Understanding consumption-related sucralose emissions — A conceptual approach combining substance-flow analysis with sampling analysis

This paper explores the potential of combining substance-flow modelling with water and wastewater sampling to trace consumption-related substances emitted through the urban wastewater. The method is exemplified on sucralose. Sucralose is a chemical sweetener that is 600 times sweeter than sucrose and has been on the European market since 2004. As a food additive, sucralose has recently increased in usage in a number of foods, such as soft drinks, dairy products, candy and several dietary products. In a field campaign, sucralose concentrations were measured in the inflow and outflow of the local wastewater treatment plant in Linköping, Sweden, as well as upstream and downstream of the receiving stream and in Lake Roxen. This allows the loads emitted from the city to be estimated. A method consisting of solid-phase extraction followed by liquid chromatography and high resolution mass spectrometry was used to quantify the sucralose in the collected surface and wastewater samples. To identify and quantify the sucralose sources, a consumption analysis of households including small business enterprises was conducted as well as an estimation of the emissions from the local food industry.The application of a simple model including uncertainty and sensitivity analysis indicates that at present not one large source but rather several small sources contribute to the load coming from households, small business enterprises and industry. This is in contrast to the consumption pattern seen two years earlier, which was dominated by one product. The inflow to the wastewater treatment plant decreased significantly from other measurements made two years earlier. The study shows that the combination of substance-flow modelling with the analysis of the loads to the receiving waters helps us to understand consumption-related emissions.     

Relative importance of wastewater treatment plants and non-point sources of perfluorinated compounds to Washington State rivers

Perfluorinated compounds (PFCs) were measured in 10 Washington State rivers and 4 wastewater treatment plants (WWTPs) under periods of low and high flows to investigate the relative importance of point and non-point sources to rivers. PFCs were detected in all samples with summed values ranging from 1.11 to 74.9 ng/L in surface waters and 62.3-418 ng/L in WWTP effluent. Concentrations in 6 of the 10 rivers exhibited a positive relationship with flow, indicating runoff as a contributing source, with PFC loads greatest at all 10 waterbodies during high flows. Perfluoroheptanoic acid:perfluorooctanoic acid homologue ratios suggest atmospheric contributions to the waterbodies are important throughout the year. Principal component analysis (PCA) indicated distinct homologue profiles for high flow, low flow, and effluent samples. The PCA demonstrates that during the spring when flows and loads are at their greatest; WWTP discharges are not the primary sources of PFCs to the river systems. Taken together, the evidence provided signifies non-point inputs are a major pathway for PFCs to surface waters in Washington State.     

Occurrence of seven artificial sweeteners in the aquatic environment and precipitation of Tianjin,China

Seventy water samples, including wastewaters, tap waters, fresh surface waters, coastal waters, groundwaters, and precipitation samples, from Tianjin, China, were analyzed for seven commonly used artificial sweeteners (ASs). The concentrations of the investigated ASs were generally in the order of wastewater treatment plant (WWTP) influent > WWTP effluent > surface water > tap water > groundwater ≈ precipitation, while the composition profiles of ASs varied in different waters. Acesulfame, sucralose, cyclamate, and saccharin were consistently detected in surface waters and ranged from 50 ng/L to 0.12 mg/L, while acesulfame was the dominant AS in surface and tap waters. Aspartame was found in all of the surface waters at a concentration up to 0.21 μg/L, but was not found in groundwaters and tap waters. Neotame and neohesperidin dihydrochalcone were less frequently detected and the concentrations were low. The concentrations of the ASs in some of the surface waters were of the same order with those in the WWTP influents, but not with the effluents, indicating there are probably untreated discharges into the surface waters. The ASs were detected in precipitation samples with high frequency, and acesulfame, saccharin, and cyclamate were the predominant ASs, with concentrations ranging from 3.5 ng/L to 1.3 μg/L. A gross estimation revealed that precipitation may act as a source for saccharin and cyclamate in the surface environment of Tianjin city. Moreover, the presence of ASs in the atmosphere was primarily assessed by taking 4 air samples to evaluate their potential source in precipitation.     

Organic contaminants in the aquatic environment I. Sources and occurrence

Literature pertaining to the sources and occurrence of organic compounds in raw, potable and waste waters is reviewed. The introduction of organic micropollutants into the hydrological cycle is considered in terms of both point and non-point source discharges and the individual industrial and domestic sources of particular classes of organic chemicals are assessed. The occurrence in waters and waste waters of a wide variety of organic contaminants has been evaluated with regard to their concentrations in particular aqueous samples and frequency of occurrence. Although specific sources are known to be responsible for the addition of certain organic compounds to water and waste water, the occurrence of particular compounds cannot always be related to a particular source. In addition, it is evident that the reported occurrence of many organic contaminants has been limited by the capabilities of presently available analytical techniques.With the number of organic chemicals in use increasing, the potential for continued contamination of water resources exists. The implications for water quality and the possible effects generated by the introduction of organic compounds into the hydrological cycle on water re-use operations are discussed.     

Evaluation of chemical indicators for tracking and apportionment of phosphorus sources to Table Rock Lake in Southwest Missouri, USA

This work evaluated the suitability of selected chemical species as indicators for tracking and apportionment of point and non-point phosphorus sources within the Table Rock Lake watershed in Southwest Missouri, USA. The species were evaluated with respect to their uniqueness to specific source types, their ability to be detected in both sources and receiving waters, and the consistency of their concentration ratios to phosphorus. Four sampling events were conducted at 15 sample locations in one year to collect water samples for measuring the concentrations of total and dissolved phosphorus, seven anions, and 19 major and trace elements. Current analytical methods were sensitive enough for quantification of most of the chemical species in both sources and the receiving waterbody. Due to the high seasonal variation of phosphorus concentrations in source samples, no chemical species had consistent concentration ratios to phosphorus across source types. However, several chemicals were found to be unique to specific sources; bromide ion can be used as a unique indicator for the effluent of the largest wastewater treatment plant in the watershed.     

The application of a recently isolated strain of Bacteroides (GB-124) to identify human sources of faecal pollution in a temperate river catchment

Recent work has suggested that bacteriophages infecting Bacteroides are a potential tool for faecal source tracking, but that different host strains may be needed for different geographic areas. This study used a recently identified strain of Bacteroides (GB-124) to detect human sources of faecal pollution in a river catchment in southeast England (UK). A total of 306 river water, municipal wastewater and animal samples were obtained over a 16-month period. Bacteriophages capable of infecting GB-124 were present in all municipal wastewaters but were not detected in faecal samples from animals, and were detected at significantly lower levels (P< 0.001) in river waters directly downstream of a dairy farm. This last observation was despite the presence of high levels of faecal indicator bacteria at this site. The study suggests that GB-124 appears to be specific to human faeces. As such it may represent an effective and low-cost method of faecal source identification.     

Identification of the sources of fecal coliforms in an urban watershed using antibiotic resistance analysis

Bacteria such as fecal coliforms are used as indicators of fecal pollution in natural waters. These bacteria are found in the feces of most wild and domestic animals and thus provide no information as to the source of fecal contamination, yet identification of indicator bacteria sources allows improved risk assessment, remediation, and total daily maximum load (TDML) assessment of environmental waters. This bacterial source tracking study was initiated in order to identify the dominant source(s) of fecal contamination in the urban watershed of Stevenson Creek in Clearwater, Florida. Five sites that represent areas where routine monitoring has previously shown high levels of fecal coliforms were sampled over 7 months. Fecal coliforms were enumerated by membrane filtration, and antibiotic resistance analysis was used to "fingerprint" a subset of randomly selected isolates and statistically match them to fingerprints of fecal coliforms from known sources (the library). A field test of the classification accuracy of the library was carried out by isolating fecal coliforms from the soil and waters surrounding a failing onsite wastewater treatment and disposal system (OSTDS). The vast majority of the isolates were classified into the human category. The major sources of fecal pollution in Stevenson Creek over the course of the study were wild animal, human, and, to a lesser extent, dog. Overall, wild animal feces were identified as the dominant source when fecal coliform levels were high, but when fecal coliform levels were low, the dominant source was identified as human. The results of this study demonstrate that the sources of fecal indicator bacteria within one urban watershed can vary substantially over temporal and spatial distances.     

Faecal-Indicator Budgets for Recreational Coastal Waters: A Catchment Approach

This paper explores the application of a catchment faecal-indicator budget approach to the examination of faecal-indicator sources impacting on coastal recreational water quality. This involves (i) the characterization of water quality in sewage effluent and riverine inputs, and (ii) measurement and estimation of input flows; the product of these components yields the input flux of indicator organisms from each source. The impact of sewage-treatment scenarios on budgets is also investigated.     

Perfluorinated alkylated substances in the aquatic environment: An Austrian case study

Perfluorinated alkylated substances (PFAS) are of global interest due to their occurrence and persistency in the environment. This study includes surface waters and sediments for the analysis of eleven PFAS. The PFAS studied can be grouped in perfluoroalkyl carboxylates (PFCAs), perfluoroalkyl sulfonates (PFS) and perfluoroalkyl sulfonamides (PFSA). The two most important compounds are perfluorooctanoate (PFOA) and perfluorooctane sulfonate (PFOS). These two substances showed the most significant values for surface water samples with maximum concentrations of 21 ng l⁻¹ for PFOA and 37 ng l⁻¹ for PFOS. Sediment samples from seven Austrian lakes and the river Danube were studied. Whereas PFSA and PFS were not detected in any sediment sample PFCAs were detected in most of the lake samples in concentrations up to 1.7 μg kg⁻¹ dry wt. PFOA, perfluorohexanoic acid (PFHxA) and perfluoroheptanoic acid (PFHpA) were detected in all Danube river sediment samples in concentrations varying from 0.1 up to 5.1 μg kg⁻¹ dry wt. For the various sampling points the proportional mass flows deriving from wastewater discharges were calculated. Whereas only up to 10% of the average flow is discharged wastewater up to more than 50% of the PFAS mass flows in the rivers can be attributed to wastewater discharges. Besides wastewater different other pathways as emissions from point sources, further degradation of precursor products, runoff from contaminated sites or surface runoff as well as dry and wet deposition have to be considered as relevant sources for PFAS contamination in surface waters.     

Sources and growth dynamics of fecal indicator bacteria in a coastal wetland system and potential impacts to adjacent waters

Coastal wetlands are receiving increased attention as a putative source of fecal indicator bacteria (FIB) in Southern California coastal waters. We examined temporal trends of water and sediment-associated FIB after rain events along with spatial sediment characteristics at two sites within the Santa Ana River wetlands and made comparisons to FIB levels observed in adjacent surf zone waters. During the first two rain events, total coliforms (TC), Escherichia coli (EC) and enterococci (ENT) in wetland water and sediment samples peaked either on the same day or within several days of the rain event, while the third resulted in elevated wetlands sediment TC levels only. TC in adjacent coastal waters consistently peaked on the same day as the rain event and decreased quickly thereafter (within 1 day). The TC/EC ratios of surf zone samples consistently fell below 10, indicating an increased probability of human fecal contamination whereas wetland TC/EC ratios were higher, averaging approximately 60 and 14 at each site. These results suggest sediment-associated FIB populations may be distinct from those found in the water samples, or at least have internal dynamics independent of water-borne populations. Increases in sediment-associated FIB may be due to in situ population growth and/or increased survival due to changes in environmental parameters (salinity, moisture and nutrient input) resulting from the rain events. Spatial differences in between the two sites may be due to sediment differences such as organic content and finer grain size and/or discrete sources of FIB.     

Identification and chemical characterization of specific organic constituents of petrochemical effluents

Based on extensive GC/MS screening analyses, the molecular diversity of petrochemical effluents discharged to a river in North Rhine-Westphalia was characterised. Within a wide spectrum of organic wastewater constituents, specific compounds that might act as source indicators have been determined. This differentiation was based on (i) the individual molecular structures, (ii) the quantitative appearance of organic compounds in treated effluents and (iii) the information on their general occurrence in the technosphere and hydrosphere. Principally, site-specific indicators have been distinguished from candidates to act as general petrochemical indicators. Further on, monitoring the environmental behaviour of target organic contaminants in an aquatic system shortly after their release into the river allowed a first evaluation of the impact of the petrogenic emission in terms of the quantity and spatial distribution.The identification of petrogenic contaminants was not restricted to constituents of the effluents only, but comprised the compounds circulating in the wastewater systems within a petrochemical plant. A number of environmentally relevant and structurally specific substances that are normally eliminated by wastewater treatment facilities were identified. Insufficient wastewater treatment, careless waste handling or accidents at industrial complexes are potential sources for a single release of the pollutants.This study demonstrates the relevance of source specific organic indicators to be an important tool for comprehensive assessment of the potential impact of petrochemical activities to the contamination of an aquatic environment.     

Part I. Identifying anthropogenic markers in surface waters influenced by treated effluents: a tool in potable water reuse

In potable water reuse, treated wastewater becomes part of the drinking water supply. An important question associated with this practice is whether or not the organic quality of the treated wastewater is chemically different from that of non-human impacted water. This question was addressed in a case study of indirect potable water reuse where the organic matrix of the South Platte River was analyzed upstream and downstream of the discharge of treated wastewater effluent using conventional water quality parameters combined with pyrolysis-GC/MS. Effluent-derived organic material (EfOM) was found to be more aliphatic and had higher organic nitrogen and halogen content compared to organic material derived from "natural" (non-anthropogenic) sources (NOM). Seasonal changes that resulted from the change in the contributions of aquatic and terrestrial sources were not observed in EfOM; but they were strongly observed in NOM under the control of natural processes. Using principal component and factor analyses, the pyrolysis fragments of phenol, alkyl-phenols, and acetic acid were identified as the seasonal indicators for the NOM set of samples. In contrast, benzaldehyde, benzonitrile, chlorobutanoic acid, furancarboxaldehyde, and methylfurancarboxaldehyde were identified as the indicators for wastewater inputs for the EfOM set of samples. Overall, the results from conventional water quality parameters and pyrolysis-GC/MS revealed that: (1) EfOM bears a chemical signature distinct from NOM and (2) under the conditions of this study, EfOM discharged to the South Platte River persisted and controlled organic quality at downstream points.     

Determination of volatile organic compounds in surface waters and treated wastewater in Greece

The occurrence of volatile organic compounds (VOCs) was studied in river water, lake water, seawater and treated wastewater in Greece from October 1998 to September 1999. The determination of 41 VOCs was performed with a Purge and Trap-Gas Chromatography-Mass Spectrometry method. Samples were collected seasonally from 10 rivers, seven lakes, three gulfs and four wastewater treatment plants. In surface water samples, 15 VOCs were detected. In wastewater samples, occurrence of 31 VOCs was observed. The results suggest that not only agricultural and industrial activity within the Greek territory, but also transboundary pollution deriving from neighbouring countries consist important sources of VOCs in surface waters of Greece. However, the measured concentrations did not in any case exceed the guideline values proposed by the EC.     

浐河水质污染特征及水质改善措施分析

针对浐河水体遭受污染问题,通过对浐河水质特征断面的10项指标进行连续监测,分析了浐河水中污染物的组成和水质特征,对污染物的携入方式进行了调查,分析评价了浐河水体污染的原因,并提出了控制浐河水质污染的对策。结果表明,浐河水体中的物理指标水温、p H、重金属指标相对正常;重金属指标中只有少量的Fe、Zn、Cr元素;污染物主要为N、P等营养物质,水体的富营养化程度较为严重;河流水体浊度总体较高且与地表径流存在较高的相关性;污染的主要原因是浐河周边的水厂、污水处理厂所排出污水的点源污染;污染改善措施采用人工湿地、管网改建等适合不同断面特征的控制方式。     

Seasonal variation in accurate identification of Escherichia coli within a constructed wetland receiving tertiary-treated municipal effluent

As the reuse of municipal wastewater escalates worldwide as a means to extend increasingly limited water supplies, accurate monitoring of water quality parameters, including Escherichia coli (E. coli), increases in importance. Chromogenic media are often used for detection of E. coli in environmental samples, but the presence of unique levels of organic and inorganic compounds alters reclaimed water chemistry, potentially hindering E. coli detection using enzyme-based chromogenic technology. Over seven months, we monitored E. coli levels using m-Coli Blue 24((R)) broth in a constructed wetland filled with tertiary-treated municipal effluent. No E. coli were isolated in the wetland source waters, but E. coli, total coliforms, and heterotrophic bacteria increased dramatically within the wetland on all sampling dates, most probably due to fecal inputs from resident wildlife populations. Confirmatory testing of isolates presumptive for E. coli revealed a 41% rate of false-positive identification using m-Coli Blue 24((R)) broth over seven months. Seasonal differences were evident, as false-positive rates averaged 35% in summer, but rose sharply to 75% in the late fall and winter. Corrected E. coli levels were significantly correlated with electrical conductivity, indicating that water chemistry may be controlling bacterial survival within the wetland. This is the first study to report that accuracy of chromogenic media for microbial enumeration in reclaimed water may show strong seasonal differences, and highlights the importance of validation of microbiological results from chromogenic media for accurate analysis of reclaimed water quality.     

Effects of anthropogenic inputs on the organic quality of urbanized streams

Due to arid conditions, population growth, and anthropogenic impacts from agricultural and urban development, wastewater effluent makes up an increasingly large percentage of surface water supplies promoting concerns about the potential ecological and human health effects associated with the organic quality of surface waters receiving treated wastewater discharge. Anthropogenic inputs alter the quality and quantity of organic carbon and also affect the ability of aquatic ecosystems to retain or transform carbon and other nutrients. In this paper, we use pyrolysis-GC/MS (Py-GC/MS) as a tool to examine whether the dissolved organic carbon (DOC) in suburban streams influenced by anthropogenic inputs displays an organic signature that is structurally different from natural organic material (NOM). Py-GC/MS was not only able to differentiate among stream sites that received discharge from upstream wastewater treatment plants and those that did not, but also distinguished stream sites influenced significantly by storm water. Distinct organic signatures were evident in stream waters with upstream wastewater treatment plant discharges regardless of the distance from effluent discharge, indicative of the persistent nature of effluent-derived organic material (EfOM). The pyrolysis fragments of 3-methyl-pyridine, 2-methyl-pyridine, pyrrole, and acetamide were identified as indicators of EfOM, supporting previous research that has suggested that protein and aminosugar derivitives are possible wastewater markers. Furthermore, pyrolysis fragments associated with soil polycarboxylic acids correlated highly with stream sites having the least anthropogenic influences.     

A simple method for the measurement of organic iodine in wastewater and surface water

Total adsorbable organic iodine (TAOI) has been used as a surrogate parameter for X-ray contrast media in municipal wastewater. Available methods require specialized equipment for pyrolyzing these compounds to convert the covalently bound iodine into iodide, which is then measured by ion chromatography. In this study we describe a simple method for liberating iodide from these compounds with Cu(II) and hydrogen peroxide. Concentrations of TAOI were measured in wastewater effluent, surface waters that were expected to be impacted by wastewater, and unimpacted surface waters. TAOI concentrations ranged between 1.9 and 16.3 microg/L I in wastewater with a median of 6.5 microg/L I. The lowest TAOI concentrations consistently were detected in a wastewater treatment plant that apparently had few hospitals within its collection area. In comparison, TAOI concentrations in surface water that was unimpacted by sewage were between 0.3 and 3.5 microg/L I. TAOI concentrations in surface waters that were impacted by sewage were consistent with the expected conservative behavior of TAOI.     

Evaluation of human adenovirus and human polyomavirus as indicators of human sewage contamination in the aquatic environment

Discharge of inadequately treated human wastewater into surface waters used for recreation, drinking water, irrigation and shellfish cultivation may present a public health hazard due to the potential shedding of high concentrations of pathogenic viruses from the human gastrointestinal tract. Human adenovirus (HAdV) and human polyomavirus (HPyV) are ubiquitous in humans and have excellent survival characteristics in the environment, so are potential candidates for indicators of human sewage contamination. Using qPCR assays, the prevalence and quantity of HAdV and HPyV JC and BK were determined in influent and effluent wastewater and receiving waters (river, urban stream, estuarine), then compared with norovirus (NoV) presence, a significant human pathogen which is not necessarily ubiquitously excreted into the environment. HAdV and HPyV were frequently detected in high concentrations in wastewater and wastewater-contaminated waters confirming their use as potential indicators for the presence of human sewage. Overall, there was a correlation between the presence of HAdV and HPyV with NoV but there were some notable exceptions including the higher frequency of NoV compared to HAdV and HPyV in estuarine waters impacted by wastewater overflows. We found that HAdV and HPyV detection by qPCR was a suitable tool for evaluating water quality and that their detection can aid in determining pollution sources, thus providing useful information for health risk assessments.     

Fecal bacteria in the rivers of the Seine drainage network (France): sources, fate and modelling

The Seine river watershed (France) is a deeply anthropogenically impacted area, due to the high population density, intense industrial activities and intensive agriculture. The water quality and ecological functioning of the different rivers of the Seine drainage network have been extensively studied during the last fifteen years within the framework of a large French multidisciplinary scientific program (PIREN Seine program). This paper presents a synthesis of the main data gained in the scope of this program concerning the microbiological water contamination of the rivers of the Seine drainage network. The more common indicator of fecal contamination (fecal coliforms) was mainly used; some complementary works used E. coli and intestinal enterococci as alternative fecal indicators. Point sources (outfall of wastewater treatment plants) and non point sources (surface runoff and soil leaching) of fecal pollution to the rivers of the watershed were quantified. Results showed that, at the scale of a large urbanised watershed as the Seine basin, the input of fecal micro-organisms by non-point sources is much lower than the inputs by point sources. However, the local impact of diffuse non-human sources (especially surface runoff of pastured fields) can be of major importance on the microbiological quality of small headwater rivers. Fecal contamination of the main rivers of the Seine watershed (Seine, Marne, Oise rivers) was studied showing high level of microbiological pollution when compared to European guidelines for bathing waters. The strong negative impact of treated wastewater effluents outfall on the microbiological quality of receiving rivers was observed in different areas of the watershed. Once released in rivers, culturable fecal bacteria disappeared relatively rapidly due to mortality (protozoan grazing, lysis) or loss of culturability induced by stress conditions (sunlight effect, nutrient concentration, temperature). Mortality rates of E. coli were studied in different types of rivers within the watershed showing, in summer conditions, no major difference in the mortality rates in small and large rivers. As a result of these studies, a module describing the dynamics of fecal bacteria has been developed and embedded within a hydro-ecological model describing the functioning of the rivers of the whole watershed (the SENEQUE model). Once validated, such a model can be used for testing predictive scenarios and thus can be a very useful tool for the management of microbiological water quality at the scale of the whole basin.     

Sources of endocrine-disrupting chemicals in urban wastewater, Oakland, CA

Synthetic endocrine-disrupting chemicals (EDCs) have been found in surface waters throughout the United States, and are known to enter waterways via discharge from wastewater treatment plants (WWTPs). Studies addressing EDCs in wastewater do not examine their specific sources upstream of WWTPs. Presented here are results of a pilot study of potential sources of selected EDCs within an urban wastewater service area. Twenty-one wastewater samples were collected from a range of sites, including 16 residential, commercial, or industrial samples, and five samples from influent and effluent streams at the WWTP. Samples were analyzed for the following known and suspected EDCs: five phthalates, bisphenol A (BPA), triclosan, 4-nonylphenol (NP), and tris(2-chloroethyl) phosphate (TCEP), using well-established methods (EPA 625 and USGS O-1433-01). Twenty of 21 samples contained at least one EDC. Phthalates were widely detected; one or more phthalate compound was identified in 19 of 21 samples. Measurement of two phthalates in a field blank sample suggests that the accuracy of sample detections for these two compounds may be compromised by background contamination. Triclosan was detected in nine samples, BPA in five samples, and TCEP in four samples; NP was not detected. The results of this and future source-specific studies may be used to develop targeted pollution prevention strategies to reduce levels of EDCs in wastewater.