmful algal blooms. There is an acute need to link the dissolved organic nitrogen (DON) decomposition with the coupled nitrification and denitrification pathways to realize the pattern shifts in the nitrogen cycle. This paper presented a lab-scale cascade upflow biofiltration system for comparison of nitrate and phosphate removal from stormwater matrices through two specialty adsorbents at three influent conditions. The two specialty adsorbents are denoted as biochar iron and perlite integrated green environmental media (BIPGEM) and zero-valent iron and perlite-based green environmental media (ZIPGEM). An initial condition with stormwater runoff, a second condition with spiked nitrate, and a third condition with spiked nitrate and phosphate were used in this study. To differentiate nitrifier and denitrifier population dynamics associated with the decomposition of DON, integrative analysis of quantitative polymerase chain reaction (qPCR) and 21 tesla Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) were performed in association with nitrate removal efficiencies for both media with or without the presence of phosphate. While the qPCR may detect one gene for a single microbe or pathogen and realize the microbial population dynamics in the bioreactors, the 21 T FT-ICR MS can separate and assign elemental compositions to identify organic compounds of DON. Results indicated that ZIPGEM obtained a higher potential for nutrient removal than BIPGEM when the influent was spiked with nitrate and phosphate simultaneously. The sustainable, scalable, and adaptable upflow bioreactors operated in sequence (in a cascade mode) can be expanded flexibly on an as-needed basis to meet the local water quality standards showing process reliability, resilience, and sustainability simultaneously.


Asunto(s)
Filtración , Nitrógeno , Nitratos , Purificación del Agua/métodos , Desnitrificación , Contaminantes Químicos del Agua , Fosfatos
2.
Water Res ; 260: 121894, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38880013

RESUMEN

Algal blooms have become a significant challenge in water treatment all over the world. In chlorination of drinking water, algal organic matter (AOM) leads to the formation of organic chloramines. The objectives of this review are to comprehensively summarize and discuss the up-to-date researches on AOM-derived organic chloramines and their chemical activities and toxicity, thereby drawing attention to the potentially chemical and hygienic risks of organic chloramines. The predominant algal species in water sources varied with location and season. AOM from cyanobacteria, green algae, and diatoms are composed of diverse composition. AOM-derived amino acids take a low portion of the precursors of organic chloramines. Both experimental kinetic data and quantum chemical calculation demonstrate the preferential formation of organic chloramines in the chlorination of model compounds (amino acids and peptides). Organic chloramines are persistent in water and can transform into dichloro- and trichloro-organic chloramines, unknown low-molecular-weight organic chloramines, and nitrogenous disinfection byproducts with the excess of free chlorine. The active chlorine (Cl+) in organic chloramines can lead to the formation of chlorinated phenolic compounds. Organic chloramines influence the generation and species of radicals and subsequent products in UV disinfection. Theoretical predictions and toxicological tests suggest that organic chloramines may cause oxidative or toxic pressure to bacteria or cells. Overall, organic chloramines, as one group of high-molecular-weight disinfection byproducts, have relatively long lifetimes, moderate chemical activities, and high hygienic risks to the public. Future perspectives of organic chloramines are suggested in terms of quantitative detection methods, the precursors from various predominant algal species, chemical activities of organic chloramines, and toxicity/impact.


Asunto(s)
Cloraminas , Halogenación , Purificación del Agua , Cloraminas/química , Eutrofización , Desinfección , Cloro/química
3.
Water Res ; 260: 121924, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38896885

RESUMEN

Drinking water treatment plants (DWTPs) in China that pioneered the biological activated carbon (BAC) process have reached 10 years of operation. There has been a renewed focus on biofiltration and the performance of old BAC filters for dissolved organic nitrogen (DON) has been poor, requiring replacement and regeneration of the BAC. Therefore, it is necessary to explore a cost-effective way to improve the water quality of the old BAC filters. To address this, low frequency ultrasound is proposed to enhance DON removal efficiency by BAC. In this study, bench and pilot tests were conducted to investigate the effect of low frequency ultrasound on DON removal by 10-year BAC. The results indicated that low frequency ultrasound significantly improved the DON removal rate increased from 15.83 % to 85.87 % and considerably inhibited the nitrogenous disinfection by-products (N-DBPs) formation potential, which was attributed to a decrease in the production of lipid-like, carbohydrate-like, and protein/amino sugar-like DON. The biomass on the BAC was significantly reduced after ultrasound treatment, and it decreased from 349.56∼388.98 nmol P/gBAC to 310.12∼377.63 nmol P/gBAC, enabling the biofilm thickness to decrease and the surface to become sparse and porous, which was conducive to oxygen and nutrients transfer. The Rhizobials associated with microbe-derived DON were stripped away during ultrasound treatment, which reduced microbe-derived DON associated with amino acids. Additionally, ultrasound regulated metabolic pathways, including amino acids, tricarboxylic acid (TCA) cycle, and nucleotide metabolism, to improve the osmotic pressure of the biofilm. In short, low frequency ultrasound treatment can enhance BAC biological properties and effectively remove DON and N-DBPs formation potentials, which provides a viable and promising strategy for improving the safety of drinking water in practice.


Asunto(s)
Carbón Orgánico , Nitrógeno , Purificación del Agua , Purificación del Agua/métodos , Carbón Orgánico/química , Biopelículas , Filtración
4.
Chemosphere ; 357: 142042, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38621490

RESUMEN

The presence of dissolved organic nitrogen (DON) in stormwater treatment processes is a continuous challenge because of the intertwined nature of its decomposition, bioavailability, and biodegradability and its unclear molecular characteristics. In this paper, 21 T Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) in combination with quantitative polymerase chain reaction was applied to elucidate the molecular change of DON and microbial population dynamics in a field-scale water filtration system filled with two specialty adsorbents for comparison in South Florida where the dry and wet seasons are distinctive annually. The adsorbents included CPS (clay-perlite and sand sorption media) and ZIPGEM (zero-valent iron and perlite-based green environmental media). Our study revealed that seasonal effects can significantly influence the dynamic characteristics and biodegradability of DON. The microbial population density in the filter beds indicated that three microbial species in the nitrogen cycle were particularly thrived for denitrification, dissimilatory nitrate reduction to ammonium, and anaerobic ammonium oxidation via competition and commensalism relationships during the wet season. Also, there was a decrease in the compositional complexity and molecular weight of the DON groups (CnHmOpN1, CnHmOpN2, CnHmOpN3, and CnHmOpN4), revealed by the 21 T FT-ICR MS bioassay, driven by a microbial population quantified by polymerase chain reaction from the dry to the wet season. These findings indirectly corroborate the assumption that the metabolism of microorganisms is much more vigorous in the wet season. The results affirm that the sustainable materials (CPS and ZIPGEM) can sustain nitrogen removal intermittently by providing a suitable living environment in which the metabolism of microbial species can be cultivated and enhanced to facilitate physico-chemical nitrogen removal across the two types of green sorption media.


Asunto(s)
Filtración , Nitrógeno , Nitrógeno/metabolismo , Filtración/métodos , Contaminantes Químicos del Agua/metabolismo , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Biodegradación Ambiental , Desnitrificación , Adsorción , Microbiota , Florida , Óxido de Aluminio/química , Eliminación de Residuos Líquidos/métodos
5.
Water Res ; 255: 121488, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38513371

RESUMEN

Waste activated sludge (WAS) is a significant phosphorus (P) repository, and there is a growing interest in P recovery from WAS. Typically, the commercial technology for treating WAS involves thermal hydrolysis pretreatment (THP) coupled with anaerobic digestion (AD). However, there is ongoing debate regarding the transformation and distribution of P throughout this process. To address this, a long-term THP-AD process was operated in this study to comprehensively investigate P transformation and distribution. The results revealed that a substantial biodegradation of dissolved organic nitrogen (DON) raised the pH of the digestate to 8.3 during the AD process. This increased pH facilitated the dissolution of Al, leading to a reduction of 6.92 mg/L of NaOH-P. Simultaneously, sulfate reduction contributed to a decrease of 11.04 mg/L of Bipy-P in the solid. However, the reduction of Bipy-P and NaOH-P in the solid did not result in an improved P release to the supernatant. Conversely, a decrease of 23.60 mg/L P in the aqueous phase was observed after anaerobic digestion. The disappeared P was primarily precipitated with Mg and Ca, driven by the increased pH, and it contributed to the increase of HCl-P in the solid from 107.80 to 144.52 mg/L. These findings were further confirmed by results obtained from scanning electron microscopy (SEM), X-ray powder diffraction (XRD), and solid-state 31P nuclear magnetic resonance (NMR) spectroscopy. This study provides valuable insights into the mechanisms of P transformation during THP-AD process that is nearly opposite from conventional AD system.

6.
Sci Total Environ ; 925: 171749, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38494009

RESUMEN

Historically, dissolved organic nitrogen (DON) has not been characterized in the nitrogen profiles of most estuaries despite its significant contribution to total nitrogen and projected increase in loading. The characterization of dissolved inorganic nitrogen (DIN) and DON processing from groundwater to surface water also remains unconstrained. This study attempts to fill in these knowledge gaps by quantifying the DON pool and potential sources in a semiarid, low inflow estuary (Baffin Bay, Texas) using stable isotope techniques. High NO3- and DON concentrations, and high δ15N-NH4+ (+55.0 ± 56.7 ‰), δ15N-NO3- (+23.9 ± 8.6 ‰) and δ15N-DON (+22.3 ± 6.5 ‰) were observed in groundwaters of a septic-influenced estuarine area, indicating coupled septic contamination and nitrification/denitrification. In contrast, groundwater of an undeveloped area provided evidence of inundation by bay water through high NH4+ concentrations and δ15N-NH4+ (+8.4 ± 3.0 ‰) resembling estuary porewater. NH4+ was the dominant nitrogen species in porewater of both areas and δ15N-NH4+ indicated production via organic nitrogen mineralization and dissimilatory nitrate reduction to ammonium. Surface water had similar nitrogen profiles (DON constituted ∼98 % of dissolved nitrogen pool) and potential source contributions, despite distinct nitrogen processing and profiles found in each water table. This was attributed to low nitrogen removal rates and prolonged mixing associated with long residence time. This study emphasizes the importance of DON in a low-inflow estuary and the isotopic approach to comprehensively examine both inorganic and organic N processing and sources serving as a guide to investigate N cycling in high DON estuaries globally.

7.
Environ Sci Technol ; 58(10): 4648-4661, 2024 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-38324528

RESUMEN

With global eutrophication and increasingly stringent nitrogen discharge restrictions, dissolved organic nitrogen (DON) holds considerable potential to upgrade advanced wastewater denitrification because of its large contribution to low-nitrogen effluents and stronger stimulation effect for algae. Here, we show that DON from the postdenitrification systems dominates effluent eutrophication potential under different carbon sources. Methanol resulted in significantly lower DON concentrations (0.84 ± 0.03 mg/L) compared with the total nitrogen removal-preferred acetate (1.11 ± 0.02 mg/L) (p < 0.05, ANOVA). With our well-developed mathematical model (R2 = 0.867-0.958), produced DON instead of shared (persist in both influent and effluent) and/or removed DON was identified as the key component for effluent DON variation (Pearson r = 0.992, p < 0.01). The partial least-squares path modeling analysis showed that it is the microbial community (r = 0.947, p < 0.01) rather than the predicted metabolic functions (r = 0.040, p > 0.1) that affected produced DON. Carbon sources rebuild the microorganism-DON interaction by affecting the structure of microbial communities with different abilities to generate and recapture produced DON to finally regulate effluent DON. This study revalues the importance of carbon source selection and overturns the current rationality of pursuing only the total nitrogen removal efficiency by emphasizing DON.


Asunto(s)
Desnitrificación , Aguas Residuales , Materia Orgánica Disuelta , Carbono , Nitrógeno/análisis , Nitrógeno/química , Eliminación de Residuos Líquidos/métodos
8.
Sci Total Environ ; 917: 170489, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38301785

RESUMEN

Estuaries receive substantial amounts of terrestrial dissolved organic nitrogen (tDON), which will be transported from the freshwater to the oceanic terminus through vigorous exchange processes. However, the intricate migration and transformation dynamics of tDON during this transportation, particularly at a molecular level, remain constrained. To address this knowledge gap, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was used for the analysis of DON molecular composition in the Pearl River Estuary (PRE), a river-dominated estuarine system influenced by intensified anthropogenic activities in southern China. The results showed a pronounced spatial-temporal variation in DON concentration in the study area. At the molecular level, tDON exhibited reduced unsaturation and aromaticity, coupled with an elevated abundance of DON compounds containing one­nitrogen atom (1 N-DON, 53.17 %) and compounds containing carbon, hydrogen, oxygen, nitrogen, and sulfur (CHONS) (27.46 %). It was evident that lignin was depleted while more oxygenated tannin compounds were generated in the freshwater-seawater mixing zone. This transformation is attributed to heightened biological activities, likely influenced by the priming effect of terrestrial nutrient inputs. In summer, the prevailing plume combined with biological activities in the strong mixing area and outer estuary increased the abundance of 3 N-DON molecules and a concurrent rise in the abundance of DON compounds containing only carbon, hydrogen, oxygen, and nitrogen (CHON), DON compounds containing carbon, hydrogen, oxygen, nitrogen, sulfur, and phosphorus (CHONSP), and CHONS. This trend also underscores the expanding role of marine plankton and microbes in the utilization of DON compounds containing carbon, hydrogen, oxygen, nitrogen, and phosphorus (CHONP). These findings provide details of tDON transformation processes at the molecular level in a river-dominated estuary and underline the estuarine hydrodynamics involved in transporting and altering DON within the estuary.


Asunto(s)
Materia Orgánica Disuelta , Hidrodinámica , Nitrógeno/análisis , Ríos , Estuarios , Carbono/análisis , Oxígeno/análisis , Azufre/análisis , Hidrógeno/análisis , Fósforo/análisis
9.
Environ Sci Technol ; 58(6): 2870-2880, 2024 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-38181504

RESUMEN

Researchers and engineers are committed to finding effective approaches to reduce dissolved organic nitrogen (DON) to meet more stringent effluent total nitrogen limits and minimize effluent eutrophication potential. Here, we provided a promising approach by adding specific doses of 2-hydroxy-1,4-naphthoquinone (HNQ) to postdenitrification bioreactors. This approach of adding a small dosage of 0.03-0.1 mM HNQ effectively reduced the concentrations of DON in the effluent (ANOVA, p < 0.05) by up to 63% reduction of effluent DON with a dosing of 0.1 mM HNQ when compared to the control bioreactors. Notably, an algal bioassay indicated that DON played a dominant role in stimulating phytoplankton growth, thus effluent eutrophication potential in bioreactors using 0.1 mM HNQ dramatically decreased compared to that in control bioreactors. The microbe-DON correlation analysis showed that HNQ dosing modified the microbial community composition to both weaken the production and promote the uptake of labile DON, thus minimizing the effluent DON concentration. The toxic assessment demonstrated the ecological safety of the effluent from the bioreactors using the strategy of HNQ addition. Overall, HNQ is a promising redox mediator to reduce the effluent DON concentration with the purpose of meeting low effluent total nitrogen levels and remarkably minimizing effluent eutrophication effects.


Asunto(s)
Naftoquinonas , Eliminación de Residuos Líquidos , Aguas Residuales , Materia Orgánica Disuelta , Nitrógeno/análisis , Eutrofización
10.
J Environ Manage ; 352: 120099, 2024 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-38232598

RESUMEN

Reservoirs are vital to meet the ever-increasing demands for freshwater in a warming climate. Dissolved organic matter (DOM) represents an important pool of carbon and can be a major concern in drinking water sources. However, insights into DOM dynamics in temperate, semi-arid reservoirs remain limited. Therefore, we investigated the variations in DOM properties in Lake Diefenbaker, a large reservoir on the Canadian Prairies, by analyzing eight years of DOM concentrations and composition through linear mixed effect modeling. Contrary to expectations, reservoir dissolved organic carbon (DOC) concentration showed no correlation with inflow from the South Saskatchewan River (p = 0.12), while dissolved organic nitrogen (DON) increased with decreasing inflow (p = 0.002). DOM optical indices (SUVA254 and E4:E6 ratio) and DOC:DON ratio revealed a pronounced influence of inflow on reservoir DOM composition (p < 0.001), i.e., allochthonous characteristics increased with increasing flow, and autochthonous characteristics increased with declining flow. Travel time corrected comparison of approximately the same water parcel along the reservoir length revealed that increasing water residence time in downstream regions led to a significant transformation in DOM composition, favoring autochthonous characteristics (mean SUVA254 reduced by 0.52 L mg-C-1 m-1, and the E4:E6 and spectral slope ratio increased by 1.6 and 0.06, respectively). Autochthonous DOC inputs likely offset the allochthonous DOC losses, which resulted in a relatively stable DOC concentration throughout the reservoir (mean 3.7 mg L-1). Additionally, the effect of a large aquaculture operation on reservoir DOM properties was investigated, but no effect was detected. The results have significant implications for managing large river-reservoirs. Autochthonous DOM poses challenges to water processing, necessitating monitoring of DOM composition for reservoir drinking water quality. Insights on climate-induced changes in DOM properties will also assist with understanding changes to habitat conditions and contaminant transport.


Asunto(s)
Materia Orgánica Disuelta , Agua Potable , Monitoreo del Ambiente/métodos , Canadá , Lagos
11.
Water Res ; 249: 120942, 2024 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-38043348

RESUMEN

Estuaries are hotspots where terrestrially originated dissolved organic matter (DOM) is modified in molecular composition before entering marine environments. However, very few research has considered nitrogen (N) modifications of DOM molecules in estuaries, limiting our understanding of dissolved organic nitrogen (DON) cycling and the associated carbon cycling in estuaries. This study integrated optical, stable isotopes (δ15N and δ13C) and molecular composition (FT-ICR MS) to characterize the transformation of DOM in the Yangtze River Estuary. Both concentration of dissolved organic carbon (DOC) and DON decreased with increasing salinity, while their δ13C and δ15N increased with the increasing salinity. A significant positive correlation was found between δ15N and δ13C during the transportation of DOM to marginal seas, indicating that the behavior of both DOC and DON are primarily controlled by the mixing of freshwater and the seawater in the YRE. During the mixing process, the DON addition was observed using the conservative mixing curves. In the view of molecular composition, DOM molecules became more aromatic as the number of N atoms increased. Spearman correlations reveal that DOM molecules with fewer N atoms exhibited a higher enrichment in protein-like components, while those with more N atoms were more enriched in humic-like components. In addition, the δ15N and δ13C tended to increase as the N content of DOM decreased. Therefore, DON molecules with fewer N atoms were likely to be transformed into those with more N atoms based on the isotopic fractionation theory. This study establishes a linkage between the molecular composition and the δ15N of DOM, and discovers the N transformation pattern within DOM molecules during the transportation to marginal seas.


Asunto(s)
Materia Orgánica Disuelta , Nitrógeno , Isótopos de Nitrógeno/análisis , Océanos y Mares , Nitrógeno/análisis , Estuarios , Ríos/química
12.
Environ Pollut ; 341: 122906, 2024 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-37952919

RESUMEN

Dissolved organic nitrogen (DON) deposition was the substantial component of dissolved total nitrogen (DTN) deposition in the world's nitrogen deposition hot spots areas. However, the information on the importance for DON deposition and its sources was still scarce, which limited the comprehensive assessment of the ecological threat from nitrogen deposition. Six sampling sites around the Danjiangkou Reservoir were set up to collect the dry and wet deposition samples from October 2017 to September 2021. The results showed that dry and wet DTN deposition averaged 34.72 kg ha-1 yr-1 and 22.27 kg ha-1 yr-1, respectively. Dry NH4+-N, NO3--N and DON deposition averaged 14.28 kg ha-1 yr-1, 5.91 kg ha-1 yr-1 and 14.53 kg ha-1 yr-1, respectively. Wet NH4+-N, NO3--N and DON deposition averaged 11.14 kg ha-1 yr-1, 3.89 kg ha-1 yr-1and 7.24 kg ha-1 yr-1, respectively. The contributions of DON to DTN were 41.85% (in dry deposition) and 32.50% (in wet deposition), respectively. Dry DON deposition varied between 26.44 kg ha-1 yr-1 and 9.11 kg ha-1 yr-1, and significantly differed among six sampling sites (P < 0.05). The different intensity of agricultural activities disturbance at the sampling sites was the important reason for the spatial variations of DON deposition. DON deposition was significantly correlated with ammonium nitrogen (NH4+-N) deposition (P < 0.05). According to the results of positive matrix factorization (PMF) model, agriculture source contributed significantly to the DON deposition, the contributions at six sampling sites ranged from 45.8% to 73.7% in dry deposition, and from 56.8% to 81.6% in wet deposition. In summary, our findings found that agricultural activities were the important factors influencing the spatial patterns of DON deposition around Danjiangkou Reservoir and provided new evidence for the anthropogenic source of DON deposition in China.


Asunto(s)
Contaminantes Atmosféricos , Compuestos de Amonio , Nitrógeno/análisis , Contaminantes Atmosféricos/análisis , Agricultura , Compuestos de Amonio/análisis , China , Monitoreo del Ambiente/métodos
13.
Front Microbiol ; 14: 1273211, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-38156017

RESUMEN

Ammonia-oxidizing archaea (AOA) and bacteria (AOB), nitrite-oxidizing bacteria (NOB), and complete ammonia oxidizers (comammox) are responsible for nitrification in nature; however, some groups have been reported to utilize labile-dissolved organic nitrogen (LDON) for satisfying nitrogen demands. To understand the universality of their capacity of LDON metabolism, we collected 70 complete genomes of AOA, AOB, NOB, and comammox from typical environments for exploring their potentials in the metabolism of representative LDON (urea, polyamines, cyanate, taurine, glycine betaine, and methylamine). Genomic analyses showed that urea was the most popular LDON used by nitrifiers. Each group harbored unique urea transporter genes (AOA: dur3 and utp, AOB: utp, and NOB and comammox: urtABCDE and utp) accompanied by urease genes ureABC. The differentiation in the substrate affinity of these transporters implied the divergence of urea utilization efficiency in nitrifiers, potentially driving them into different niches. The cyanate transporter (cynABD and focA/nirC) and degradation (cynS) genes were detected mostly in NOB, indicating their preference for a wide range of nitrogen substrates to satisfy high nitrogen demands. The lack of genes involved in the metabolism of polyamines, taurine, glycine betaine, and methylamines in most of nitrifiers suggested that they were not able to serve as a source of ammonium, only if they were degraded or oxidized extracellularly as previously reported. The phylogenetic analyses assisted with comparisons of GC% and the Codon Adaptation Index between target genes and whole genomes of nitrifiers implied that urea metabolic genes dur3 and ureC in AOA evolved independently from bacteria during the transition from Thaumarchaeota to AOA, while utp in terrestrial AOA was acquired from bacteria via lateral gene transfer (LGT). Cyanate transporter genes cynS and focA/nirC detected only in a terrestrial AOA Candidadus Nitrsosphaera gargensis Ga9.2 could be gained synchronously with Nitrospira of NOB by an ancient LGT. Our results indicated that LDON utilization was a common feature in nitrifiers, but metabolic potentials were different among nitrifiers, possibly being intensely interacted with their niches, survival strategies, and evolutions.

14.
Proc Natl Acad Sci U S A ; 120(49): e2305763120, 2023 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-38015845

RESUMEN

Marine dissolved organic nitrogen (DON) is one of the planet's largest reservoirs of fixed N, which persists even in the N-limited oligotrophic surface ocean. The vast majority of the ocean's total DON reservoir is refractory (RDON), primarily composed of low molecular weight (LMW) compounds in the subsurface and deep sea. However, the composition of this major N pool, as well as the reasons for its accumulation and persistence, are not understood. Past characterization of the analytically more tractable, but quantitatively minor, high molecular weight (HMW) DON fraction revealed a functionally simple amide-dominated composition. While extensive work in the past two decades has revealed enormous complexity and structural diversity in LMW dissolved organic carbon, no efforts have specifically targeted LMW nitrogenous molecules. Here, we report the first coupled isotopic and solid-state NMR structural analysis of LMW DON isolated throughout the water column in two ocean basins. Together these results provide a first view into the composition, potential sources, and cycling of this dominant portion of marine DON. Our data indicate that RDON is dominated by 15N-depleted heterocyclic-N structures, entirely distinct from previously characterized HMW material. This fundamentally new view of marine DON composition suggests an important structural control for RDON accumulation and persistence in the ocean. The mechanisms of production, cycling, and removal of these heterocyclic-N-containing compounds now represents a central challenge in our understanding of the ocean's DON reservoir.

15.
Water Res ; 244: 120461, 2023 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-37639992

RESUMEN

Non-aeration microalgae-bacteria biofilm has attracted increasing interest for its application in low cost wastewater treatment. However, it is unclear the quantified biofilm characteristics dynamics and how biofilm bioactivity affects performance and nitrogen metabolisms during wastewater treatment. In this work, a push-flow microalgae-bacteria biofilm reactor (PF-MBBfR) was developed for aeration-free greywater treatment. Comparatively, organic loading at 1.27 ± 0.10 kg COD/(m3⋅d) gave the highest biofilm concentration, density, specific oxygen generation (SOGR) and consumption rates (SOCR), and pollutants removal rates. Contributed to low residual linear alkylbenzene sulfonates and bioactivity, reactor downstream showed low bacteria and protein concentrations and SOCR (12.8 mg O2/g TSS·h), but high microalgae, carbohydrate, biofilm density, SOGR (49.4 mg O2/g TSS·h) and pollutants removal rates. Dissolved organic nitrogen (DON) showed higher molecular weight, CHONS and fraction with 4 atoms of N in reactor upstream. Most of nitrogen was fixed to newly synthesized biomass during assimilation process by related functional enzymes, minor contributed to denitrification due to low N2 emission. High nitrogen assimilation by microalgae showed high SOGR, which favored efficient multiple pollutants removal and reduced DON emission. Our findings favor the practical application of PF-MBBfR based on biofilm bioactivity, enhancing efficiency and reducing DON emission for low- energy-input wastewater treatment.


Asunto(s)
Contaminantes Ambientales , Microalgas , Bacterias , Biopelículas , Nitrógeno , Oxígeno
16.
Sci Total Environ ; 904: 166291, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-37586508

RESUMEN

Karenia brevis blooms occur almost annually in southwest Florida, imposing significant ecological and human health impacts. Currently, 13 nutrient sources have been identified supporting blooms, including nearshore anthropogenic inputs such as stormwater and wastewater outflows. A 21-day bioassay was performed, where K. brevis cultures were inoculated with water sourced from three stormwater ponds along an age gradient (14, 18, and 34 yrs.) and one municipal wastewater effluent sample, with the aim of identifying biomolecular classes and transformations of dissolved organic matter (DOM) compounds used by K. brevis. All sample types supported K. brevis growth and showed compositional changes in their respective DOM pools. Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) catalogued the molecular composition of DOM and identified specific compound classes that were biodegraded. Results showed that K. brevis utilized species across a wide range of compositions that correspond to amino sugars, humic, and lignin-like biomolecular classes. The municipal wastewater and the youngest stormwater pond (SWP 14) effluent contained the largest pools of labile DOM compounds which were bioavailable to K. brevis, which indicates younger stormwater pond effluents may be as ecologically important as wastewater effluents to blooms. Conversely, generation of DOM compounds of greater complexity and a wide range of aromaticity was observed with the older (SWP 18 and SWP 34) stormwater pond treatments. These data confirm the potential for stormwater ponds and/or wastewater to contribute nutrients which can potentially support K. brevis blooms, revealing the need for improved nutrient retention strategies to protect coastal waters from the potential ill effects of urban effluent.


Asunto(s)
Dinoflagelados , Floraciones de Algas Nocivas , Humanos , Materia Orgánica Disuelta , Estanques/química , Aguas Residuales
17.
Water Res ; 244: 120446, 2023 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-37572459

RESUMEN

Marginal seas play a crucial role in the cycling of dissolved organic nitrogen (DON) between the terrestrial and marine environments. However, very few studies have considered the molecular transformation of DON in marginal seas, leaving the DON molecular modifications in its cycling largely unknown. Therefore, this study examined DON cycling in the Bohai Sea and Yellow Sea, two semi-closed marginal seas in northern China, using stable isotopes (δ15N and δ13C), optical characteristics, and molecular compositions. Compared to the Yellow Sea, the Bohai Sea had a weaker exchange with the open ocean, resulting in higher concentrations, lower δ15N, and more recalcitrant properties in DON. The DON cycling showed significant differences inside and outside the Yellow Sea Cold Water (YSCW). Degradation was the major sink of DON in the YSCW, during which more highly unsaturated compounds and carboxyl-rich alicyclic molecules were produced. Nitrogen atoms were found to be removed from the molecules with more N atoms to those with fewer ones during the DON degradation. This study discovered the molecular modifications in DON cycling and highlighted the intrinsic mechanisms in the cycling of DON in marginal seas.


Asunto(s)
Materia Orgánica Disuelta , Monitoreo del Ambiente , Océanos y Mares , Agua de Mar , Nitrógeno/análisis , Agua , China
18.
Chemosphere ; 337: 139384, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37414300

RESUMEN

With the recent focus on using advanced water treatment processes for water reuse, interest is growing for utilizing enhanced coagulation to remove dissolved chemical species. Up to 85% of the nitrogen in wastewater effluent is made up of dissolved organic nitrogen (DON), but there is a knowledge gap regarding its removal during coagulation, which can be influenced by DON characteristics. To address this issue, tertiary-treated wastewater samples were analyzed before and after coagulation with polyaluminum chloride and ferric chloride. Samples were size-fractionated into four molecular weight fractions (0.45 µm, 0.1 µm, 10 kDa, and 3 kDa) using vacuum filtration and ultrafiltration. Each fraction was further evaluated by coagulating it separately to assess DON removal during enhanced coagulation. The size fractionated samples were also separated into hydrophilic and hydrophobic fractions using C18 solid phase extraction disks. Fluorescence excitation-emission matrices were used to investigate the characteristics of dissolved organic matter contributing to DON during the coagulation process. The results showed that DON compounds of size <3 kDa constituted a majority of the total DON. Coagulation removed more than 80% DON from size fractions 0.45 µm-0.1 µm and 0.1 µm-10 kDa, but less than 20% was removed from 10 kDa to 3 kDa and <3 kDa fractions. Coagulation on pre-filtered samples removed 19% and 25% of the <3 kDa DON fraction using polyaluminum chloride and ferric chloride, respectively. In all molecular weight fractions, hydrophilic DON compounds were found to be dominant (>90%), and enhanced coagulation was not effective in removing hydrophilic DON compounds. LMW fractions respond poorly to enhanced coagulation due to their hydrophilic nature. Enhanced coagulation effectively removes humic acid-like substances, but poorly removes proteinaceous compounds such as tyrosine and tryptophan. This study's findings provide insights into DON behavior during coagulation and factors affecting its removal, potentially improving wastewater treatment strategies.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Aguas Residuales , Materia Orgánica Disuelta , Nitrógeno/análisis , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos
19.
Sci Total Environ ; 896: 165243, 2023 Oct 20.
Artículo en Inglés | MEDLINE | ID: mdl-37394069

RESUMEN

The study of nitrogen (N) transformation in urban ecosystems is crucial in the protection of coastal water bodies because excess N may fuel harmful algae blooms (HABs). The purpose of this investigation was to study and identify the forms and concentrations of N in rainfall, throughfall, and stormwater runoff for 4 storm events in a subtropical urban ecosystem and to use fluorescence spectroscopy to evaluate the optical properties and expected lability of dissolved organic matter (DOM) in the same samples. The rainfall contained both inorganic and organic N pools, and organic N as nearly 50 % of total dissolved N in the rainfall. As water moved through the urban water cycle, from rainfall to stormwater and from rainfall to throughfall, it was enriched in total dissolved N, with most of the enrichment coming from dissolved organic N. Throughfall fluxes of total dissolved N were as high as 0.67 kg ha-1, compared to 0.44 kg ha-1 from rainfall, suggesting that the urban tree canopy can facilitate anthropogenic subsidies of N to the urban water cycle. Through analysis of sample optical properties, we saw that the throughfall presented the highest humification index and the lowest biological index when compared to rainfall, suggesting throughfall likely consists of higher molecular weight compounds of greater recalcitrance. This study highlights the importance of the dissolved organic N fraction of urban rainfall, stormwater, and throughfall and shows how the chemical composition of dissolved organic nutrients can change as rainfall is transformed into throughfall in the urban tree canopy.

20.
Sci Total Environ ; 893: 164944, 2023 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-37336412

RESUMEN

This study evaluated the ability to remove dissolved organic matter (DOM), particularly dissolved organic nitrogen (DON), at a molecular level using Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) in a full-scale reject water treatment project comprising three steps of short-cut nitrification and denitrification, two-stage AO, and ultrafiltration membrane system. The results indicated that short-cut nitrification and denitrification were effective in reducing the DON concentration from an average of about 180 mg/L to 43 mg/L. The average molecular weight of DOM showed a decreasing trend from 238 Da to 160 Da. The percentage of nitrogen-containing organic compounds (CHON-DOM), which is the primary component of reject water DOM, increased from 65.79 % to 72.35 %, while the percentage of CHO-DOM decreased from 20.67 % to 15.24 %. The percentage of CHOS-DOM remained stable at 12.21 %-13.54 %. The percentage of protein-DOM decreased from 50.32 % to 18.40 %, while lignin-DOM increased from 36.16 % to 55.88 % and carbohydrate-DOM increased from 2.68 % to 9.74 %. The short-cut nitrification and denitrification and ultrafiltration membrane system both generated more unsaturated, highly aromatic DOM. This study provides insights into the effects of different wastewater treatment processes on the evolution of DOM/DON, which can be useful for effective DON control.

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