Occurrence of Pharmaceuticals and Personal Care Products in Wastewater Systems

Transcription

1 ccurrence of Pharmaceuticals and Personal are Products in Wastewater Systems Yutaka SUZUKI *, Koya KMRI, rata RD, orihide KD, Makoto YSJIM Water Quality Research Team, Water Environment Research Group, Public Works Research Institute 1. Introduction Recently, there has been a growing public concern about the emergence of environmental pollution of water sources from pharmaceuticals and personal care products (PPPs). onsidering the route PPPs take to reach water environment, wastewater treatment plants (WWTPs) may facilitate their initial entry. If PPPs are not properly treated during the wastewater treatment process, they can contaminate water environment, including drinking water sources. onsidering the current level of knowledge regarding this problem, it is necessary to clarify the fates of PPPs in WWTPs to identify appropriate treatment methods. In our research, we analyzed the presence of PPPs in several WWTPs to clarify the concentrations and fates of PPPs along the units of wastewater treatment. In addition, toxic effects of antibiotics on aquatic organisms were evaluated with ecotoxicity s, and ecological risk of the antibiotics was evaluated by comparison between concentrations in water environment and ecotoxicity results. 2. Survey Sites and Methods Surveys were conducted in four or six WWTPs employing conventional activated process, depending on the type of the PPPs. Twenty four-hour water flow proportional composite samples were collected from several sampling locations in each WWTP. The target PPPs were four anti-inflammatories (aspirin, ketoprofen, ibuprofen, naproxen), a phenolic antiseptic (triclosan), three amide pharmaceuticals (crotamiton, diethyltoluamide, carbamazepine) and two antibiotics (levofloxacin, clarithromycin). They were analyzed with GMS or LSMSMS after sample extraction and purification according to the methods by akada,. et al.(26) and Yasojima, M. et al.(26). Ecotoxicity was evaluated with the s using bacterium, alga and crustacean. * 1-6 Minamihara, Tsukuba, Ibaraki, Japan ysuzuki@pwri.go.jp

2 3. ccurrence and Fate of PPPs The PPP concentrations in the influent were of the order of hundreds ngl, except for carbamazepine of the order of tens ngl. lmost all of the PPPs existed in the dissolved form except for triclosan and antibiotics, which might be the reason for no remarkable decrease after the primary. During the biological treatment, two anti-inflammatories (aspirin and ibuprofen) and triclosan were effectively removed, while the remaining anti-inflammatories (ketoprofen and naproxen), diethyltoluamide and antibiotics showed around 5% reduction, and crotamiton and carbamazepine was hardly removed. The fates of PPPs were evaluated by calculating the mass balance of PPPs in the WWTPs. Ibuprofen was significantly removed and degraded by the activated in the aeration (Figure 1), while triclosan was removed by the adsorption to the activated and the accumulation in the was observed (Figure 2). ntibiotics was removed mainly by the adsorption to the activated, and accumulation in the was observed..9 gday <.2 gday 36 gday gday Figure 1 Mass balance of ibuprofen in WWTP Figure 2 Mass balance of triclosan in WWTP 4. Ecotoxicity of ntibiotics Microtox using marine fluorescent bacterium and Daphnia immobilization showed that levofloxacin (LVFX) and clarithromycin (M) have no acute toxicity on bacterium. Meanwhile, algal growth inhibition revealed that LVFX and M have a toxicity to microalga, but the phytotoxicity of M was about 1 fold higher than that of LVFX. omparison of the concentration in aquatic environment and PE indicates that M discharged into aquatic environment may affect algae if dilution rate is low. Reference akada,. et al.(26) Pharmaceutical chemicals and endocrine disrupters in municipal wastewater in Tokyo and their removal during activated treatment, Water Research 4, Yasojima, M. et al.(26) ccurrence of levofloxacin, clarithromysin and azithromycin in wastewater treatment plant in Japan, Wat. Sci. & Tech., 53(11),

3 ccurrence of Pharmaceuticals and Personal are Products in Wastewater Systems Yutaka SUZUKI*, Koya KMRI*, rata RD*, orihide KD* and Makoto YSJIM** *Water Quality Research Team Water Environment Research Group Public Works Research Institute **Towa Kagaku orporation Public Works Research Institute 1. Introduction - Growing public concern about the environment pollution of pharmaceuticals and personal care products (PPPs) -From existing research, wastewater treatment plants (WWTPs) may facilitate the initial entry of PPPs to water environment -It is important to clarify the occurrence and fates of PPPs in WWTPs to evaluate both the effect of treated wastewater on water environment and the performance of WWTPs to remove PPPs -In our research, we conducted surveys in several WWTPs to clarify the concentrations and fates of PPPs along the units of wastewater treatment. -In addition, toxic effects of PPPs on aquatic organisms were evaluated with ecotoxicity s. 2. ccurrence and Fate of PPPs (nti-inflammatory Drugs, etc.) in WWTPs Sedimentation Tank eration Tank Effluent Effluent hlorine Disinfection Sedimentation Tank Treatment method : onventional activated process Treatment capacity : 22,5~7, m 3 d umber of plants surveyed : 4 Sampling : omposite sample taken every 2 hours PPPs grouping by structural characteristics nti-inflammatory drugs: spirin, Ibuprofen, Fenoprofen, aproxen, Mefenamic cid, aving carboxl group (-) Phenolic antiseptic: Group 3 Fenoprofen Fenoprofen Ibuprofen 3 3 spirin 3 3 aproxen 3 acid Mefenamic cid Group aving Phenol Group Group Group mide pharmaceuticals: (relieve itching) arbamazepine (ntiepileptic) Group 殺菌剤 鎮痒剤 2 arbamazepine 抗てんかん薬 1 phase concentration change along treatment units (1) Ibuprofen 8 Ibprofen 濃度 (ngl) Tricrosan 濃度 (ngl) 5 Inf : PE : Effluent SE : Effluent : Effluent 4 aproxen 濃度 (ngl) 2 phase concentration change along treatment units (2) aproxen 濃度 (ngl) Inf : PE : Effluent SE : Effluent : Effluent

4 e 濃度 (ngl) phase concentration change along treatment units (3) arbamazepine arbamazepine 濃度 (ngl) Inf : PE : Effluent SE : Effluent : Effluent verage PPP removal ratio in WWTPs PPPs Removal ratio (%) spirin nti-inflammatory 96 Ibuprofen nti-inflammatory 95 ntiseptic 9 aproxen nti-inflammatory 55 nti-inflammatory 5 relieve itching 2 arbamazepine ntiepileptic -25 Mefenamic acid nti-inflammatory -24 From the survey of 4 WWTPs, -PPPs (anti-inflammatory drugs, etc) concentraion in dissolved phase in influent ranged from hundreds to one thousand ngl except for arbamazepine -PPPs could be classified into three groups by the removal ratio in WWTPs Mass balance of PPPs including solid phase concentration a) Ibuprofen b) gday gday <.2 gday 2.6 gday c) 12. gday d) arbamazepine gday gday 1.3 gday From the mass balance survey in a WWTP, -lmost of all of the PPPs existed in the dissolved phase, except for which mostly existed in solid phase. -Ibuprofen was decomposed in the biological treatment process effectively - was removed by the adsorption to the activetaed, and was accumulated in the activated in a high concentration. - and arbamazepine was hardly changed in the process 3. ccurrence and Fate of ntibiotics in WWTP Levofloxacin(LVFX LVFX) 3 F Sampling 3 Screen eration arithromycin (M) Sampling points oncentration oncentration change of antibiotics along treatment units LVFX n=6 eration median max min oncentration M n=6 eration median max min ctivated reactors onventional activated process 1 Effect of return? or deconjugation? or other factors?

5 LVFX M Mass balance of antibiotics eration eration (μgd) From the survey of antibiotics, -ntibiotics concentration in the influent ranged from hundreds to one thousand ngl, and the removal ratio in WWTPs was around 5% -LVFX was removed by the adsorption to the activated, and was accumulated in the activated in a high concentration -M accumulation in the was small, which might indicate biodegradation by the activated 4. Effect of PPPs on quatic rganisms Ecotoxicity s (acute toxicity) applied - acterium: Microtox - lga: lgal growth inhibition - rustacean: Daphnia acute immobilization spirin PPPs Levofloxacin arithromycin Results of Ecotoxicity s Microtox 5min E5 15min.6 lgal growth inhibition E5 96hour hour.4 E5 (mgl) Daphnia acute immobilization 48hour.4 : o Effect omparison between E5 and the concentration of wastewater (μgl) (b or c)a arithromycin (μgl) (b or c)a E5 (a) 4 11 (b) (c) From the ecotoxicity s, - ntiseptic agent () showed toxicity on acterium and rustacean - ntibiotics showed inhibition to lgal growth - The toxic effect concentration was in the order of mgl except for arithromycin - arithromycin in treated wastewater might be evaluated to have toxic effect on lga if E is obtained onclusion - The concentration of most PPPs in influent ranged from hundreds to one thousand ngl - Several patterns of PPP removal in the treatment process were observed; a) effectively decomposed by activated b) adsorbed to activated c) hardly changed - Some PPPs showed ecotoxicity, but the concentration of the order of mgl - ntibiotic in treated wastewater might be evaluated to have toxic effect on lga