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You have full access to this open access article. Despite the fact that there are tens of thousands of thermal baths in existence, knowledge about the occurrence of pharmaceutically active compounds PhACs in untreated thermal wastewater is very limited. Because used thermal water is typically legally discharged into surface waters without any treatment, the effluent poses environmental risks for the receiving water bodies. The aim of this study was to show the occurrence patterns and spatiotemporal characteristics of PhACs in thermal wastewater. Six thermal water outflows of different thermal baths were tested in different seasons in the Budapest metropolitan region Hungary , and diurnal analysis was performed. After solid-phase extraction, the samples were analysed and quantified by coupling supercritical fluid chromatography and mass spectrometry to perform simultaneous multi-residue drug analysis. The results confirm that water discharge pipes directly transport pharmaceuticals into surface water bodies; 34 PhACs were measured to be over the limit of quantification at least once, and 21 of them were found in more than one water sample. The local anaesthetic drug lidocaine, antiepileptic carbamazepine, analgesic derivative tramadol and illicit drug cocaine were detected in more than half of the samples. As demonstrated by the diurnal fluctuation, drug contamination of thermal waters can significantly vary, even for similar types of baths; furthermore, the quantity and types of some pollutants rapidly change in the discharged thermal wastewater. Surface waters are polluted by pharmaceutically active compounds PhACs , which are regarded as widespread contaminants Aus der Beek et al. The negative impact of certain PhACs, such as endocrine-disrupting chemicals e. This problem is exacerbated by the fact that some of the more persistent and slowly decomposing agents reach the drinking water supply Leung et al. These PhACs consequently appear in the human food chain Carter et al. The European Union has referred to the Water Framework Directive to establish a watchlist of the most important contaminants that need to be monitored. In addition to communal sewage Kasprzyk-Hordern et al. Thermal spa water that has been discharged into natural waters is also considered to be a legal source of contamination. Thermal water used for bathing, unlike that utilized for purposes of energetics, must not be reinjected into the aquifer because of the presence of bacteria and other contaminants, therefore it is typically discharged into surface receivers. Although, in general, used thermal water is known to have a potentially harmful environmental impact e. A related test was carried out by Avar et al. Figures released by the Global Wellness Institute show the extent to which the thermal mineral springs industry contributes to the more than 4. Thermal spas that use water from hot springs or drilled wells can be found in nearly countries. Several thousand establishments discharge untreated thermal water into natural receivers, thereby harming the vulnerable ecosystem. Earlier research has proven that a significant amount of PhACs enter swimming pool water during use. Most of this contamination is the result of unhygienic behaviour e. Other bodily fluids, such as perspiration due to warm water, can also play an important role Kanan and Karanfil ; Keuten et al. To date, PhAC monitoring has mainly been performed using the water of swimming pools with water recirculation technology, and where the water is disinfected with chlorine and undergoes further treatment before being partially discharged into the communal sewage system; thus, this water does not reach natural waters directly. Ekowati et al. Fantuzzi et al. They also found 11 of the 48 monitored PhACs; regarding illicit drugs, only cocaine and its metabolites were identified in nine swimming pools. Disinfection and chlorination in swimming pools help to keep certain pharmaceutical substances e. Alternatively, water recirculation technology can also influence the amount of certain PhACs, as some of the water remains in the system for longer time periods, i. In the case of swimming pools, the incoming tap water may already be contaminated by PhACs Suppes et al. Thus, to preserve its therapeutic effects, the water cannot be diluted with municipal water and cooled, and it cannot be disinfected like the water of swimming pools, therefore, there is a larger amount and variety of active microbial life in thermal water as compared to treated water. Thermal pools typically have a filling and draining system, or an instantaneous system. The used thermal water is continuously and directly discharged into natural waters without any further treatment; this means that the PhACs that it may contain are also discharged into natural waters Farsang et al. In countries in temperate and cold zones, where most thermal spas can be found, spa use is more seasonal than swimming pool use, and this impacts the potential contamination of the outflowing water CP , Ferrante et al. Tourist influx in the summer causes the number of visitors to increase, and can also profoundly impact contamination levels. Tourists from abroad are overrepresented in summer visitors, whereas the ratio of elderly locals is higher during the winter HCSO Thus, it is necessary to determine the effects of wellness and therapeutic tourism on PhAC loads in thermal spas. Hungary, particularly its capital, Budapest, has a number of thermal spas, some of which are internationally renown Erfurt-Cooper and Cooper Although there are risks attributed to the presence of PhACs and illicit drugs in surface waters, and there are many thermal bath outflows all over the world, the contribution of thermal spas has not yet been investigated. The analysis summarized in this paper was performed within the framework of a 3-year-long research project supported by the Hungarian government that examined PhAC contamination in the Budapest metropolitan region. Water samples were collected from the open-ended water discharge pipes of six Hungarian thermal baths in and around Budapest from which effluent is directly transported to surface waters. Each of these baths have drilled thermal wells, and the sampled water outflows were located m from the baths. In this study, the baths were blindly marked as A through F. Spas A, B and C are located in the central part of Budapest; their number of visitors exceeds , per year. They are open to tourists throughout the entire year, and, in addition to the pools with certified therapeutic water, they also offer cold-water pools for recreational purposes. Spas D, E and F are located in the outskirts and suburbs of Budapest. They are also open throughout the entire year, and, like Spas A-C, they have pools with therapeutic water, and cold-water pools. However, these spas are smaller, and receive ,, visitors per year HCSO The thermal pools of the sampled spas are visited by more than people in a single day in the winter, at the larger spas, the number of thermal pool users exceeds people per day in summer. The sampled water pipes directly transport the used thermal water collected from the thermal pools to surface waters. The water from the discharge pipes is not directly related to the nominal capacity of thermal wells, and some thermal spas have more than one water outflow. Overall, the water chemistry-related parameters pH, conductivity, mineral content of the sampled water were consistent with the official data on the certified thermal waters, as provided by each of the spas; therefore, the volume of non-thermal-pool water in outflow pipes, such as water sourced from non-thermal pools, was, with one exception, negligible at the time of sampling. The sampling was always performed between the time period of and , as the contaminated thermal water was presumed to be passing through the discharge pipes by this time because of the filling and draining system. However, the off-season sample from Spa B was corrupted during laboratory preparations, causing the measured values to be unreliable; therefore, they were not used in the analysis. Thus, 17 water samples were used in the seasonal analysis. It was not feasible to sample Spas A and B on the same day because of logistical problems, namely - parallel with diurnal monitoring at Spa A - other spas were also sampled. Therefore, diurnal samples were obtained from Spa B during a large-scale international music festival. Because the admission fee to the festival included free access to the spa, there was a large number of foreign visitors. A total of seven 26 July , Thursday, h and four 12 August , Sunday, h samples were collected from Spas A and B, respectively; note that an unplanned additional sample was obtained from Spa A because the composition of the discharged water was visibly observed to suddenly change. Thus, diurnal fluctuations were analysed as based on 12 samples from two locations. Spa B has two thermal water outflows, and the water from the other discharge pipe is used by a different institution for heating and irrigation; therefore, the sampled outdoor outflow was not always operating at full capacity. Consequently, four samples were collected per day, at times when the output water pressure was high for longer periods of time. All samples 2. The water was sampled at the joint, open-ended water discharge pipes of the selected thermal spas; thus, the samples reflect all the thermal water pools of each spa. The samples collected to measure the levels of organic PhACs were preserved in formic acid at a pH level below 2. To determine the basic hydrochemical properties, 0. To assess carbon and nitrogen content, 50 ml of each sample was collected and preserved in formic acid at a pH level below 2. To determine the heavy metal content, 15 mL of water was collected in a centrifuge tube; then, the sample was filtered by using a 0. The temperature, conductivity and redox potential of the outflowing water were simultaneously measured as each sample was collected. All of these variables were also measured in the laboratory, Table S1 provides the corresponding values. Details of the sample preparation process and setup for analysis have been previously reported Maasz et al. To summarize, the water samples were acidified with formic acid and spiked with corresponding mass-labelled internal standard to the sample quantification and compensation the matrix effect and chemical losses during the sample preparation. The sample was fully prepared within 24 h from the sampling. The evaporated by nitrogen gas stream eluates were reconstituted with acetonitrile and transferred to vials within 30 days. Derivatization by dansyl-chloride of steroid agents was performed to reach the appropriate sensitivity. Data were recorded in three technical replicates by MassLynx software V4. Separation of compounds was performed on a 3. The MS measurement was performed in positive ion mode. The electrospray ionization source was operated at a spray voltage of 3 kV in both positive and negative ion modes, and at a cone voltage of 30 V. The samples were used to identify PhACs, including pharmaceutical derivatives, illicit drugs and alkaloids such as cocaine and caffeine. The agents to be analysed were determined based on Hungarian consumption data and the toxicological effect profile. The PhACs were categorized into the following nine groups for analysis: 1 antidepressants, 2 antiepileptics, 3 anxiolytics, 4 cardiovascular drugs, 5 hormones and derivatives, 6 stimulants, psychedelics, hallucinogens and their metabolites, 7 nonsteroidal anti-inflammatory drugs NSAIDs , 8 anaesthetics and analgesics, 9 other including alkaloids, such as caffeine. The groups can be directly compared to the classification systems described in the relevant literature on PhAC contamination of swimming pools e. Thirty-four of the monitored PhACs were found to exceed their respective LOQ value at least once in one of the water samples Table S3 ; additionally, 21 of the PhACs were detected in more than one sample. There are significant differences in the frequency of occurrence and concentration levels of the detected PhACs Table 1. The average concentration of caffeine, i. It is present in various food items and health supplements e. Note that, whether a PhAC is prescription or non-prescription does not impact the frequency of its occurrence in the samples. For some active substances e. These findings can be used to compare the proportions of the different groups of PhACs Fig. Although hormones were the most frequent, the occurrence of hallucinogenic drugs was also higher than their ratio within then monitored PhACs. The increased proportion of antiepileptics e. Moreover, as with swimming pool water Ekowati et al. In contrast, anxiolytics and anaesthetics were not observed in high concentrations, although some of their representative compounds, such as tramadol and lidocaine, were detected in many of the samples. The latter two PhACs were also found to be highly persistent, as reported by Bollmann et al. It should be noted that neither the occurrence or concentration of PhACs was found to be related to the chemical properties of the spa water Table S1. This also suggests that PhAC content is independent of the water source, and that the analysed PhACs are chemically stable enough to not interact with the high solute components of the thermal water. Regarding the PhACs that were detected only once, Spa B, which is very popular with foreign visitors, exhibited the highest rate of occurrence of single detection four of six samples. Accordingly, the lowest occurrence three of 10 samples was found at Spa A, which also has a high number of domestic and international visitors; one antidepressant bupropion and two cardiovascular drugs betaxolol, verapamil were detected only once there. Alternatively, one antidepressant tiapride and one anxiolytic cinolazepam were found to be unique agents in three samples from Spa C. Although there were single occurrences of antidepressants at all of the international baths, this was not the case for any of the local spas. Note that the above-mentioned PhACs were not included in further analysis since they were only found in one sample. Seasonal analysis of the 17 samples collected from all outflows revealed hormones to be the most prevalent group in the summer. Of the eight detected hormones, only testosterone was found to occur in every season; hormones related to contraceptives were detected in all of the summer samples Fig. This is consistent with the empirical fact that young women tend to visit thermal baths more often during their summer holiday HCSO Alternatively, drugs used for the treatment of cardiovascular disorders e. Two of the four cardiovascular PhACs were not detected in the high-tourist season, and the remaining two were only found in a few samples. Various PhACs, such as the anaesthetics tramadol and lidocaine, were found in most of the water samples, regardless of the season. The possible reasons for the high proportion and persistence of antiepileptics have been discussed above. It should be noted that the absence of lamotrigine in the summer samples was unexpected. This phenomenon cannot be explained using the currently available results; thus, its interpretation necessitates further investigation. As was observed in the results from swimming pools in Italy Fantuzzi et al. This finding indicates that cocaine consumption is also widespread among the local population, as Thomas et al. However, the absolute peaks were observed in the summer at spas frequented by tourists Table S3. Regarding geographical variation, research has shown that, as compared to spas mainly visited by the locals, nearly all PhACs occur more frequently at international thermal spas within the city centre, and that the average concentrations of the detected PhACs are higher, especially in the cases of cocaine and certain hormones. The exceptions are the two forms of oestrogen and the cardiovascular drug propafenone, which occur more frequently at spas located outside of the city Fig. Eight water samples were collected for Spa A diurnal analysis, and only 15 of the possible PhACs were detected Fig. It should be noted that nearly half of the identified PhACs were hormones, and that the occurrence and non-occurrence of many other agents were atypical. EE2 was identified at high concentrations average: The oestrogens were found to dynamically fluctuate, exhibiting no apparent patterns. Different types of hormones testosterone, progesterone, levonorgestrel were only occasionally measured at low concentrations. Of the anaesthetics, lidocaine was dominant in terms of frequency and concentration. Additionally, the steadily high concentration of EE2 indicates persistent contamination throughout the entire day. It is also noteworthy that the typically frequently detected carbamazepine Aus der Beek et al. Although they were detected in only three samples, alkaloids were found to have the highest concentration, i. Additionally, although cocaine was detected in only two of the eight samples, its metabolite benzoylecgonine was present in five samples. The next highest peaks occurred in the noon and midnight samples. The sample, and the sample containing the murky water observed at according to general water chemistry, this sample was due to pool rinsing , were found to have the fewest PhACs, even though both samples also contained lidocaine and EE2. Regarding the diurnal analysis for Spa B, which has international visitors, of the 15 PhACs that were found, only one-third of them were hormones Fig. Some of the detected hormones were also found at Spa A e. Additionally, only the concentration of E1 was stable, as the concentrations of the other hormones fluctuated throughout the day; specifically, their occurrence was inconsistent. Because there was no accumulation, the persistent presence of these compounds indicates continuous and largely invariable levels of contamination. Although Fantuzzi et al. Thus, the persistently high concentration as a result of continuous contamination is rather relevant. It should be noted that, although the cocaine metabolite benzoylecgonine was detected in several samples from Spa A under the condition of low cocaine occurrence, this metabolite was not detected at Spa B. This is unexpected, as benzoylecgonine is much more stable than cocaine and the concentration of the former is generally higher McCall et al. The background of this finding has been unknown yet, presumably, some other sources of cocaine other than human metabolism might have been present in the thermal water of Spa B. Regarding daily fluctuation, the number and concentrations of PhACs were found to reach their peak in the early afternoon. Weng et al. However, this theory is not fully supported by the findings of this study; although one sample was found to have a high concentration of caffeine, it was absent in four of the samples note: eight total samples. This supports the view that the measurements from swimming pools with strongly chlorinated water and water recirculation systems can only be indirectly compared to thermal spa systems. Analysing all of the samples off-season, pre-season, main season and diurnal monitoring from the two international spas, which are similar in size and target the same type of visitors, revealed that the frequency and concentration of carbamazepine are constantly low at Spa A, unlike those at Spa B. However, as compared to Spa B, the frequent occurrence of hormones and constant presence and high concentration of EE2 at Spa A are relevant. The findings of this study reveal that significant amounts of PhACs enter thermal waters through the human body of visitors, and are then directly transported to surface waters. The measured concentrations indicate that thermal spas are not the main sources of contamination even though the emission of PhACs can still be relevant. The study itself, and the interpretation of the results, have some constraints. For example, the exact number, age and type local inhabitants vs. Furthermore, no previous studies, to which the results of this study can be compared, could be found. Nevertheless, our results can facilitate accurate assessment of the environmental pollution caused by DTWW, they also suggest the following:. The concentrations and frequency of occurrence of PhACs contaminating the environment could be seasonal and dependent on the type of visitors. Many types of visitors use illicit drugs, as they were detected at international and local spas. However, although the concentrations of these PhACs increased at the time of an international music festival, there was no sudden change in the concentrations of other substances. As compared to the corresponding swimming pool measurements, PhACs remain in thermal pools for shorter periods of time, and at lower concentrations, because of the different filling and draining water treatment processes; furthermore, the types of PhACs can significantly change within a few hours in a thermal pool. Thus, the sampling time at thermal spas can be a critical determining factor. However, the concentrations of carbamazepine, diclofenac and cocaine, which are usually ubiquitous and very harmful to the environment, were negligible at one of the sampled spas, whereas the occurrence and concentrations of certain hormones were extremely high. Because the treatment and discharge technology and the type of visitors are not sufficient to justify such significant differences, it is likely that different microbial compositions and activity levels are contributing factors. Further research is required to better support the development of environmental risk reduction procedures. Environ Toxicol Chem 35 4 Drug Test Analysis 8 1 Environ Sci Pollut Res Sci Total Environ J Hazard Mater J Agric Food Chem 62 4 Water Res Czech Journal of Tourism 6 1 Article Google Scholar. Environ Health Perspect 6 Curr Envir Health Rpt 1 2 Tour Manag Perspect Environ Sci Pollut Res 23 14 Erfurt-Cooper P, Cooper M Health and wellness tourism: spas and Hot Springs. Channel view publications, Bristol, UK. Etchepare R, van der Hoek JP Health risk assessment of organic micropollutants in greywater for potable reuse. EU Environ Eng Manag J 14 5 Tour Manag Global Wellness Economy Monitor Global wellness institute, global wellness economy monitor, October HCSO Annual reports on turnover of baths. Hungarian Central Statistical Office, Heberer T Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicol Lett Chemosphere Kanan A, Karanfil T Formation of disinfection by-products in indoor swimming pool water: the contribution from filling water natural organic matter and swimmer body fluids. Kim B-H Ecology of a cyanobacterial mat community in a Korean thermal wastewater stream. Aquat Ecol Water Sci Technol 67 6 Trends Anal Chem Env Poll B Springer Verlag, Berlin-Heidelberg, Germany, Google Scholar. Environ Int Environ Health Perspect 7 Environ Sci Technol Lett 4 4 Compr Anal Chem Ecotoxicol Environ Saf Forensic Sci Int Environ Sci Technol Environ Pollut Hun Geo Bull A comprehensive identification of disinfection by-products and assessment of mutagenicity of chlorinated and brominated swimming poolwater. Environ Health Perspect 11 Roberts PH, Thomas KV The occurrence of selected pharmaceuticals in wastewater effluent and surface waters of the lower Tyne catchment. Smith, M. Health, tourism and hospitality: spas, wellness and medical travel. Book Google Scholar. J Water Health 15 5 Acta Microbiol Immunol Hung 63 2 Environ Sci Pollut Res 23 7 Environ Sci Technol Lett 1 12 Download references. You can also search for this author in PubMed Google Scholar. Correspondence to Attila Csaba Kondor. The authors declare that they have no known competing financial interests or personal relationship that could have appeared to influence the results presented in this paper. Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations. Reprints and permissions. Jakab, G. Thermal baths as sources of pharmaceutical and illicit drug contamination. Environ Sci Pollut Res 27 , — Download citation. Received : 13 July Accepted : 25 September Published : 02 December Issue Date : January Anyone you share the following link with will be able to read this content:. Sorry, a shareable link is not currently available for this article. Provided by the Springer Nature SharedIt content-sharing initiative. Download PDF. Abstract Despite the fact that there are tens of thousands of thermal baths in existence, knowledge about the occurrence of pharmaceutically active compounds PhACs in untreated thermal wastewater is very limited. First report on the occurrence of pharmaceuticals and cocaine in the coastal waters of Santa Catarina, Brazil, and its related ecological risk assessment Article 22 April Occurrence of illicit drugs and selected pharmaceuticals in Slovak municipal wastewater Article 17 August Use our pre-submission checklist Avoid common mistakes on your manuscript. Introduction Surface waters are polluted by pharmaceutically active compounds PhACs , which are regarded as widespread contaminants Aus der Beek et al. Materials and methods Sampling properties Water samples were collected from the open-ended water discharge pipes of six Hungarian thermal baths in and around Budapest from which effluent is directly transported to surface waters. PhAC analysis Details of the sample preparation process and setup for analysis have been previously reported Maasz et al. Results and discussion General results Thirty-four of the monitored PhACs were found to exceed their respective LOQ value at least once in one of the water samples Table S3 ; additionally, 21 of the PhACs were detected in more than one sample. Full size image. Conclusions The findings of this study reveal that significant amounts of PhACs enter thermal waters through the human body of visitors, and are then directly transported to surface waters. Nevertheless, our results can facilitate accurate assessment of the environmental pollution caused by DTWW, they also suggest the following: The concentrations and frequency of occurrence of PhACs contaminating the environment could be seasonal and dependent on the type of visitors. Hungarian Central Statistical Office, Heberer T Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. View author publications. Ethics declarations Declaration of interest The authors declare that they have no known competing financial interests or personal relationship that could have appeared to influence the results presented in this paper. Electronic supplementary material. About this article. Cite this article Jakab, G. Copy to clipboard. Search Search by keyword or author Search. Navigation Find a journal Publish with us Track your research.