Responses of anammox and sulfur/pyrite autotrophic denitrification in one-stage system to high nitrogen load: Performance, metabolic and bacterial community.

To remove residual nitrate from anammox process and achieve efficient nitrogen removal, a two-stage system (TAS) with the two individual reactors and a one-stage system (OAS) with the spatial functional areas in one reactor were established via anammox coupling sulfur autotrophic denitrification. The total nitrogen removal efficiency (TNRE) of OAS system (97.85 ± 1.92%) was higher than that of TAS system (93.63 ± 1.87%) under the influent NH4+-N and NO2--N of 227 and 300 mg/L. Meanwhile, the responses of microbial metabolism to high nitrogen load were investigated in term of microbial metabolites, electron transfer and metabolic activity. Microbial metabolites characteristics demonstrated that the OAS system secreted more EPS with lower protein (PN)/polysaccharide (PS) ratio than that in the TAS system, which was beneficial to protect bacteria from high nitrogen load. Electrochemical analysis suggested that the secretion of electron conductive substance (such as PN, PS) and redox active substances (such as flavin mononucleotide, the binding of flavins and cytochrome c on the outer membrane) were increased in the OAS system, which promoted the electron transfer efficiency. Moreover, the electron transport system activity (ETSA) values and ATP contents in OAS system were higher than that in the TAS system, which indicated that metabolic activity was improved in OAS system under the stimulation of high nitrogen load. Additionally, the bacterial community analysis indicated that the functional bacteria of Candidatus_Kuenenia and Armatimonadetes_gp5 had higher abundance in the OAS system than that in the TAS system, which was beneficial to realize the stable nitrogen removal performance. Overall, the responses mechanism of the OAS system was established to explain the resistant to high nitrogen load.

Fate of phthalates in a river receiving wastewater treatment plant effluent based on a multimedia model.

Phthalic acid esters (PAEs) can enter environment media by secondary effluent discharge from wastewater treatment plants (WWTP) into receiving rivers, thus posing a threat to ecosystem health. A level III fugacity model was established to simulate the fate and transfer of four PAEs in a study area in Tianjin, China, and to evaluate the influence of WWTP discharge on PAEs levels in the receiving river. The results show that the logarithmic residuals of most simulated and measured values of PAEs are within one order of magnitude with a good agreement. PAEs in the study area were mainly distributed in soil and sediment phases, which accounted for 84.66%, 50.26%, 71.96% and 99.09% for dimethyl phthalate (DMP), diethyl phthalate (DEP), dibutyl phthalate (DBP) and di-(2-ethylhexyl) phthalate (DEHP), respectively. The upstream advection accounted for 77.90%, 93.20%, 90.21% and 90.93% of the total source of DMP, DEP, DBP and DEHP in the river water, respectively, while the contribution of secondary effluent discharge was much lower. Sensitivity analysis shows that emission and inflow parameters have greater influences on the multimedia distributions of PAEs than physicochemical and environmental parameters. Monte Carlo analysis quantifies the uncertainties and verifies the reliability of the simulation results.

Apparent relationships between anthropogenic factors and climate change indicators and POPs deposition in a lacustrine system.

Climate change and anthropogenic activities are expected to impact the environmental behaviors and fates of persistent organic pollutants (POPs), however, quantitative studies on these combined factors are scarce. In this study, dichlorodiphenyltrichloroethane (DDTs), polycyclic aromatic hydrocarbons (PAHs), and polychlorinated biphenyls (PCBs) were used as examples to identify how and when those factors may be related to the deposition of POPs in the sediment of Lake Chaohu, China, using generalized additive models (GAMs). Three historical trends of DDT, PAH, and PCB deposition were delineated in a dated sediment core encompassing ~100 years of historical record: a steady state or gradually increasing stage, a rapidly increasing stage, and a declining stage. The GAM results showed that aquatic total phosphorus (TP) concentrations and regional GDP (anthropogenic factors) were dominant contributors to POP accumulation rates in the lake sediment. The fitted relationships between air temperature and sedimentary DDT and PAH concentrations were linear and negative, while a positive linear relationship was found for PCBs, suggesting that Lake Chaohu may have become a net source for DDTs and PAHs, and a sink for PCBs, under a progressively warming climate.

Historical records of polycyclic aromatic hydrocarbon deposition in a shallow eutrophic lake: Impacts of sources and sedimentological conditions.

Sediment core samples collected from Lake Chaohu were analyzed for 15 priority polycyclic aromatic hydrocarbons (PAHs) to assess the spatial and temporal distributions of the PAHs during lacustrine sedimentary processes and regional economic development. Assessing the PAH sedimentary records over an approximately 100-year time span, we identified two stages in the PAH inputs and sources (before the 1970s and after the 1970s) in the eastern lake region near a village, whereas three stages (before the 1950s, 1950s-1990s and after the 1990s) were identified in the western lake region near urban and industrial areas. Rapid increases in the PAH depositional fluxes occurred during the second stage due to increased human activities in the Lake Chaohu basin. The composition and isomeric ratios of the PAHs revealed that pyrolysis is the main source of PAHs in this lake. Strong positive relationships between PAH concentration and the total organic carbon concentration, sediment grain size (<4µm), as well as the local population and Gross Domestic Product indicated that the sedimentary conditions impact the depositional characteristics of the PAHs; simultaneously, socioeconomic activities, such as energy consumption and the levels of urban industrialization and civilization, affect both the composition and abundance of the PAHs.

A method for simulating spatial fates of chemicals in flowing lake systems: Application to phthalates in a lake.

In order to describe spatio-temporal distribution of chemicals in flowing lake systems, a dynamic multimedia fate model of chemicals with spatial differentiation was constructed by coupling the level IV fugacity model with lake hydrodynamics. It was successfully applied to four phthalates (PAEs) in a lake recharged by reclaimed water and its accuracy was verified. Results show that under the long-term influence of flow field, the distributions of PAEs in both lake water and sediment have significant spatial heterogeneity of 2∼5 orders of magnitude, but present different distribution rules, which was explained by analysis of PAE transfer fluxes. The spatial distribution of PAEs in the water column depends on hydrodynamic conditions and whether the primary source is reclaimed water or atmospheric input. Slow water exchange and flow speed promote the migration of PAEs from water to sediment, causing them to always accumulate in sediments far away from the recharging inlet. Uncertainty and sensitivity analysis show that the PAE concentrations in water phase are mainly affected by emission and physicochemical parameters, while those in sediment phase are also sensitive to environmental parameters. The model can provide important information and accurate data support for the scientific management of chemicals in flowing lake systems.

Paper-Based Microfluidic Sensors for Onsite Environmental Detection: A Critical Review.

A newly developed research topic, fabricated paper-based microfluidic sensors, was discussed in the field of low-cost environmental detection. Distinguished with the traditional dipstick or lateral-flow setups, these paper-based microfluidic sensors can serve as a tool for onsite quantitative and semi-quantitative measurements, without risks to cause environmental pollution. They have attracted increasing interest since the first easy-fabricated paper-based setup reported by Whitesides group in 2007. Most of the publications utilized paper-based sensors in clinical detection. In recent years, some groups started to use these sensors in environmental measurement, leading to precise, easy operation, low-cost, and eco-friendly methods for onsite detection. In this review, paper-based microfluidic sensors were briefly introduced, followed by literatures review and discussion for future perspectives.

Characterization and flocculation performance of a newly green flocculant derived from natural bagasse cellulose.

A newly green natural polymer bagasse cellulose based flocculant (PBCF) was synthesized utilizing a grafting copolymerization method for effectively enhancing humic acid (HA) removal from natural water. This work aims to investigate flocculation behavior of PBCF in synthetic water containing HA, and the effects of flocculant dose and initial solution pH on flocculation performance. Results showed that PBCF functioned well at a flocculant dose of 60 mg/L and pH ranging from 6.0 to 9.0. The organic removal efficiency in synthetic water in terms of HA (UV254) and chemical oxygen demand (COD Mn) were up to 90.6% and 91.3%, respectively. Furthermore, the charge neutralization and adsorption bridging played important roles in HA removal. When applied for lake water, PBCF removed 91.6% turbidity and 50.0% dissolved organic matter, respectively. In short, PBCF demonstrates great potential in water treatment in a safe and environmentally friendly or 'green' way.

Polychlorinated biphenyl detection in organic solvents with paper-based analytical devices.

Sample pretreatment process is usually performed before real sample detection. Extraction is one of the most prevalent pretreatment methods. Due to the unequal solubility in two liquid phases, target is extracted (usually from water to organic phase) and further detected with laboratory instruments. Although the analytical instruments have high sensitivity and selectivity, they are relatively expensive and require skilful hands, which is restricted to laboratory use. Here, paper-based analytical devices (µPADs) for measuring samples extracted with organic solvents were tested. The µPADs were employed as a filter for buffer exchange, allowing the transfer of targets from organic solvent to water-based buffer, which could be specifically detected by water-based assays. As an example, polychlorinated biphenyls (PCBs) in n-hexane were detected with aptamer and gold nanoparticles (AuNPs) on µPADs within 30 min. The result of colour change can be recognized from 70.0 ng/L with a low loading amount (0.5 µL). Instead of laboratory instrumental analysis with relative high cost, this assay showed the promising utility of µPADs for target detection after sample pretreatment, which could be utilized as a general platform for inexpensive onsite detection.

Occurrence, migration and health risk of phthalates in tap water, barreled water and bottled water in Tianjin, China.

This study was to investigate the occurrence, migration and health risk of phthalic acid esters (PAEs) in tap water, barreled water and bottled water in Tianjin, China. Six priority controlled PAEs were measured, among which the detection frequency of butyl benzyl phthalate (BBP), dibutyl phthalate (DBP) and di(2-ethylhexyl) phthalate (DEHP) was 100%, while the others were not detected. The concentration of DEHP was higher than BBP and DBP in all the samples. The initial ∑3PAEs concentrations in tap water, barreled water and bottled water were 2.409 ± 0.391 µg/L, 1.495 ± 0.213 µg/L and 1.963 ± 0.160 µg/L, respectively. Boiling tap water could reduce the PAEs content to an extent, but they increased significantly in hot tap water contacting with disposable plastic cups. The migration of PAEs in barreled water and bottled water were positively correlated with storage time and temperature, which could be described by exponential models. The hazard indexes of PAEs in different types of drinking water were very low. However, the human carcinogenic risks of DEHP will reach the maximum acceptable risk level of 10-6 when bottled water is stored for 8.8 days at 40 °C, 7.7 days at 50 °C, or 6.1 days at 60 °C.

Specific microbial diversity and functional gene (AOB amoA) analysis of a sponge-based aerobic nitrifying moving bed biofilm reactor exposed to typical pharmaceuticals.

Four bench-scale sponge-based aerobic nitrifying moving bed biofilm reactors (MBBRs) were used to treat municipal wastewater containing typical pharmaceuticals (1 mg/L, 2 mg/L and 5 mg/L). This preliminary research aims to investigate the effects of sulfadiazine (SDZ), ibuprofen (IBU) and carbamazepine (CBZ) on nitrification performance and explore specific microbial diversity and functional gene (Ammonia-oxidizing bacteria (AOB), amoA) of MBBRs. After 90 days of operation, the MBBR without pharmaceuticals could remove up to 97.4 ± 1.5% of NH4+-N while the removals of NH4+-N by the MBBRs with SDZ, IBU and CBZ were all suppressed to varying degrees. Based on the Shannon and Chao 1 index, the specific microbial diversity and richness in biofilm samples increased at a range of 1 mg/L to 2 mg/L pharmaceuticals (SDZ, IBU or CBZ) and started decreasing after the pharmaceutical concentration was higher than 2 mg/L. The determination of functional gene (AOB amoA) showed that Proteobacteria was the most dominant bacteria within all biofilms with the relative abundance ranging from 24.81% to 55.32%. Furthermore, Nitrosomonas was the most numerous genus in AOB, followed by Campylobacter and Thauera, whose relative abundance shifted under the pressure of different pharmaceuticals.

Comparison study on the ammonium adsorption of the biochars derived from different kinds of fruit peel.

Application of biochars to remove inorganic nitrogen (NH4+, NO2-, NH3, NO, NO2, N2O) from wastewater and agricultural fields has gained a significant interest. This study aims to investigate the relationship between ammonium sorption and physicochemical properties of biochars derived from different kinds of fruit peel. Biochars from three species of fruit peel (orange, pineapple and pitaya) were prepared at 300, 400, 500 and 600 °C with the residence time of 2 h and 4 h. Their characteristics and sorption for ammonium was evaluated. The results show a clear effect of pyrolysis conditions on physicochemical properties of biochars, including elemental composition, functional groups and pH. The maximum NH4+ adsorption capacities were associated with biochars of orange peel (4.71 mg/g) and pineapple peel (5.60 mg/g) produced at 300 °C for 2 h. The maximum NH4+ adsorption capacity of the pitaya peel biochar produced at 400 °C for 2 h was 2.65 mg/g. For all feedstocks, biochars produced at low temperatures showed better NH4+ adsorption capacity. It was found that biochars had better adsorption efficiency on ammonium at a pH of 9. Adsorption kinetics of ammonium on biochars followed the pseudo-second-order kinetic model while Langmuir isotherm model could well simulate the adsorption behavior of ammonium on biochars. The adsorption mechanism of ammonium on biochars predominantly involved surface complexation, cation exchange and electrostatic attraction. Conclusively, the fruit peel-derived biochars can be used as an alternative to conventional sorbents in water treatment.

Characterization and sulfonamide antibiotics adsorption capacity of spent coffee grounds based biochar and hydrochar.

A large amount of spent coffee grounds is produced as a processing waste each year during making the coffee beverage. Sulfonamide antibiotics (SAs) are frequently detected in the environment and cause pollution problems. In this study, biochar (BC) and hydrochar (HC) were derived from spent coffee grounds through pyrolysis and hydrothermal carbonization, respectively. Their characteristics and sulfonamide antibiotics adsorption were investigated and compared with reference to adsorption capacity, adsorption isotherm and kinetics. Results showed BC possessed more carbonization and less oxygen-containing functional groups than HC when checked by Elemental Analysis, X-ray diffraction, X-ray photoelectron spectrometry and Fourier transform infrared. These groups affected the adsorption of sulfonamide antibiotics and adsorption mechanism. The maximum adsorption capacities of BC for sulfadiazine (SDZ) and sulfamethoxazole (SMX) were 121.5 µg/g and 130.1 µg/g at 25 °C with the initial antibiotic concentration of 500 µg/L, respectively. Meanwhile the maximum adsorption capacities of HC were 82.2 µg/g and 85.7 µg/g, respectively. Moreover, the adsorption mechanism for SAs adsorbed onto BC may be dominated by π-π electron donor-acceptor interactions, yet the SAs adsorption to HC may be attributed to hydrogen bonds. Further analysis of the adsorption isotherms and kinetics, found that physical and chemical interactions were involved in the SAs adsorption onto BC and HC. Overall, results suggested that: firstly, pyrolysis was an effective thermochemical conversion of spent coffee grounds; and secondly, BC was the more promising adsorbent for removing sulfonamide antibiotics.

Occurrence, fate and health risk assessment of 10 common antibiotics in two drinking water plants with different treatment processes.

The occurrence of antibiotics in drinking water has become a serious problem worldwide as they are a potential and real threat to human health. In this study, the variability of 10 typical antibiotics in two drinking water plants was investigated in two seasons (n = 12). The total concentrations of target antibiotics in raw water were significantly higher in winter than in summer, which may be attributed to the more frequent occurrence of colds and respiratory diseases as well as less rainfall in winter. The efficiency in removing the antibiotics varied from -46.5% to 45.1% in water plant A (WP-A) using a conventional process and 40.3% to 70.3% in water plant B (WP-B) with an advanced treatment process. Results indicated that the antibiotics in WP-A were mainly removed via the coagulation process. However in WP-B, the ultraviolet + chlorination process played a key role in antibiotics removal, followed by the pre-ozone + coagulation process. According to the human health risk assessment, it was suggested that the risk of drinking water was significantly higher than that of skin contact. However, the risk of carcinogenesis and non-carcinogenesis caused by antibiotics was at an acceptable level.

Food waste based biochars for ammonia nitrogen removal from aqueous solutions.

Biochar derived from waste has been increasingly considered as a potential green adsorbent due to its significant ability and affordable production costs. This study prepared and evaluated 7 types of food waste-based biochars (FWBBs) (including meat and bone, starchy staples, leafy stemmed vegetables, nut husks, fruit pericarp, bean dreg and tea leaves). The impacts of raw materials, pyrolysis temperatures (300, 400, 500, 600 and 700 °C), and residence time (2 h and 4 h) on the removal of ammonia nitrogen at different ammonia nitrogen concentrations (5, 10, 20, 50, 100, 150 mg/L) were investigated. The batch equilibrium and kinetic experiments confirmed that a FWBB dosage of 3 g/L at 25 °C could remove up to 92.67% ammonia nitrogen. The Langmuir isotherm model had the best fit to equilibrium experimental data with a maximum adsorption capacity of 7.174 mg/g at 25 °C. The pseudo-second order kinetic model well describes the ammonia nitrogen adsorption.

Historical record of polychlorinated biphenyls (PCBs) and special occurrence of PCB 209 in a shallow fresh-water lake from eastern China.

Concentrations of polychlorinated biphenyls (PCBs) were measured in dated sediment cores collected from the fifth largest freshwater lake in China, Lake Chaohu, to investigate PCB temporal trends, accumulation, and environmental fate. Total PCB concentrations in Lake Choahu sediments ranged from 0.03 to 24.11 ng g-1 (d.w.). PCB 209 was the dominant congener, accounting for 45.5%-83.9% of total PCBs detected after the mid-20th century. All PCB congeners were positively correlated with total organic carbon (TOC) concentrations. TOC-normalized PCB concentrations exhibited three stages of variation over time: a slight increase from their emergence in the early 20th century, followed by a rapid increase since the late 1950s (peaking in the late 1980s), before a general decrease to the present. Both compositional PCB patterns and principal component analysis (PCA) indicated a source switch from commercial PCBs to other sources. Major contributions of PCB209 to total PCBs in Lake Chaohu sediments is a highlight of this study, with results showing that PCB209 was derived from the upstream city of Hefei, and the production of phthalocyanine-type pigments is the likely source of PCB209.

National investigation of semi-volatile organic compounds (PAHs, OCPs, and PCBs) in lake sediments of China: Occurrence, spatial variation and risk assessment.

In this study, a large scale investigation of semi-volatile organic compounds (SVOCs) in sediments from 52 lakes, located in five geographic regions across China, was conducted to assess sediment quality in terms of organic contaminants. Concentrations of polycyclic aromatic hydrocarbons (PAHs), organochlorine pesticides (OCPs), and polychlorinated biphenyls (PCBs) in sediment were found to range between 17.00-6,633, 0.12-45.24, and 0.03-13.99ngg-1, respectively. Lake sediments from different regions exhibited variation in contamination levels, and in the compositions of isomers. The descending order of contamination levels for the three SVOCs groups (i.e., ∑PAHs, ∑OCPs, ∑PCBs) were as follows: the eastern plain region (EPR)>the Yunnan-Guizhou plateau (YGP)>the northeast China region (NCR)>the Qinghai-Tibet plateau (QTP)>the Mongolia-Xinjiang plateau (MXP). High molecular weight PAHs, OCPs and PCBs were found at high concentrations in parts of the EPR and YGP, while lighter isomers were likely to be atmospherically transported, resulting in their nationwide distribution. The sources and type variation (local input or atmospheric deposition) are the primary controls of spatial variation. Additionally, human related socio-economic factors, and geographic conditions also played important roles in influencing the spatial differentiation. According to simple sediment quality guidelines (SQG), the risks posed by PCBs in sediments were not as serious as those posed by PAHs and DDT.

Spatial distribution, potential risk assessment, and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in sediments of Lake Chaohu, China.

Twenty-nine sediment samples were collected from Lake Chaohu, a shallow eutrophic lake in Eastern China, and were analyzed for 15 priority polycyclic aromatic hydrocarbons (PAHs) to determine the spatial distribution and exposure risks of PAHs. Three receptor models, the principal component analysis-multiple linear regression (PCA-MLR) model, the positive matrix factorization (PMF) model, and the Unmix model, were used in combination with the PAHs diagnostic ratios to investigate the potential source apportionment of PAHs. A clear gradient in the spatial distribution and the potential toxicity of PAHs was observed from west to east in the sediments of Lake Chaohu. ∑15PAH concentrations and the TEQ were in the range of 80.82-30 365.01 ng g(-1) d.w. and 40.77-614.03, respectively. The highest values of the aforementioned variables were attributed to urban-industrial pollution sources in the west lake region, and the levels decreased away from the river inlets. The three different models yielded excellent correlation coefficients between the predicted and measured levels of the 15 PAH compounds. Similarly, source apportionment results were derived from the three receptor models and the PAH diagnostic ratios, suggesting that the highest contribution to the PAHs was from coal combustion and wood combustion, followed by vehicular emissions. The PMF model yielded the following contributions to the PAHs from gasoline combustion, diesel combustion, unburned petroleum emissions, and wood combustion: 34.49, 24.61, 16.11, 13.01, and 11.78 %, respectively. The PMF model produced more detailed source apportionment results for the PAHs than the PCA-MLR and Unmix models.