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1、Institute of Food Chemistry, Technical Uniuersity of Berlin, Sekr. TIB 4 /3 -1, Gustau -Meyer -Allee 25, 13355 Berlin, GermanyReceived 21 January 2002; received in revised form 24 January 2002; accepted 25 January 2002AbstractThe occurrence and fate of pharmaceutically active compounds （PhACs） in th

2、e aquatic environment has been recognized as one of the emerging issues in environmental chemistry. In some investigations carried out in Austria, Brazil, Canada, Croatia, England, Germany, Greece, Italy, Spain, Switzerland, The Netherlands, and the U.S., more than 80 compounds, pharmaceuticals and

3、several drug metabolites, have been detected in the aquatic environment. Several PhACs from various prescription classes have been found at concentrations up to the g/l-level in sewage influent and effluent samples and also in several surface waters located downstream from municipal sewage treatment

4、 plants （STPs）. The studies show that some PhACs originating from human therapy are not eliminated completely in the municipal STPs and are, thus, discharged as contaminants into the receiving waters. Under recharge conditions, polar PhACs such as clofibric acid, carbamazepine, primidone or iodinate

5、d contrast agents can leach through the subsoil and have also been detected in several groundwater samples in Germany. Positive findings of PhACs have, however, also been reported in groundwater contaminated by landfill leachates or manufacturing residues. To date, only in a few cases PhACs have als

6、o been detected at trace-levels in drinking water samples. 2002 Elsevier Science Ireland Ltd. All rights reserved.Keywords: PhACs; Sewage contaminants; Bank filtration; Surface, ground- and drinking water1. Introduction and backgroundIn recent years, the occurrence and fate of pharmaceutically activ

7、e compounds （PhACs） in the aquatic environment has been recognized as one of the emerging issues in environmental chemistry （Stan and Heberer, 1997; Halling- Srensen et al., 1998; Daughton and Ternes, 1999; Daughton and Jones-Lepp, 2001; Ku mmerer,E -mail address: hebererfoodchemistry.de （T. Heberer

8、）.2001; Verstraeten et al., in press）. The disposal of unused medication via the toilet seems to be of minor importance but many of the pharmaceuti- cals applied in human medical care are not com- pletely eliminated in the human body. Often they are excreted only slightly transformed or even unchang

9、ed mostly conjugated to polar molecules （e.g. as glucoronides）. These conjugates can easily be cleaved during sewage treatment and the origi- nal PhACs will then be released into the aquatic environment mostly by effluents from municipal0378-4274/02/$ - see front matter 2002 Elsevier Science Ireland

10、 Ltd. All rights reserved. PII: S0378-4274（02）00041-3 sewage treatment plants （STPs）. Several investiga- tions have shown some evidence that substances of pharmaceutical origin are often not eliminated during waste water treatment and also not biode- graded in the environment （Ternes, 1998a; Zwiener

11、 et al., 2000; Heberer, in press）. Under recharge conditions, residues of PhACs may also leach into groundwa- ter aquifers （Verstraeten et al., in press）. Thus, they have already been reported to occur in ground- and drinking water samples from water works using bank filtration or artificial ground-

12、 water recharge downstream from municipal STPs （Heberer and Stan, 1997; Heberer et al., 1997; Heberer, in press）.The presence of PhACs from human medical care in groundwater may, however, also be caused by other sources such as landfill leachates （Eckel et al., 1993; Holm et al., 1995; Ahel and Jeli

13、cic, 2001） or manufacturing residues （Red- dersen et al., submitted）. Nowadays, and espe- cially in the industrialized countries, strong regulations and advanced manufacturing prac- tices shall prevent such spills. In the past, regula- tions were not as strong and in several cases therelease of prod

14、uction residues was either tolerated or even accepted. Such spills could result in Su- perfund sites which may be responsible for to- days findings of PhAC residues in the environment （Reddersen et al., submitted）. But the occurrence of pharmaceutical residues in the environment may also be caused b

15、y agriculture applying large amounts of PhACs as veterinary drugs and feed additives in livestock breeding. Fig. 1 shows possible sources and pathways for the occurrence of PhAC residues in the environ- ment.Three years ago, Daughton and Ternes （1999） wrote a comprehensive review on PhACs and person

16、al care products （PCPs） in the environment and also mentioned some future research needs. In the meantime, some new data on the occur- rence, fate, and removal of PhACs in the aquatic environment have been published. This paper gives an overview on the current state of the scientific knowledge. It i

17、s restricted to PhACs originating from human application and compiles most recent data and information from some scientific studies and projects carried out in Eu- rope and the U.S.Fig. 1. Scheme showing possible sources and pathways for the occurrence of pharmaceutical residues in the aquatic envir

18、onment.2. Occurrence of PhACs in sewage, surface, ground- and drinking waterThe occurrence of the PhACs in the aquatic environment has been investigated in several stud- ies in Austria, Brazil, Canada, Croatia, England, Germany, Greece, Italy, Spain, Switzerland, The Netherlands and the U.S. More th

19、an 80 PhACs from various prescription classes have been de- tected up to the g/l-level in sewage, surface and groundwater.2.1. Analgesics and anti -inflammatory drugsThis section compiles data from PhACs primar- ily used as pain killers. Most analgesics also have anti-inflammatory and antipyretic pr

20、operties. Large amounts of pain killers are prescribed in human medical care but often they are sold at much higher quantities without prescription as so-called over-the-counter （OTC） drugs. In Ger- many, prescription data is accessible via the health insurance companies but only rough esti- mations

21、 are possible for those amounts of drugs donated as medication in hospitals or sold as OTC drugs （Stan and Heberer, 1997）.Acetaminophen （paracetamol） and acetylsaly- cylic acid （ASA） are the two most popular pain killers mainly sold as OTC drugs. In Germany, the total quantities of ASA sold per year

22、 have been estimated at 500 tons （Ternes, 2001）. Nev- ertheless, other analgesics such as diclofenac or ibuprofen sold in Germany at annual quantities of approximately 75 and 180 tons, respectively （Ter- nes, 2001）, have been recognized as being more important for the water-cycle. ASA was detected a

23、t a median concentration of only 0.22 g/l in sewage effluents in Germany （Ternes, 1998a）. In the same study, the median concentration of ASA in surface water samples was below the detection limits.As a pro-drug, ASA is, however, easily de- graded by deacetylation into its more active form salicylic

24、acid and into two other metabolites namely ortho -hydroxyhippuric acid and the hy- droxylated metabolite gentisic acid. Ternes （1998a）, Ternes et al. （1998b） detected salicylic acid, ortho -hydroxyhippuric acid and gentisic acidin sewage influent samples at concentrations up to54, 6.8, and 4.6 g/l,

25、respectively. Ternes et al. （1998b） observed that all three compounds were efficiently removed by the municipal STPs and only salicylic acid was detected at very low con- centrations in sewage effluents and also in rivers. Heberer （in press） also reported average concen- trations of only 0.04 g/l fo

26、r salicylic acid in sewage effluents. But in this study, the average influent concentrations of 0.34 g/l were relatively low, too. On the other hand, much higher concen- trations of salicylic acid up to 13 g/l were de- tected in sewage effluents in Greece and Spain （Farre et al., 2001; Heberer et al

27、., 2001a）. Residues of salicylic acid do not necessarily have to derive from ASA. Other sources such as the use of salicylic acid as keratolytic, dermatice, and preservative of food or its natural formation are even more likely to be responsible for the occur- rence of this compound in the aquatic e

28、nviron- ment （Heberer, in press）.The other most prominent pain killer acetamin- ophen is also easily degraded and removed by the STPs. In investigations of sewage effluents and rivers in Germany, acetaminophen was only de- tected in less than 10% of all sewage effluents and not detected in river wat

29、er （Ternes, 1998a）. In investigations of 142 streams in the U.S. suscepti- ble for contaminations by municipal sewage effluents, Kolpin et al. （in press） detected acet- aminophen in 17% of all samples at maximum concentrations up to 10 g/l.Approximately, 75 tons of the prescription drug diclofenac a

30、re annually sold in Germany （Ternes,2001）. In long-term monitoring investigations of sewage and surface water samples from Berlin, Germany, Heberer et al. （in press b） identified diclofenac as one of the most important PhAC present in the water-cycle. Average concentrations of 3.02 and 2.51 g/l were detected in the influents and effluents of the municipal STPs, respectively. This low removal rate of only 17% demonstrates the persistence of diclofenac in the STPs and was also r