Behavior of Human Antibiotics in Wastewater Treatment Plants

Antibiotics resident in sewage and in the water environment have become an emerging public concern in many developed countries. Also in Japan, studies about their concentrations in the environment and in the discharge from sewage treatment plants have begun to be reported. The objectives of this res...

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Published inENVIRONMENTAL ENGINEERING RESEARCH Vol. 42; pp. 357 - 368
Main Authors YASOJIMA, Makoto, KOBAYASHI, Yoshikazu, TANAKA, Hiroaki, KOMORI, Koya, SUZUKI, Yutaka, NAKADA, Norihide
Format Journal Article
LanguageEnglish
Japanese
Published Japan Society of Civil Engineers 2005
公益社団法人 土木学会
Subjects
Online AccessGet full text
ISSN1341-5115
1884-829X
DOI10.11532/proes1992.42.357

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Abstract Antibiotics resident in sewage and in the water environment have become an emerging public concern in many developed countries. Also in Japan, studies about their concentrations in the environment and in the discharge from sewage treatment plants have begun to be reported. The objectives of this research were to clarify the behavior in sewage treatment plants about selected human antibiotics, namely levofloxacin (LVFX), clarithromycin (CAM) and azithromycin (AZM). In samples of filtered influents and secondary effluents, average concentrations of LVFX, CAM and AZM were 552, 301ng/L, 647, 359ng/L and 260, 138ng/L, respectively. Removal efficiencies of LVFX, CAM and AZM in sewage treatment plants were 46%, 45% and 47%, respectively. These removal efficiencies and sludge retention time (SRT) in their reactors had some correlation. When the pH dependability of octanol-water partition coefficients (Kow) of LVFX, CAM and AZM was examined in this study, clear pH dependability was observed in the range from pH 3 to 9. As a result of batch test of sorption to activated sludge, sorption was suggested to be major removal mechanism for LVFX and AZM. On the other hand, biodegradation was suggested to be major removal mechanism for CAM. Further, behavior of these antibiotics including suspended solid and activated sludge was clarified in a pilot plant. As a result of this survey, one to ten times high concentrations of LVFX, CAM and AZM in activated sludge was detected than water phase, which demonstrated that these antibiotics tend to be sorbed to activated sludge. However, Log Kow alone was not able to explain this adsorption phenomenon. In contrast, Log Kd had a possibility that it could be explained.
AbstractList Antibiotics resident in sewage and in the water environment have become an emerging public concern in many developed countries. Also in Japan, studies about their concentrations in the environment and in the discharge from sewage treatment plants have begun to be reported. The objectives of this research were to clarify the behavior in sewage treatment plants about selected human antibiotics, namely levofloxacin (LVFX), clarithromycin (CAM) and azithromycin (AZM). In samples of filtered influents and secondary effluents, average concentrations of LVFX, CAM and AZM were 552, 301ng/L, 647, 359ng/L and 260, 138ng/L, respectively. Removal efficiencies of LVFX, CAM and AZM in sewage treatment plants were 46%, 45% and 47%, respectively. These removal efficiencies and sludge retention time (SRT) in their reactors had some correlation. When the pH dependability of octanol-water partition coefficients (Kow) of LVFX, CAM and AZM was examined in this study, clear pH dependability was observed in the range from pH 3 to 9. As a result of batch test of sorption to activated sludge, sorption was suggested to be major removal mechanism for LVFX and AZM. On the other hand, biodegradation was suggested to be major removal mechanism for CAM. Further, behavior of these antibiotics including suspended solid and activated sludge was clarified in a pilot plant. As a result of this survey, one to ten times high concentrations of LVFX, CAM and AZM in activated sludge was detected than water phase, which demonstrated that these antibiotics tend to be sorbed to activated sludge. However, Log Kow alone was not able to explain this adsorption phenomenon. In contrast, Log Kd had a possibility that it could be explained.
Author KOBAYASHI, Yoshikazu
SUZUKI, Yutaka
NAKADA, Norihide
YASOJIMA, Makoto
KOMORI, Koya
TANAKA, Hiroaki
Author_FL 八十島 誠
田中 宏明
小森 行也
中田 典秀
鈴木 穣
小林 義和
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  organization: Water Environment Research Group, Public Works Research Institute
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  fullname: NAKADA, Norihide
  organization: Water Environment Research Group, Public Works Research Institute
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References 20) Golet, E. M., Xifra, I., Siegrist, H., Alder, A. C., and Giger, W.; Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil, Environmental Science and Technology, 37, pp.3243-3249, 2003.
14) 鈴木俊也, 宇佐美美穂子, 永山敏廣; 河川水中のアレルギー治療薬のモニタリング, 第39回日本水環境学会年会講演集, p.613, 2005.
17) 平松啓一; 抗生物質が効かない, 270pp.集英社, 1999.
16) 宮本英樹; 細菌の逆襲が始まった, 200pp.河出書房新社, 2000.
18) Golet, E. M., Alder, A. C., Hartmann, A., Temes, T. A. and Giger, W.; Trace determination of fluoroquinolone antibacterial agents in urban wastewater by solid-phase extraction and liquid chromatography with fluorescence detection, Analytical Chemistry, 73, pp.3632-3638, 2001.
4) Calamari, D., Zuccato, E., Castiglioni, S., Bagnati, R. and Fanelli, R.; Strategic survey of therapeutic drugs in the rivers Po and Lambro in Northern Italy, Environmental Science and Technology, 37, pp.1241-1248, 2003.
26) 辻彰; 2004年版薬剤師のための常用医薬品情報集, 1253pp.廣川書店, 東京, 2004
28) Johannes, T; Sorption of veterinary pharmaceuticals in soils: A review, Environmental Science and Technology, 35, pp.3397-3406, 2001
27) Syracuse Research Corporation, http://www.syrres.com/esc/kowwin.htm
10) 篠原裕之, 谷島利勝, 高田秀重, 中田典秀, 田中宏明;下水処理場におけるオゾン処理および砂濾過処理による医薬品とエストロゲン様物質の除去, 第39回日本水環境学会年会講演集, p.481, 2005.
9) 中田典秀, 小森行也, 鈴木穣, 八十島誠, 田中宏明; 下水処理過程における解熱鎮痛剤, 抗てんかん薬等医薬品の動態, 第39回日本水環境学会年会講演集, p.57, 2005.
15) 厚生労働省医政局; 薬事工業生産動態統計年報平成14年, pp.210-359, じほう, 2003.
2) Ternes, T. A.; Occurrence of drugs in German sewage treatment plants and rivers, Water Research, 32, pp.3245-3260, 1998.
25) 独立行政法人医薬品医療機器総合機構; 医薬品医療機器情報提供ホームページ, http://www.info.pmda.go.jp
29) Namkung, E. and Rittmann, B. E.; Estimating volatile organic compounds emissions from publicly owned treatment works, Journal of Water Pollutant Control Fed., 59, 670
23) Reverté, S., Borrull, F., Pocurull, E. and Marcé, R. M; Determination of antibiotic compounds in water by solid-phase extraction-high-performance liquid chromatography-(electrospray) mass spectrometry, Journal of Chromatography A, 1010, pp.225-232, 2003.
19) Mcardell, C. S., Molnar, E., Suter, M. J. E, and Giger, W.; Occurrence and fate of macrolide antibiotics in wastewater treatment plants and in the Glatt Valley Watershed, Switzerland, Environmental Science and Technology, 37, pp.5479-5486, 2003.
5) ERAVMIS, http://www.silsoe.cranfield.ac.uk/ecochemistry/eravmis
6) ENVIRPHARMA, http://www.envirpharma.org
8) 清野敦子, 古荘早苗, 益永茂樹; わが国の水環境中における人用・動物用医薬品の存在, 水環境学会誌, 27, pp.685-691, 2004.
13) 八十島誠, 小森行也, 中田典秀, 鈴木穣, 田中宏明; ヒト用抗生物質の下水処理場における実態, 第39回日本水環境学会年会講演集, p.56, 2005.
3) Kolpin, D. W, Furlong, E. T., Meyer, M. T., Thurman, E. M., Zaugg, S. D., Barber, L. B. and Buxton, H. T.; Pharmaceuticals, hormones, and other organic wastewater contaminants in U. S. streams, 1999-2000: A national reconnaissance, Environmental Science and Technology, 36, pp.1202-1211, 2002.
24) Giger, W., Alder, A. C., Golet, E. M., Kohler, H. P. E., McArdell, C. S., Molnar, E., Siegrist, H. and Suter, M. J. F.; Occurrence and fate of antibiotics as trace contaminants in wastewaters, sewage sludges, and surface waters, ENVIRONMENTAL ANALYSIS, 57, 485-491, 2003.
22) 小林義和, 田中宏明, 人十島誠, 小森行也, 鈴木穣; 下水処理場における人用抗生物質の動態, 第42回下水道研究発表会要旨集, pp.558-560, 2005.
21) 田中信夫, 中村昭四郎; 抗生物質大要-化学と生物活性, 433pp.東京大学出版会, 東京, 1995.
1) Hirsch, R., Ternes, T., Haberer, K. and Kratz, K. L.; Occurrence of antibiotics in the aquatic environment, The Science of Total Environment, 225, pp.109-118, 1999.
12) 柿本貴志, 大澤輝真, 船水尚行; バイオトイレ内微生物に対する抗生物質の影響と活性の回復に関する研究, 第39回日本水環境学会年会講演集, p.55, 2005.
11) 浦瀬太郎, 田中俊至; 性状の異なる活性汚泥による医薬品等の分解・吸着速度, 第39回日本水環境学会年会講演集, p.54, 2005.
7) 八十島誠, 山下尚之, 中田典秀, 小森行也, 鈴木穣, 田中宏明; 下水処理水中に含まれるレボフロキサシン, クラリスロマイシンの分析と藻類生長への影響, 水環境学会誌27, pp.707-714, 2004.
References_xml – reference: 22) 小林義和, 田中宏明, 人十島誠, 小森行也, 鈴木穣; 下水処理場における人用抗生物質の動態, 第42回下水道研究発表会要旨集, pp.558-560, 2005.
– reference: 15) 厚生労働省医政局; 薬事工業生産動態統計年報平成14年, pp.210-359, じほう, 2003.
– reference: 26) 辻彰; 2004年版薬剤師のための常用医薬品情報集, 1253pp.廣川書店, 東京, 2004
– reference: 3) Kolpin, D. W, Furlong, E. T., Meyer, M. T., Thurman, E. M., Zaugg, S. D., Barber, L. B. and Buxton, H. T.; Pharmaceuticals, hormones, and other organic wastewater contaminants in U. S. streams, 1999-2000: A national reconnaissance, Environmental Science and Technology, 36, pp.1202-1211, 2002.
– reference: 1) Hirsch, R., Ternes, T., Haberer, K. and Kratz, K. L.; Occurrence of antibiotics in the aquatic environment, The Science of Total Environment, 225, pp.109-118, 1999.
– reference: 14) 鈴木俊也, 宇佐美美穂子, 永山敏廣; 河川水中のアレルギー治療薬のモニタリング, 第39回日本水環境学会年会講演集, p.613, 2005.
– reference: 16) 宮本英樹; 細菌の逆襲が始まった, 200pp.河出書房新社, 2000.
– reference: 6) ENVIRPHARMA, http://www.envirpharma.org/
– reference: 29) Namkung, E. and Rittmann, B. E.; Estimating volatile organic compounds emissions from publicly owned treatment works, Journal of Water Pollutant Control Fed., 59, 670
– reference: 11) 浦瀬太郎, 田中俊至; 性状の異なる活性汚泥による医薬品等の分解・吸着速度, 第39回日本水環境学会年会講演集, p.54, 2005.
– reference: 19) Mcardell, C. S., Molnar, E., Suter, M. J. E, and Giger, W.; Occurrence and fate of macrolide antibiotics in wastewater treatment plants and in the Glatt Valley Watershed, Switzerland, Environmental Science and Technology, 37, pp.5479-5486, 2003.
– reference: 10) 篠原裕之, 谷島利勝, 高田秀重, 中田典秀, 田中宏明;下水処理場におけるオゾン処理および砂濾過処理による医薬品とエストロゲン様物質の除去, 第39回日本水環境学会年会講演集, p.481, 2005.
– reference: 13) 八十島誠, 小森行也, 中田典秀, 鈴木穣, 田中宏明; ヒト用抗生物質の下水処理場における実態, 第39回日本水環境学会年会講演集, p.56, 2005.
– reference: 2) Ternes, T. A.; Occurrence of drugs in German sewage treatment plants and rivers, Water Research, 32, pp.3245-3260, 1998.
– reference: 4) Calamari, D., Zuccato, E., Castiglioni, S., Bagnati, R. and Fanelli, R.; Strategic survey of therapeutic drugs in the rivers Po and Lambro in Northern Italy, Environmental Science and Technology, 37, pp.1241-1248, 2003.
– reference: 27) Syracuse Research Corporation, http://www.syrres.com/esc/kowwin.htm
– reference: 28) Johannes, T; Sorption of veterinary pharmaceuticals in soils: A review, Environmental Science and Technology, 35, pp.3397-3406, 2001
– reference: 17) 平松啓一; 抗生物質が効かない, 270pp.集英社, 1999.
– reference: 8) 清野敦子, 古荘早苗, 益永茂樹; わが国の水環境中における人用・動物用医薬品の存在, 水環境学会誌, 27, pp.685-691, 2004.
– reference: 9) 中田典秀, 小森行也, 鈴木穣, 八十島誠, 田中宏明; 下水処理過程における解熱鎮痛剤, 抗てんかん薬等医薬品の動態, 第39回日本水環境学会年会講演集, p.57, 2005.
– reference: 23) Reverté, S., Borrull, F., Pocurull, E. and Marcé, R. M; Determination of antibiotic compounds in water by solid-phase extraction-high-performance liquid chromatography-(electrospray) mass spectrometry, Journal of Chromatography A, 1010, pp.225-232, 2003.
– reference: 7) 八十島誠, 山下尚之, 中田典秀, 小森行也, 鈴木穣, 田中宏明; 下水処理水中に含まれるレボフロキサシン, クラリスロマイシンの分析と藻類生長への影響, 水環境学会誌27, pp.707-714, 2004.
– reference: 20) Golet, E. M., Xifra, I., Siegrist, H., Alder, A. C., and Giger, W.; Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil, Environmental Science and Technology, 37, pp.3243-3249, 2003.
– reference: 12) 柿本貴志, 大澤輝真, 船水尚行; バイオトイレ内微生物に対する抗生物質の影響と活性の回復に関する研究, 第39回日本水環境学会年会講演集, p.55, 2005.
– reference: 5) ERAVMIS, http://www.silsoe.cranfield.ac.uk/ecochemistry/eravmis/
– reference: 21) 田中信夫, 中村昭四郎; 抗生物質大要-化学と生物活性, 433pp.東京大学出版会, 東京, 1995.
– reference: 25) 独立行政法人医薬品医療機器総合機構; 医薬品医療機器情報提供ホームページ, http://www.info.pmda.go.jp/
– reference: 24) Giger, W., Alder, A. C., Golet, E. M., Kohler, H. P. E., McArdell, C. S., Molnar, E., Siegrist, H. and Suter, M. J. F.; Occurrence and fate of antibiotics as trace contaminants in wastewaters, sewage sludges, and surface waters, ENVIRONMENTAL ANALYSIS, 57, 485-491, 2003.
– reference: 18) Golet, E. M., Alder, A. C., Hartmann, A., Temes, T. A. and Giger, W.; Trace determination of fluoroquinolone antibacterial agents in urban wastewater by solid-phase extraction and liquid chromatography with fluorescence detection, Analytical Chemistry, 73, pp.3632-3638, 2001.
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Snippet Antibiotics resident in sewage and in the water environment have become an emerging public concern in many developed countries. Also in Japan, studies about...
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SubjectTerms activated sludge
human antibiotics
octanol-water partition coefficients
sludge retention time
sorption
Title Behavior of Human Antibiotics in Wastewater Treatment Plants
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