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The global consumed volumes of carbamazepine and diclofenac can be estimated by the dose per capita, with differences between developed and developing countries

Carbamazepine and diclofenac: removal in wastewater treatment plants and occurrence in water bodies.

Chemosphere, no. 8 (2008): 1151-1161

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摘要

In the aquatic environment, pharmaceuticals have been widely found. Among them, carbamazepine and diclofenac were detected at the highest frequency. To evaluate the worldwide environmental impacts of both drugs, their global consumption volumes are estimated, based on the dose per capita. The metabolites of these pharmaceuticals are also ...更多

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简介
  • Pharmaceuticals have been widely found. Among them, carbamazepine and diclofenac were detected at the highest frequency.
  • The removal efficiencies and mechanisms of both drugs in the wastewater treatment plants (WWTPs) are discussed with the actual state of knowledge
  • The occurrences of both drugs are examined in various water bodies including WWTP effluents, surface waters, groundwater and drinking water.
  • If the pharmaceutical residues are not effectively removed from the water by the drinking water treatment facilities, the pharmaceuticals are unintentionally consumed by humans
  • One such example is clofibric acid, a lipid regulator metabolite that was found in tap water in Berlin at concentrations between 10 and 165 ng LÀ1 (Stan et al, 1994).
  • The authors propose a simplified estimate of the global pharmaceutical consumption with the following assumptions: (a) pharmaceutical
重点内容
  • In the aquatic environment, pharmaceuticals have been widely found
  • Pharmaceutical residues can be introduced into groundwater through surface water filtration, leakage, groundwater recharge, etc
  • If the pharmaceutical residues are not effectively removed from the water by the drinking water treatment facilities, the pharmaceuticals are unintentionally consumed by humans
  • The global consumed volumes of carbamazepine and diclofenac can be estimated by the dose per capita, with differences between developed and developing countries
  • Some metabolites of diclofenac that are recovered from urine represent a higher proportion of an oral dose than unchanged diclofenac and could build up at higher concentrations at the wastewater treatment plants (WWTPs) as well
  • The removal efficiency of carbamazepine is less than 10% in most cases while that of diclofenac varies from 0% to 80%, depending on the operation conditions of WWTPs
结果
  • Investigations found that carbamazepine is persistent and its removal efficiencies by the WWTPs are mostly below 10% (Fig. 2).
  • In the whole range of SRT plotted, the removal efficiency of carbamazepine is no more than 30%
  • In most cases, it is below 10%, and is clearly independent of the SRT.
  • The removal efficiency of carbamazepine is less than 10% in most cases while that of diclofenac varies from 0% to 80%, depending on the operation conditions of WWTPs. The authors appreciate the anonymous reviewers whose excellent comments significantly improved the quality of this manuscript
结论
  • Conclusions and outlook

    The global consumed volumes of carbamazepine and diclofenac can be estimated by the dose per capita, with differences between developed and developing countries.
  • Some metabolites of diclofenac that are recovered from urine represent a higher proportion of an oral dose than unchanged diclofenac and could build up at higher concentrations at the WWTPs as well.
  • Studies on those metabolites in the environment are insufficient
总结
  • Introduction:

    Pharmaceuticals have been widely found. Among them, carbamazepine and diclofenac were detected at the highest frequency.
  • The removal efficiencies and mechanisms of both drugs in the wastewater treatment plants (WWTPs) are discussed with the actual state of knowledge
  • The occurrences of both drugs are examined in various water bodies including WWTP effluents, surface waters, groundwater and drinking water.
  • If the pharmaceutical residues are not effectively removed from the water by the drinking water treatment facilities, the pharmaceuticals are unintentionally consumed by humans
  • One such example is clofibric acid, a lipid regulator metabolite that was found in tap water in Berlin at concentrations between 10 and 165 ng LÀ1 (Stan et al, 1994).
  • The authors propose a simplified estimate of the global pharmaceutical consumption with the following assumptions: (a) pharmaceutical
  • Objectives:

    The objectives of this paper are to summarize the current body of knowledge on both drugs, including their consumption, metabolism, removal in wastewater treatment plants, occurrences in all types of water bodies, and their ecotoxicity.
  • Results:

    Investigations found that carbamazepine is persistent and its removal efficiencies by the WWTPs are mostly below 10% (Fig. 2).
  • In the whole range of SRT plotted, the removal efficiency of carbamazepine is no more than 30%
  • In most cases, it is below 10%, and is clearly independent of the SRT.
  • The removal efficiency of carbamazepine is less than 10% in most cases while that of diclofenac varies from 0% to 80%, depending on the operation conditions of WWTPs. The authors appreciate the anonymous reviewers whose excellent comments significantly improved the quality of this manuscript
  • Conclusion:

    Conclusions and outlook

    The global consumed volumes of carbamazepine and diclofenac can be estimated by the dose per capita, with differences between developed and developing countries.
  • Some metabolites of diclofenac that are recovered from urine represent a higher proportion of an oral dose than unchanged diclofenac and could build up at higher concentrations at the WWTPs as well.
  • Studies on those metabolites in the environment are insufficient
表格
  • Table1: Physical, chemical and pharmacological properties of carbamazepine and diclofenac
  • Table2: Annual consumed volumes of carbamazepine (CBZ) and diclofenac (DFC) in some countries and estimation of their global volumes
  • Table3: Toxicity data of carbamazepine and diclofenac in the literatures
Download tables as Excel
基金
  • Yongjun Zhang is supported by a scholarship from the State of Berlin under the program of Nachwuchsförderungsgesetz (NaFöG)
研究对象与分析
samples: 26
WWTP effluents are important gateways where carbamazepine can enter the water cycle. In a survey conducted by Ternes (1998), carbamazepine was detected in all 30 WWTP effluents with a 90percentile of 3700 ng LÀ1 and in 24 of 26 samples from 20 rivers with a 90-percentile of 820 ng LÀ1. The maximum concentration of carbamazepine in WWTP effluents was 6300 ng LÀ1, which was also the maximum detected concentration of all 32 drugs in the survey

inhabitants: 96000
Hospital wastewater is another contributor to pharmaceutical residues in the sewage effluent due to the high consumption density of some drugs in the hospital. Heberer and Feldmann (2005) investigated a municipal WWTP that treats both household sewage (96 000 inhabitants) and five hospital effluents (2339 beds together) and found that 26% and 17% of the total carbamazepine and diclofenac, respectively, in the WWTP was from the hospitals. Considering all of other pharmaceuticals largely used in hospitals, treating hospital wastewaters separately from household effluents could prevent pharmaceutical residues entering the aquatic environment to some extent

samples: 43
Diclofenac. In a survey by Ternes (1998), diclofenac was detected in all 49 WWTP effluents with a 90-percentile of 1600 ng LÀ1 in all 43 samples from 22 rivers with a 90-percentile of 800 ng LÀ1. Paxéus (2004) detected diclofenac in all ten sampled WWTP effluents in the five EU countries he sampled

引用论文
  • 1061 915 BLAC (2003)
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  • 151 n.a. Thacker (2005)
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  • DPC—dose per capita; England population – UK; National Statistics (2001); EU population – EUROPA (2006); other populations – UN (2005).
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  • consumption is not balanced between developing countries and developed countries because of economic, medical, and culture differences; (b) the annual dose per capita (DPC) is the same in developing countries and also same among developed countries; (c) developing countries only consume 20% of the global pharmaceuticals despite accounting for approximately 80% of the world’s population (Cohen et al., 2005). The DPC of a drug in a country is calculated by dividing the annual consumption of the drug by its population. The average DPC of a drug in the developed countries is calculated by dividing the volumes consumed in the countries listed in Table 2 by the sum of their populations. The global consumption is estimated to be: Average DPI of developed countries  ðworld population  0:2Þ 0:8
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  • The estimated global consumptions of carbamazepine and diclofenac are shown in Table 2. Since the DPC of carbamazepine in the USA is significantly lower than that of other countries, two average developed country DPCs are calculated: one including the USA and the other excluding the USA. Their mean value is accepted as the final DPC of developed countries and is used to the estimate. The globally consumed volumes of carbamazepine and diclofenac are estimated to be 1014 tons and 940 tons per year, respectively. Both estimated values are in accordance with IMS Health data: 942 tons of carbamazepine and 877 tons of diclofenac were sold in 2007 in 76 major countries which are believed to account for 96% of the global pharmaceutical market.
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  • (28% in faeces plus 1% in urine). Furthermore, CBZ-diol is also a metabolite of oxcarbazepine which is a derivative of carbamazepine, with an extra oxygen atom on the dibenzazepine ring (Theisohn and Heimann, 1982). Therefore, one may expect to observe a higher concentration of CBZ-diol in water bodies. Unfortunately, limited studies have been conducted on those metabolites in the aquatic environment to date. Miao and Metcalfe (2003) and Miao et al. (2005) investigated the occurrences of carbamazepine metabolites in a WWTP effluent and a surface water. They observed that the concentration of CBZ-diol was approximately three times that of carbamazepine. Therefore, more studies should be conducted on the environmental fate of carbamazepine metabolites.
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  • 4. Removal in WWTP Most WWTPs use activated sludge processes wherein microorganisms are applied to mineralize the pollutants to water and carbon dioxide, or degrade them to acceptable forms. Pollutants can also be removed from water by stripping into air or by sorption onto sludge that is regularly discharged. Some substances may be subject to phototransformation. Therefore, the removal of pharmaceutical residues in activated sludge processes includes four mechanisms: biotransformation, air stripping, sorption and phototransformation. However, the project of POSEIDON found that a Henry coefficient more than 3 Â 10À3 (–) was required for the significant stripping in a bioreactor with fine bubble aeration (POSEIDON, 2006). Accordingly, the removal of carbamazepine and diclofenac (Henry coefficients: 1.09 Â 10À5, 4.79 Â 10À7 (–), respectively) by air stripping is limited and thus is omitted from the following discussion.
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  • The sorption behavior of diclofenac onto sludge is similar to that of carbamazepine. Its water–sludge distribution coefficient is 16 L kgÀSS1 (Ternes et al., 2004). Although larger than that of carbamazepine, the coefficient is still too low for significant attachment onto the sludge. Diclofenac and carbamazepine were classified in the same biodegradability group of below 0:1 L kgÀSS1 dÀ1 when considering a first order degradation constant (kbiol) in WWTPs (Joss et al., 2006). Quintana et al. (2005) investigated the biodegradation of diclofenac by activated sludge. They found no transformation of diclofenac over 28 days, neither when diclofenac was the sole source of carbon (20 mg LÀ1), nor when it was dispersed in milk powder (2 mg LÀ1 per 50 mg LÀ1). The poor biodegradation of diclofenac was confirmed recently by Kimura et al. (2007) in batch elimination experiments using sludge from WWTPs and MBR, respectively.
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  • An interesting phenomenon is the increased effluent concentrations of carbamazepine (Clara et al., 2004b; Joss et al., 2005; Vieno et al., 2007) and diclofenac (Lishman et al., 2006). One explanation is the daily concentration fluctuations during the sampling period (Clara et al., 2004b), which could be avoided by long term observation. The other explanation for the increased concentrations is the cleavage of glucuronide conjugates of those pharmaceuticals by enzymatic processes in the treatment plant (Ternes, 1998; Vieno et al., 2007). In the biological treatment processes, this cleavage makes it complex to evaluate the biodegradation of those residues since it is difficult to distinguish the bio-reduction from the cleavage increase.
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  • In activated sludge processes, it is the microorganism that mineralizes or transforms pollutants. Only organisms that are able to reproduce themselves during the designed sludge retention time (SRT) can be detained and enriched in the system (Kreuzinger et al., 2004; Clara et al., 2005a). Therefore, high SRTs allow for the enrichment of slowly growing bacteria and, consequently, the establishment of a more diverse biocoenosis with broader physiological capabilities, as compared to WWTPs that are operated at low SRTs.
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  • In the above studies, removal efficiencies at different SRTs were obtained from many WWTPs where the wastewater composition and other operational parameters could influence the removal efficiencies. Strenn et al. (2004) studied the removal of both drugs in a lab scale sequencing batch reactor (SBR) with synthetic wastewater. They evaluated the removal at SRTs from one day to 30 days and did not find an improvement in removal efficiencies of carbamazepine or diclofenac by increasing SRTs. Joss et al. (2005) studied the removal of carbamazepine and diclofenac in a pilot membrane bioreactor (MBR) with SRTs of 16 days to 75 days. Biodegradation of both drugs was independent of SRTs and sorption onto sludge did not increase either.
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  • Although high SRTs were obtained in MBR, micro- and ultra-filtration membranes did not promote any additional detention of both drugs. The removal efficiencies in MBR were comparable to conventional activated sludge processes operating at the same sludge age (Clara et al., 2005b).
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  • Carbamazepine can be photolysed under sunlight irradiation but only at relatively low rate. Andreozzi et al. (2002) studied the phototransformation of carbamazepine in double-distilled water and calculated its half-life to be 121.6 h, which is much lower than that of diclofenac shown above. In a study of Andreozzi et al. (2003), the half-life of carbamazepine was approximately 100 days in double distilled water; however, under the same conditions sulphamethoxazole, diclofenac, ofloxacin and propranolol underwent fast degradation with half-lives of 2.4, 5.0, 10.6 and 16.8 days, respectively. Thus, the phototransformation of carbamazepine in WWTPs is negligible.
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  • However, attentions should be put upon the presence of photosensitizers and inner filters in wastewater. For example, humic acids were found to act as inner filters for carbamazepine and diclofenac, decreasing their phototransformation, but as photosensitizers for sulphamethoxazole, clofibric acid, oflaxocin and propranolol, improving their phototransformation (Andreozzi et al., 2003). Furthermore, attentions ought to be paid to the byproducts of photosensitive compounds. It has been reported that diclofenac can form a product, chlorocarbazole 2a, which causes cell lysis with a markedly higher efficiency than the parent drug (Encinas et al., 1998).
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  • WWTP effluents are important gateways where carbamazepine can enter the water cycle. In a survey conducted by Ternes (1998), carbamazepine was detected in all 30 WWTP effluents with a 90percentile of 3700 ng LÀ1 and in 24 of 26 samples from 20 rivers with a 90-percentile of 820 ng LÀ1. The maximum concentration of carbamazepine in WWTP effluents was 6300 ng LÀ1, which was also the maximum detected concentration of all 32 drugs in the survey. Carbamazepine has been found in WWTP effluents around the world: Europe, the USA, Canada, Japan, and South Korea (Fig. 4). This list is expected to grow in the future. Carbamazepine concentrations in WWTP effluents are usually around hundreds of nanograms per liter, but can sometimes occur in micrograms per liter, with values varying from one country to another.
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  • due to the phototransformation process which, however, is not as effective in the hypolimnion. Löffler et al. (2005) also found that carbamazepine was highly recalcitrant to elimination in a water/ sediment system at laboratory scale. The time required for a 50%
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  • In a survey by Ternes (1998), diclofenac was detected in all 49 WWTP effluents with a 90-percentile of 1600 ng LÀ1 in all 43 samples from 22 rivers with a 90-percentile of 800 ng LÀ1. Paxéus (2004) detected diclofenac in all ten sampled WWTP effluents in the five EU countries he sampled. The concentrations of diclofenac ranged from 140 ng LÀ1 to 1480 ng LÀ1, with a median value of 290 ng LÀ1. The input of diclofenac through tributaries downstream of the WWTPs around Lake Greifensee in Switzerland was estimated to be in the range of 10–29 g dÀ1 (Buser et al., 1998). It was also detected in a stream (24.5 ng LÀ1) in Ohio, USA.
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  • Diclofenac has been found in estuaries as well. Thomas and Hilton (2004) investigated five estuaries in the UK and detected diclofenac at a maximum concentration of 195 ng LÀ1 (Mersey estuary) and a median concentration of less than 8 ng LÀ1. In the estuary of the river Elbe at the North Sea, it was detected at a concentration of 6.2 ng LÀ1 (Weigel et al., 2002). No data have been reported on its presence in the marine environment. The maximum concentration of diclofenac in surface waters is reported as 1030 ng LÀ1, detected in Berlin by Heberer et al. (2002).
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  • Diclofenac showed high retardation factors in the column experiments (Rf = 2.0 in Scheytt et al., 2004, and Rf = 2.6 in Mersmann et al., 2002), which indicated that it has its low mobility in the groundwater. The column experiments of Scheytt et al. (2006) found a 35% removal of diclofenac. Its low mobility may prevent it from having a large presence in groundwater to some extent. Although diclofenac was still detected in the groundwater in some cases, its concentrations were generally lower than those of carbamazepine. It was found in six of seven drinking water wells in the Hérault watershed in the Mediterranean region at concentrations around 2 ng LÀ1 (Rabiet et al., 2006). The maximum concentration in groundwater was found to be 380 ng LÀ1 in the catchment area of a drinking water plant in Berlin (Heberer et al., 1998). It has only been detected in drinking water in a sample taken from a private drinking water tap in Berlin at a concentration of less than 10 ng LÀ1 (Heberer, 2002b).
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