Fate of natural estrogen conjugates in municipal sewage transport and treatment facilities
The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six...
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| Published in | The Science of the total environment Vol. 302; no. 1; pp. 199 - 209 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Shannon
Elsevier B.V
20.01.2003
Elsevier Science |
| Subjects | |
| Online Access | Get full text |
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| Abstract | The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six activated sludge sewage treatment plants (STPs) were measured. The analytical method was based on solid-phase extraction by using a Carbograph 4 cartridge and Liquid Chromatography-tandem Mass Spectrometry. On average, a group of 73 women selected to represent a typical cross section of the female inhabitants of a Roman condominium, excreted 106, 14 and 32 μg/day of conjugated estriol (E
3), estradiol (E
2) and estrone (E
1), respectively. Apart from some E
3 in pregnancy urine, free estrogens were never detected in urine samples. Estrogen sulfates represented 21% of the total conjugated estrogens. This situation changed markedly in the condominium collecting tank. Here, significant amounts of free estrogens were observed and the estrogen sulfate to estrogen glucuronated ratio rose to 55/45. A laboratory biodegradation test confirmed that glucuronated estrogens are readily deconjugated in unmodified domestic wastewater, presumably due to the large amounts of the β-glucuronidase enzyme produced by fecal bacteria (
Escherichia coli). Deconjugation continued in sewer transit. At the STP entrance, free estrogens and sulfated estrogens were the dominant species. The sewage treatment completely removed residues of estrogen glucuronates and with good efficiency (84–97%) the other analytes, but not E
1 (61%) and estrone-3-sulfate (E
1-3S) (64%). Considering that (1) E
1 has half the estrogenic potency of E
2, (2) the amount of the former species discharged from STPs into the receiving water was more than ten times larger than the latter one and (3) a certain fraction of E
1-3S could be converted to E
1 in the aquatic environment, E
1 appears to be the most important natural endocrine disrupter. |
|---|---|
| AbstractList | The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six activated sludge sewage treatment plants (STPs) were measured. The analytical method was based on solid-phase extraction by using a Carbograph 4 cartridge and Liquid Chromatography-tandem Mass Spectrometry. On average, a group of 73 women selected to represent a typical cross section of the female inhabitants of a Roman condominium, excreted 106, 14 and 32 microg/day of conjugated estriol (E(3)), estradiol (E(2)) and estrone (E(1)), respectively. Apart from some E(3) in pregnancy urine, free estrogens were never detected in urine samples. Estrogen sulfates represented 21% of the total conjugated estrogens. This situation changed markedly in the condominium collecting tank. Here, significant amounts of free estrogens were observed and the estrogen sulfate to estrogen glucuronated ratio rose to 55/45. A laboratory biodegradation test confirmed that glucuronated estrogens are readily deconjugated in unmodified domestic wastewater, presumably due to the large amounts of the beta-glucuronidase enzyme produced by fecal bacteria (Escherichia coli). Deconjugation continued in sewer transit. At the STP entrance, free estrogens and sulfated estrogens were the dominant species. The sewage treatment completely removed residues of estrogen glucuronates and with good efficiency (84-97%) the other analytes, but not E(1) (61%) and estrone-3-sulfate (E(1)-3S) (64%). Considering that (1) E(1) has half the estrogenic potency of E(2), (2) the amount of the former species discharged from STPs into the receiving water was more than ten times larger than the latter one and (3) a certain fraction of E(1)-3S could be converted to E(1) in the aquatic environment, E(1) appears to be the most important natural endocrine disrupter. The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six activated sludge sewage treatment plants (STPs) were measured. The analytical method was based on solid-phase extraction by using a Carbograph 4 cartridge and Liquid Chromatography-tandem Mass Spectrometry. On average, a group of 73 women selected to represent a typical cross section of the female inhabitants of a Roman condominium, excreted 106, 14 and 32 mu g/day of conjugated estriol (E sub(3)), estradiol (E sub(2)) and estrone (E sub(1)), respectively. Apart from some E sub(3) in pregnancy urine, free estrogens were never detected in urine samples. Estrogen sulfates represented 21% of the total conjugated estrogens. This situation changed markedly in the condominium collecting tank. Here, significant amounts of free estrogens were observed and the estrogen sulfate to estrogen glucuronated ratio rose to 55/45. A laboratory biodegradation test confirmed that glucuronated estrogens are readily deconjugated in unmodified domestic wastewater, presumably due to the large amounts of the beta -glucuronidase enzyme produced by fecal bacteria (Escherichia coli). Deconjugation continued in sewer transit. At the STP entrance, free estrogens and sulfated estrogens were the dominant species. The sewage treatment completely removed residues of estrogen glucuronates and with good efficiency (84-97%) the other analytes, but not E sub(1) (61%) and estrone-3-sulfate (E sub(1)-3S) (64%). Considering that (1) E sub(1) has half the estrogenic potency of E sub(2), (2) the amount of the former species discharged from STPs into the receiving water was more than ten times larger than the latter one and (3) a certain fraction of E sub(1)-3S could be converted to E sub(1) in the aquatic environment, E sub(1) appears to be the most important natural endocrine disrupter. The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six activated sludge sewage treatment plants (STPs) were measured. The analytical method was based on solid-phase extraction by using a Carbograph 4 cartridge and Liquid Chromatography-tandem Mass Spectrometry. On average, a group of 73 women selected to represent a typical cross section of the female inhabitants of a Roman condominium, excreted 106, 14 and 32 μg/day of conjugated estriol (E 3), estradiol (E 2) and estrone (E 1), respectively. Apart from some E 3 in pregnancy urine, free estrogens were never detected in urine samples. Estrogen sulfates represented 21% of the total conjugated estrogens. This situation changed markedly in the condominium collecting tank. Here, significant amounts of free estrogens were observed and the estrogen sulfate to estrogen glucuronated ratio rose to 55/45. A laboratory biodegradation test confirmed that glucuronated estrogens are readily deconjugated in unmodified domestic wastewater, presumably due to the large amounts of the β-glucuronidase enzyme produced by fecal bacteria ( Escherichia coli). Deconjugation continued in sewer transit. At the STP entrance, free estrogens and sulfated estrogens were the dominant species. The sewage treatment completely removed residues of estrogen glucuronates and with good efficiency (84–97%) the other analytes, but not E 1 (61%) and estrone-3-sulfate (E 1-3S) (64%). Considering that (1) E 1 has half the estrogenic potency of E 2, (2) the amount of the former species discharged from STPs into the receiving water was more than ten times larger than the latter one and (3) a certain fraction of E 1-3S could be converted to E 1 in the aquatic environment, E 1 appears to be the most important natural endocrine disrupter. The concentrations of free and conjugated natural estrogens were measured in female urine, in a domestic tank collecting wastewater from a residential block with approximately 250 inhabitants, and in sewage-treatment-plant influents and effluents. The study was conducted in Rome, Italy. The rate of conversion of conjugated estrogens to their free forms in domestic wastewater was estimated from a laboratory experiment. Results showed that 106, 14, and 32 mu g of conjugated estriol, estradiol, and estrone, respectively, were excreted daily by the study subjects, and free estrogens were never detected. Estrogen sulfates were less abundant than estrogen glucuronides in the urine samples. Significant amounts of free estrogens were found in the collection tank, however, suggesting that deconjugation in sewers occurred more rapidly than expected, which could have been due to the high concentration of Escherichia coli and other bacteria in the tank. Results from the laboratory biodegradation test showed that estrogen glucuronides were degraded rapidly, whereas the sulfates were much more recalcitrant to biotransformation. The free estrogen-to-conjugated estrogen concentration ratio in the collection tank was 0.91, increasing to 2.0 at the entrance to the sewage-treatment plant. The surviving glucuronides were removed completely by sewage treatment, but a large fraction of the sulfates passed through the treatment system. The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six activated sludge sewage treatment plants (STPs) were measured. The analytical method was based on solid-phase extraction by using a Carbograph 4 cartridge and Liquid Chromatography-tandem Mass Spectrometry. On average, a group of 73 women selected to represent a typical cross section of the female inhabitants of a Roman condominium, excreted 106, 14 and 32 microg/day of conjugated estriol (E(3)), estradiol (E(2)) and estrone (E(1)), respectively. Apart from some E(3) in pregnancy urine, free estrogens were never detected in urine samples. Estrogen sulfates represented 21% of the total conjugated estrogens. This situation changed markedly in the condominium collecting tank. Here, significant amounts of free estrogens were observed and the estrogen sulfate to estrogen glucuronated ratio rose to 55/45. A laboratory biodegradation test confirmed that glucuronated estrogens are readily deconjugated in unmodified domestic wastewater, presumably due to the large amounts of the beta-glucuronidase enzyme produced by fecal bacteria (Escherichia coli). Deconjugation continued in sewer transit. At the STP entrance, free estrogens and sulfated estrogens were the dominant species. The sewage treatment completely removed residues of estrogen glucuronates and with good efficiency (84-97%) the other analytes, but not E(1) (61%) and estrone-3-sulfate (E(1)-3S) (64%). Considering that (1) E(1) has half the estrogenic potency of E(2), (2) the amount of the former species discharged from STPs into the receiving water was more than ten times larger than the latter one and (3) a certain fraction of E(1)-3S could be converted to E(1) in the aquatic environment, E(1) appears to be the most important natural endocrine disrupter.The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment. Levels of conjugated and free estrogens in (1) female urine; (2) a septic tank collecting domestic wastewater; (3) influents and effluents of six activated sludge sewage treatment plants (STPs) were measured. The analytical method was based on solid-phase extraction by using a Carbograph 4 cartridge and Liquid Chromatography-tandem Mass Spectrometry. On average, a group of 73 women selected to represent a typical cross section of the female inhabitants of a Roman condominium, excreted 106, 14 and 32 microg/day of conjugated estriol (E(3)), estradiol (E(2)) and estrone (E(1)), respectively. Apart from some E(3) in pregnancy urine, free estrogens were never detected in urine samples. Estrogen sulfates represented 21% of the total conjugated estrogens. This situation changed markedly in the condominium collecting tank. Here, significant amounts of free estrogens were observed and the estrogen sulfate to estrogen glucuronated ratio rose to 55/45. A laboratory biodegradation test confirmed that glucuronated estrogens are readily deconjugated in unmodified domestic wastewater, presumably due to the large amounts of the beta-glucuronidase enzyme produced by fecal bacteria (Escherichia coli). Deconjugation continued in sewer transit. At the STP entrance, free estrogens and sulfated estrogens were the dominant species. The sewage treatment completely removed residues of estrogen glucuronates and with good efficiency (84-97%) the other analytes, but not E(1) (61%) and estrone-3-sulfate (E(1)-3S) (64%). Considering that (1) E(1) has half the estrogenic potency of E(2), (2) the amount of the former species discharged from STPs into the receiving water was more than ten times larger than the latter one and (3) a certain fraction of E(1)-3S could be converted to E(1) in the aquatic environment, E(1) appears to be the most important natural endocrine disrupter. |
| Author | Mancini, R. Nazzari, M. Samperi, R Mastropasqua, R. Di Corcia, A. Gentili, A. D'Ascenzo, G. |
| Author_xml | – sequence: 1 givenname: G. surname: D'Ascenzo fullname: D'Ascenzo, G. – sequence: 2 givenname: A. surname: Di Corcia fullname: Di Corcia, A. email: antonio.dicorcia@uniroma1.it – sequence: 3 givenname: A. surname: Gentili fullname: Gentili, A. – sequence: 4 givenname: R. surname: Mancini fullname: Mancini, R. – sequence: 5 givenname: R. surname: Mastropasqua fullname: Mastropasqua, R. – sequence: 6 givenname: M. surname: Nazzari fullname: Nazzari, M. – sequence: 7 givenname: R surname: Samperi fullname: Samperi, R |
| BackLink | http://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=14474831$$DView record in Pascal Francis https://www.ncbi.nlm.nih.gov/pubmed/12526909$$D View this record in MEDLINE/PubMed |
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| Keywords | Conjugated natural estrogens Aqueous municipal environment LC-MS-MS detection Urine Activated sludge Chemical analysis Pollutant behavior Metabolite Estrogen Endocrine disruptor Estradiol Biological purification Persistence Domestic waste water Estrone Estriol Waste water purification Sex steroid hormone Degradation product |
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| References | Routledge, Sheahan, Desbrow, Sumpter, Waldock (BIB25) 1998; 32 Stanczyk, Miyakawa, Goebelsmann (BIB28) 1980; 137 Desbrow, Routledge, Brighty, Sumpter, Waldock (BIB10) 1998; 32 Andreolini, Borra, Caccamo, Di Corcia, Samperi (BIB5) 1987; 59 Lee, Peart (BIB20) 1998; 81 Belfroid, Van der Horst, Vethaak, Schäfer, Rijs, Wegener, Cofino (BIB8) 1999; 225 Ternes, Stumpf, Mueller, Haberer, Wilken, Servos (BIB29) 1999; 225 Fotsis, Jarvenpaa, Adlercreutz (BIB13) 1980; 12 Johnson, Sumpter (BIB17) 2001; 35 Caccamo, Carfagnini, Di Corcia, Samperi (BIB9) 1988; 434 Zangh, Henion (BIB32) 1999; 71 Ternes, Kreckel, Mueller (BIB30) 1999; 225 Preziosi (BIB22) 1998; 70 Baronti, Curini, D'Ascenzo, Di Corcia, Gentili, Samperi (BIB7) 2000; 24 Nasu, Goto, Kato, Oshima, Tanaka (BIB21) 2001; 43 Adlercreutz, Fotsis, Bannwart, Hämäläinen, Bloigu, Ollus (BIB3) 1986; 24 Key, Pike, Brown, Hermon, Allen, Wang (BIB18) 1996; 74 Purdom, Hardiman, Bye, Eno, Tyler, Sumpter (BIB23) 1994; 8 Tyler, Routledge (BIB31) 1998; 70 Shore, Gurevitz, Shemesh (BIB27) 1993; 51 Dray, Dray, Tiller, Ulman (BIB12) 1972; 123 Adlercreutz, Jarvenpaa (BIB2) 1982; 17 Shackleton (BIB26) 1986; 379 Baker, Jennison, Kelley (BIB6) 1980; 12 Johnson, Belfroid, Di Corcia (BIB16) 2000; 256 Fotsis, Adlercreutz (BIB14) 1987; 28 Routledge, Sumpter (BIB24) 1997; 272 Allen, Matthiesen, Scott, Haworth, Feist, Thain (BIB4) 1999; 233 Körner, Bolz, Süssmuth, Hiller, Schuller, Hanf, Hagenmaier (BIB19) 2000; 40 Adlercreutz, Brown, Collins, Goebelsman, Kellie, Campbell, Spieler, Braissand (BIB1) 1982; 17 Di Corcia, Bellioni, Madbouly, Marchese (BIB11) 1996; 733 Jobling, Nolan, Tyler, Brighty, Sumpter (BIB15) 1998; 32 |
| References_xml | – volume: 59 start-page: 1720 year: 1987 end-page: 1725 ident: BIB5 article-title: Estrogen conjugates in late-pregnancy fluids: extraction and group separation by a graphitized carbon black cartridge and quantification by high-performance liquid chromatography publication-title: Anal Chem – volume: 40 start-page: 1131 year: 2000 end-page: 1142 ident: BIB19 article-title: Input/output balance of estrogenic active compounds in a major municipal sewage plant in Germany publication-title: Chemosphere – volume: 71 start-page: 3955 year: 1999 end-page: 3964 ident: BIB32 article-title: Quantitative and qualitative determination of estrogen sulfates in human urine by liquid chromatography/tandem mass spectrometry using 96-well technology publication-title: Anal Chem – volume: 17 start-page: 695 year: 1982 end-page: 702 ident: BIB1 article-title: The measurement of urinary steroid glucuronides as indices of the fertile period in women publication-title: J Steroid Biochem – volume: 256 start-page: 163 year: 2000 ident: BIB16 article-title: Estimating steroid estrogen input into activated sludge treatment works and observation on their removal from the effluent publication-title: Sci Total Environ – volume: 8 start-page: 275 year: 1994 end-page: 285 ident: BIB23 article-title: Estrogenic effects of effluents from sewage treatment works publication-title: Chem Ecol – volume: 70 start-page: 1617 year: 1998 end-page: 1631 ident: BIB22 article-title: Endocrine disrupters as environmental signallers: an introduction publication-title: Pure Appl Chem – volume: 225 start-page: 81 year: 1999 end-page: 90 ident: BIB29 article-title: Behavior and occurrence of estrogens in municipal sewage treatment plants-I. Investigations in Germany, Canada and Brazil publication-title: Sci Total Environ – volume: 12 start-page: 503 year: 1980 end-page: 508 ident: BIB13 article-title: Purification of urine for quantification of the complete steroid profile publication-title: J Steroid Biochem – volume: 35 start-page: 4697 year: 2001 end-page: 4703 ident: BIB17 article-title: Removal of endocrine—disrupting chemicals in activated sludge treatment works publication-title: Environ Sci Technol – volume: 233 start-page: 5 year: 1999 end-page: 10 ident: BIB4 article-title: The extent of estrogenic contamination in the UK estuarine and marine environments—further survey of flounder publication-title: Sci Total Environ – volume: 17 start-page: 639 year: 1982 end-page: 645 ident: BIB2 article-title: Assay of estrogens in human feces publication-title: J Steroid Biochem – volume: 28 start-page: 203 year: 1987 end-page: 213 ident: BIB14 article-title: The multi-component analysis of estrogens in urine by ion exchange chromatography and GC-MS-I. 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Chemical fractionation and in vitro biological screening publication-title: Environ Sci Technol – volume: 12 start-page: 411 year: 1980 end-page: 415 ident: BIB6 article-title: A possible method for the detection of ovulation and the determination of the fertile period publication-title: J Steroid Biochem – volume: 32 start-page: 1559 year: 1998 end-page: 1565 ident: BIB25 article-title: Identification of estrogenic chemicals in STW effluent. 2. In vivo responses in trout and roach publication-title: Environ Sci Technol – volume: 733 start-page: 383 year: 1996 end-page: 393 ident: BIB11 article-title: Trace determination of phenols in natural waters by a new graphitized carbon black cartridge and re-analysis after phenol derivatization publication-title: J Chromatogr – volume: 137 start-page: 433 year: 1980 end-page: 450 ident: BIB28 article-title: Direct immunoassay of urinary estrogen and pregnandiol glucuronides during the menstrual cycle publication-title: Am J Obstet Gynecol – volume: 43 start-page: 101 year: 2001 end-page: 108 ident: BIB21 article-title: Study on endocrine disrupting chemicals in wastewater treatment plants publication-title: Water Sci Technol – volume: 32 start-page: 2498 year: 1998 end-page: 2506 ident: BIB15 article-title: Widespread sexual disruption in wild fish publication-title: Environ Sci Technol – volume: 123 start-page: 853 year: 1972 end-page: 857 ident: BIB12 article-title: Hydrolysis of urine metabolites of different steroid hormones by (-glucuronidase from publication-title: Ann Ist Pasteur – volume: 225 start-page: 91 year: 1999 end-page: 99 ident: BIB30 article-title: Behavior and occurrence off estrogens in municipal sewage treatment plants-II. Aerobic batch experiments with activated sludge publication-title: Sci Total Environ – volume: 24 start-page: 289 year: 1986 end-page: 296 ident: BIB3 article-title: Urinary estrogen profile determination in young Finnish vegetarian and omnivorous women publication-title: J Steroid Biochem – volume: 81 start-page: 1209 year: 1998 end-page: 1216 ident: BIB20 article-title: Determination of 17(-estradiol and its metabolites in sewage effluent by solid-phase extraction and gas chromatography/mass spectrometry publication-title: J AOAC Inter – volume: 51 start-page: 361 year: 1993 end-page: 366 ident: BIB27 article-title: Estrogen as an environmental pollutant publication-title: Bull Environ Contam Toxicol – volume: 74 start-page: 1313 year: 1996 end-page: 1316 ident: BIB18 article-title: Cigarette smoking and urinary estrogen excretion in pre-menopausal post-menopausal women publication-title: Br J Cancer |
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| Snippet | The aim of this study was to investigate the fate of the conjugated forms of the three most common natural estrogens in the municipal aqueous environment.... The concentrations of free and conjugated natural estrogens were measured in female urine, in a domestic tank collecting wastewater from a residential block... |
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| SubjectTerms | Activated sludge Adolescent Adult Aged Applied sciences Aqueous municipal environment Chromatography, Liquid Conjugated natural estrogens Escherichia coli estrogens Estrogens - analysis Estrogens - urine Exact sciences and technology Female Humans Italy LC-MS-MS detection Mass Spectrometry Middle Aged Other wastewaters Pollution Reference Values Sewage - chemistry Waste Disposal, Fluid Wastewaters Water Pollutants - analysis Water treatment and pollution |
| Title | Fate of natural estrogen conjugates in municipal sewage transport and treatment facilities |
| URI | https://dx.doi.org/10.1016/S0048-9697(02)00342-X https://www.ncbi.nlm.nih.gov/pubmed/12526909 https://www.proquest.com/docview/14657566 https://www.proquest.com/docview/19770728 https://www.proquest.com/docview/72956282 |
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