Migration and transformation behaviors of antibiotics in water-sediment system under simulated light and wind waves.

Antibiotics can generally be detected in the water-sediment systems of lakes. However, research on the migration and transformation of antibiotics in water-sediment systems based on the influences of light and wind waves is minimal. To address this research gap, we investigated the specific impacts of light and wind waves on the migration and transformation of three antibiotics, norfloxacin (NOR), trimethoprim (TMP), and sulfamethoxazole (SMX), under simulated light and wind waves disturbance conditions in a water-sediment system from Taihu Lake, China. In the overlying water, NOR was removed the fastest, followed by TMP and SMX. Compared to the no wind waves groups, the disturbance of big wind waves reduced the proportion of antibiotics in the overlying water. The contributions of light and wind waves to TMP and SMX degradation were greater than those of microbial degradation. However, the non-biological and biological contributions of NOR to degradation were almost equal. Wind waves had a significant impact on the microbial community changes in the sediment, especially in Methylophylaceae. These results verified the influence of light and wind waves on the migration and transformation of antibiotics, and provide assistance for the risk of antibiotic occurrence in water and sediments.

Influence by varying organic matter content and forms in suspended particulate matter: impacts on the adsorption of tetracycline and norfloxacin.

Antibiotics are commonly detected in natural waters. The organic matter (OM) in suspended particulate matter (SPM) has a critical impact on the adsorption of antibiotics in water. We investigated the contribution of OM content and form to the adsorption of tetracycline (TC) and norfloxacin (NOR) in the SPM of Taihu Lake. To change the content and form of OM in SPM, the samples were subjected to pyrolysis at 505 ˚C and oxidization with H2O2, respectively. Combustion almost completely removed OM, while oxidation removed most of the OM and transformed the remaining OM. Regardless of whether the OM changed or not, the adsorption of NOR and TC by SPM was more in line with the pseudo-second-order kinetic model instead of pseudo-first-order. The fitting of the intraparticle diffusion model showed that the removal of OM had a certain degree of change in the adsorption process. The isothermal adsorption of TC in all samples was more in line with the Temkin model. The isothermal adsorption of NOR in the oxidized sample conformed to the Temkin model, while it conformed to the Langmuir model in the original sample and the sample removed OM via combustion. The adsorption capacity of SPM with almost complete removal of OM significantly decreased, while conversely, the adsorption capacity of SPM after oxidation increased. This indicates that both the content and form of OM affect the adsorption of antibiotics by SPM, and the form of OM has a greater impact. The contribution of OM to NOR adsorption was greater than that of TC. In conclusion, the results verify the importance of OM in adsorbing antibiotics onto SPM, which may provide basic data for antibiotic migration in surface water.

Variable promotion of algae and macrophyte organic matter on methanogenesis in anaerobic lake sediment.

Shallow lakes are an important natural source of atmospheric methane (CH4), and the input of autochthonous organic matter (OM) into their sediments encourages methanogenesis. Although algal- and macrophytic-originated OM in these lakes are expected to have different impacts on methanogenesis and methanogenic archaeal communities in lake sediments owing to their various properties, their specific influence and role in sediment remain unclear. In this study, a 148-day incubation was carried out by adding algal- and macrophytic-OM to the sediments of shallow eutrophic Lake Chaohu and Lake Taihu in China. CH4 was periodically monitored, while the methanogens were examined via qPCR and high-throughput sequencing at the end of incubation. Algal-OM stimulated CH4 production more than macrophytic-OM in both sediments, with the rates initially increasing and then decreasing before reaching a relative constant. Macrophytic-OM promoted CH4 production to a comparable extent in both lakes, while algal-OM promoted greater CH4 in Lake Chaohu than in Lake Taihu. However, algal-OM did not significantly increase mcrA gene copies, while macrophytic-OM did by 17.0-20.1-fold. Algal-OM potentially promoted the methylotrophic pathway in Lake Taihu but did not change the methanogenic structure in Lake Chaohu. Comparatively, macrophytic-OM promoted CH4 production mainly by acetoclastic methanogen proliferation in both lakes. More CH4 release with algal-OM compared to macrophytic-OM deserves further attention owing to the prevailing increasing algal blooms and the declining macrophyte population in lakes.

Effects of florfenicol on methane accumulation and changes in the structure of the prokaryotic community in a water-sediment system.

Florfenicol has been widely used in the veterinary and aquaculture to control bacterial diseases because of its high efficacy, quick effect, and low cost. The water-sediment system has become an important sink for florfenicol, and the anaerobic environment of lake sediments is favorable for methane (CH4) production. Although antibiotics may impact methanogenesis under anaerobic conditions, the influence of florfenicol on CH4 accumulation in anaerobic water-sediment system remains uncertain. This study evaluated how florfenicol affects CH4 accumulation and the structure of the prokaryotic community in a water-sediment system. Anaerobic systems with different florfenicol concentrations (0, 0.2, 1, 5 and 10 mg/L) were incubated and CH4 accumulation, pH, total organic carbon content, degradation ratio of florfenicol, and structure of the prokaryotic community were monitored. It was found that CH4 accumulation raised in low florfenicol (0.2 and 1 mg/L) systems during the growth period, while CH4 accumulation declined in high florfenicol (5 and 10 mg/L) systems. In the first 13 d, 83.67-99.30 % of florfenicol degraded in different treatments. The addition of florfenicol also influenced the structure of the prokaryotic community of the sediments. Proteobacteria and Chloroflexi were dominant at the phylum level. The dominant taxa at the order level gradually changed from Methanomicrobiales to Methanobacteriales, and finally to Methanosarcinales, indicating the dynamic transformation of methanogens in the reactor. This study reveals the effects of florfenicol on CH4 production under anaerobic conditions and provides a theoretical basis for further research on the underlying mechanisms. The findings also provide some basic data on the impact of new pollutants on the global carbon cycle and greenhouse gas emission.

Effects of suspended particulate matter from natural lakes in conjunction with coagulation to tetracycline removal from water.

Coagulation is a common method used to remove suspended particulate matter (SPM) from the water supply. SPM has preferable adsorption ability for antibiotics in water; therefore, SPM adsorption and coagulation may be a possible way to remove tetracycline (TC) from water. This study carried out coagulation experiments combining SPM collected from a natural lake at a location with three common coagulants-polyaluminum sulfate, polyaluminum chloride, and polyferric sulfate-under different pH values, exploring the adsorption of TC by SPM, coagulation of SPM with TC, and the primary influencing factors of this process. The maximum removal rate of TC can reach 97.87% with an SPM concentration of 1000 mg/L. Multi-factor analysis of variance showed the importance of various TC removal factors, which were ranked as follows: SPM concentration â‰« initial TC concentration > type of coagulant > pH values. The higher the SPM concentration, the better the TC removal (p < 0.001). Fourier infrared spectroscopy results demonstrated the strong adsorption effect of SPM on TC after being combined with a coagulant, and scanning electron microscopy also indicated that SPM becomes effective nuclei in the coagulation process, which is a possible reason for better TC removal. However, the effluent turbidities under 1000 mg/L SPM concentrations were high without coagulant aid. With the addition of coagulant aid anion polyacrylamide, the TC removal remained unchanged, effluent turbidity significantly reduced, and the TC desorption became low. These results indicate that applying SPM from natural lakes in the coagulation process could potentially remove TC in water.

Electrolysis-sulfate-reducing up-flow sludge bed-biological contact oxidation reactor for Norfloxacin removal from wastewater with high sulfate content.

This study investigated the treatment of 100-mg/L Norfloxacin (NOR) wastewater containing high concentrations of sulfate through a combination of electrolysis, sulfate-reducing up-flow sludge bed (SRUSB), and biological contact oxidation reactor (BCOR) treatments. Results revealed that after 62 h, the reaction system had processed over 97% of the NOR. Additionally, electrolysis with sodium sulfate as the electrolyte transformed 87.8% of the NOR but only 33.5% of the total organic carbon (TOC). In the SRUSB, the TOC and SO42- contents were simultaneously reduced by 87.4% and 95.6%, respectively, providing a stable environment to the BCOR. In the BCOR, 36.3% and 85.9% of the NOR and TOC were degraded. High-performance liquid chromatography-tandem mass spectrometry analysis identified three possible degradation pathways under the attack of -OH during electrolysis, including defluorination, piperazinyl ring transformation, and quinolone ring transformation. Furthermore, the Illumina HiSeq sequencing results demonstrated that the sulfate-reducing bacteria (represented by Desulfobacter and Desulfobulbus) in the SRUSB and the sulfate-oxidizing bacteria (mainly consisting of Gammaproteobacteria and Alphaproteobacteria) in the BCOR played important roles in carbon chain oxidation and benzene ring opening and thoroughly degraded the electrolysis products. Thus, this method effectively overcomes the incomplete degradation and low removal efficiency issues associated with single electrolysis or biological methods in traditional processes.

Spatial variations in diffusive methane fluxes and the role of eutrophication in a subtropical shallow lake.

Shallow lakes account for most of the diffusive CH4 emissions from global lakes, and they also suffer from eutrophication worldwide. Determining the effect of eutrophication on diffusive CH4 fluxes is fundamental to understanding CH4 emissions in shallow lakes. This study aimed to investigate the spatial variations in diffusive CH4 fluxes and explore the role of eutrophication in Lake Chaohu, a large and shallow eutrophic lake in the lower reaches of the Yangtze River. A one-year field observation was carried out to examine CH4 concentrations in the sediment and water and the diffusive fluxes of CH4 across the sediment-water interface (Fs-w) and water-air interface (Fw-a). Both Fs-w (0.306-1.56 mmol m-2 d-1) and Fw-a (0.097-0.529 mmol m-2 d-1) were upward and showed significant spatial heterogeneity and were significantly positively correlated. Parameters related to eutrophication had significant positive relationships with Fw-a, and the total phosphorus distribution in the water explained the greatest proportion of the spatial variation in Fw-a. Distance to shore and water depth were inversely correlated with Fw-a and modified the effects of eutrophication. Overall, the results provide direct evidence of the key role of eutrophication in shaping the spatial distribution of diffusive CH4 fluxes and a scientific basis for predicting changes in CH4 emissions with future eutrophication changes in shallow lakes in subtropical zones.

Impact of sediment characteristics on adsorption behavior of typical antibiotics in Lake Taihu, China.

Sediment adsorption is one of the main fates of antibiotics in aquatic environments. However, few studies have compared the physicochemical properties of sediments from the same aquatic ecosystem but at different locations and correlated them with antibiotic adsorption efficiency. To predict the adsorption of antibiotics in water-sediment systems more accurately, this study conducted experiments with tetracycline (TC) and oxytetracycline (OTC) in tetracyclines, ciprofloxacin (CIP) in fluoroquinolones, and roxithromycin (ROX) in macrolides. Sediments from different locations in Lake Taihu, China, were collected to determine the adsorption properties of CIP, TC, OTC, and ROX. Moreover, the physicochemical properties of the sediments were measured and the correlation between these properties and antibiotic adsorption were discussed to establish a model for predicting adsorption parameter Kd. The antibiotic adsorption performance of sediments was high in heavily polluted and grassy areas but poor in estuarine areas of the lake, suggesting that adsorption effectiveness was affected by the physicochemical properties of sediments. Based on the established model, the specific surface area, organic carbon, and cation exchange capacity played the most significant roles. The study further determined that the predicted and actual values showed a good linear fitting relationship. Therefore, the model effectively predicted the antibiotic adsorption performance of different sediments and provided recommendations for the environmental trend and risk assessment of antibiotics.

Effect of particle size on adsorption of norfloxacin and tetracycline onto suspended particulate matter in lake.

Aquatic systems are important sinks of antibiotics; however, their final destination has not been completely elucidated. Therefore, we investigated the adsorption behaviors of suspended particulate matter (SPM) in lakes to support the analysis of the migration and transformation of antibiotics in lacustrine environments. SPM was collected from Meiliang Bay (ML) and Gonghu Bay (GH) in Lake Taihu, China, which was sieved into four particle sizes of >300, 150-300, 63-150, and <63 µm for subsequent antibiotic adsorption experiments. All particles exhibited rapid and substantial adsorption of tetracycline and norfloxacin. Most size fractions fit a Langmuir model, indicative of monomolecular adsorption, except the <63-µm fraction, which fit a Freundlich model. Particle size had a substantial influence on antibiotic adsorption; the 63-150-µm fraction had the greatest adsorption capacity, while the >300-µm fraction had the lowest capacity. The influence of particle size on adsorption was mainly related to SPM physicochemical properties, such as cation exchange capacity, surface area, and organic matter content, rather than types of functional groups. Considering the mass ratios, the <63-µm fraction had the greatest contribution to adsorption. Antibiotics adsorbed onto the SPM from ML and GH exhibited different behaviors. The ML SPM settled more readily into sediment, and larger, denser particles were more resistant to resuspension. Conversely, the GH SPM was more likely to be found in the water column, and larger, less-dense particles remained in the water column. These results help improve our understanding of the interactions between SPM and antibiotics in aquatic systems.

Effects of wind-wave disturbances on adsorption and desorption of tetracycline and sulfadimidine in water-sediment systems.

Wind-wave disturbances frequently disperse sediment particles into overlying water, which facilitates the adsorption and desorption of contaminants in aquatic ecosystems. Tetracycline (TC) and sulfadimidine (SM2) are common antibiotics that are frequently found in aquatic environments. This study utilized microcosms, comprising sediment and water from Lake Taihu, China, to examine the adsorption and desorption of TC and SM2 under different wind-wave disturbances in a shallow lake environment. The adsorption experiments were conducted with three different concentrations (1, 5, 10 mg/L) of TC and SM2 in the overlying water, and two different (background and strong) wind-wave conditions for 72 h. Subsequently, four microcosms were employed in a 12-h desorption study. Analysis of adsorption progress showed that TC concentration in the overlying water decreased quickly, while SM2 remained almost constant. In the desorption experiments, SM2 released to the overlying water was an order of magnitude greater than TC. These results indicate that sediment particles strongly adsorb TC but weakly adsorb SM2. Compared to background conditions, the strong wind-wave conditions resulted in higher concentrations of TC and SM2 in sediment and facilitated their migration to deeper sediment during adsorption, correspondingly promoting greater release of TC and SM2 from sediment particles into the overlying water during desorption.

Migration of two antibiotics during resuspension under simulated wind-wave disturbances in a water-sediment system.

In this study, the migration of antibiotics (norfloxacin, NOR; and sulfamethoxazole, SMX) under simulated resuspension conditions across the sediment-water interface were quantified for two locations in China: point A, located in Meiliang Bay of Lake Taihu, and point B, located in Dapukou of Lake Taihu. The concentrations of suspended solids (SS) in the overlying water amounted to 100, 500, and 1000 mg/L during background, moderate, and strong simulated wind-wave disturbances, respectively. At each SS level, the initial concentrations of the two antibiotics were set to 1, 5, and 10 mg/L. The results showed that both resuspended SS and the initial concentration of antibiotics could influence the migration of NOR in the water-sediment system. Specifically, both higher SS and initial antibiotic concentrations were associated with higher rates of migration and accumulation of NOR from water to sediment. In contrast, the migration of SMX in the water-sediment system was not impacted by SS or initial antibiotic concentration. The adsorption capacities of sediments for NOR and SMX were significantly different at both locations, possibly reflecting differences in cation exchange capacity (CEC) and organic material (OM) contents. In general, higher CEC and OM values were found in sediments with a higher adsorption capacity for the antibiotics. When CEC and OM values of sediments were higher, the adsorption capacity reached up to 51.73 mg/kg. Large differences in the migration from water to sediment were observed for the two antibiotics, with NOR migration rates higher than those of SMX. The accumulation of NOR in surface sediment during resuspension was about 14 times higher than that of SMX. The main reason for this is that the chemical adsorption of NOR is seldom reversible. Overall, this study demonstrates that resuspension of NOR and SMX attached to sediments under simulated wind-wave disturbances can promote the migration of the antibiotics from water to sediment; these results could be useful for assessing the migration and fate of commonly used antibiotics in water-sediment systems.

Removal of chromium (VI) from water using nanoscale zerovalent iron particles supported on herb-residue biochar.

A composite material consisting of nanoscale zerovalent iron particles supported on herb-residue biochar (nZVI/BC) was synthesized and used for treatment of Cr(VI)-contaminated water. The effects of initial pH, chromium concentration, contact time, and competition with coexisting anions and natural organic matter (NOM) were also investigated. nZVI/BC was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and scanning electron microscopy analysis (SEM), and the Brunauer-Emmett-Teller surface area was measured. TEM and X-ray photoelectron spectroscopy (XPS) analysis before and after reaction with Cr(VI) showed that reduction and coprecipitation occurred during hexavalent chromium adsorption. The removal of Cr(VI) was highly pH-dependent and the adsorption kinetics data agreed well with the pseudo-second-order model. The presence of SO42- and humic acid promoted Cr(VI) removal at both low and high concentrations, while the HCO3- inhibited the reaction. These results prove that nZVI/BC can be an effective reagent for removal of Cr(VI) from solutions.

Low-cost magnetic herbal biochar: characterization and application for antibiotic removal.

Magnetic biochar (M-BC) was derived from herbal medicine waste, Astragalus membranaceus residue, and was used as an adsorbent for ciprofloxacin removal from aqueous solutions. The M-BC was characterized by Brunauer-Emmett-Teller surface area analyses, Fourier transform infrared spectrometry, X-ray diffraction analysis, hysteresis loops, scanning electron microscopy energy-dispersive spectrometry, and X-ray photoelectron spectroscopy. The BET surface area increased from 4.40 to 203.70 m2/g after pyrolysis/magnetic modification. Batch experiments were performed at different dosages, initial concentrations, contact times, and solution pHs. Adsorption performances were evaluated using Langmuir and Freundlich isotherm models, and the results indicated that the Langmuir model appropriately described the adsorption process. The kinetic data were better fitted by a pseudo-second-order kinetic model. The maximum ciprofloxacin removal was observed at pH 6 (adsorption capacity of 68.9 ± 3.23 mg/g). Studies demonstrated that magnetically modified biochar might be an attractive, cost-effective, and easily separated adsorbent for contaminated water. Graphical abstract.

Heavy Metal Pollution, Fractionation, and Potential Ecological Risks in Sediments from Lake Chaohu (Eastern China) and the Surrounding Rivers.

Heavy metal (Cr, Ni, Cu, Zn, Cd, and Pb) pollution, fractionation, and ecological risks in the sediments of Lake Chaohu (Eastern China), its eleven inflowing rivers and its only outflowing river were studied. An improved BCR (proposed by the European Community Bureau of Reference) sequential extraction procedure was applied to fractionate heavy metals within sediments, a geoaccumulation index was used to assess the extent of heavy metal pollution, and a risk assessment code was applied to evaluate potential ecological risks. Heavy metals in the Shuangqiao and Nanfei Rivers were generally higher than the other studied sites. Of the three Lake Chaohu sites, the highest concentrations were identified in western Chaohu. Heavy metal pollution and ecological risks in the lake's only outflowing river were similar to those in the eastern region of the lake, to which the river is connected. Heavy metal concentrations occurred in the following order: Cd > Zn > Cu > Pb ≈ Ni ≈ Cr. Cr, Ni, and Cu made up the largest proportion of the residual fraction, while Cd was the most prominent metal in the exchangeable and carbonate-included fraction. Cd posed the greatest potential ecological risk; the heavy metals generally posed risks in the following order: Cd > Zn > Cu > Ni > Pb > Cr.

Oxygen and phosphorus dynamics in freshwater sediment after the deposition of flocculated cyanobacteria and the role of tubificid worms.

Flocculation is a promising method for controlling harmful algal blooms; however, little is known about the effects of algae deposition by flocculation on benthic oxygen (O2) and nutrient dynamics. In this study, we aimed to investigate the influence of cyanobacteria flocculation deposition on benthic O2 and phosphorus (P) dynamics and the role of tubificid worms in the process. Chitosan and sediment particles were used to flocculate and deposit cyanobacteria cells onto lake sediment. The impulse deposition of algal flocculation degraded the deposited algal cells, which decreased the O2 penetration depth in sediment and increased the O2 uptake rate. Algae deposition also increased the soluble reactive P (SRP) in pore water and loosely adsorbed P in sediment, and changed SRP flux. Tubificid worms transported algal cells deeper into the sediment, mitigated their degradation, and altered the O2 penetration depth, but not the O2 uptake rate. Tubificid worms enhanced the increase in pore-water SRP and loosely adsorbed P in sediment. Therefore, the deposition of algal flocculation modifies the benthic O2 and P dynamics, and tubificid worms can mitigate or enhance some of these processes.

[Statistical analysis of factors influencing N2O emission from paddy fields in Asia].

Most previous studies attributed variation in N2O emission from paddy fields to water managements and fertilizer input. In this study, we compiled a database of N2O emission from paddy fields in Asia, including water management, type and amount of nitrogen fertilizer, soil property, climate and rice types. After screening the influencing factors with statistical significance (p < 0.01) such as different water managements, N input, different organic N types, interaction of soil total nitrogen content and different pH levels, different annual temperature levels, and different rice types, a linear model was established to link N2O emission to those factors, which could totally explain up to 60.7% of the observed variation in N2O emission. The most important influencing factor was the amount of N fertilizer input, which had significantly positive correlation with N2O fluxes. Relative emission fluxes of continuous flooding, intermittent irrigation and wet irrigation were 0.17:0.56: 1. The soil total nitrogen content had significantly positive effect on N2O fluxes while the optimum pH for N2O emission was pH > 8. Straw of N-fixing crop had much higher fluxes than other organic fertilizers while manure had no significant effects on increasing N2O emission. Application of other crop straws actually reduced N2O emission by 36%, as compared with fields without organic N input. The relative fluxes for early rice and later rice were 71% and 48% of that for single rice, respectively. Inclusion of more influencing factors such as soil property, climate and rice type helped explaining more of the variations in the observed N2O emission from paddy fields.