SUPPORTING INFORMATION
Triclosan occurrence in freshwater systems in the United States (1999-
2012): A meta-analysis
Angela L. Perez
†
, Marianna Anderle de Sylor
†
, Andrew J. Slocombe
†
, Mindy G.
Lew
†
, Ken M. Unice
‡
, and Ellen P. Donovan
†
†
ChemRisk, 101 2 nd Street, Suite 700, San Francisco, CA 94105
‡
ChemRisk, 20 Stanwix Street, Suite 505, Pittsburgh, PA 15222
Pages S1-S24; includes Table S1, S2; Figures S1, S2
Word count including text, figures, tables, and references: 4249
S1
1 Table S1. Reported analytical limits of detection (LODs), sample numbers, and methods information from the
2 studies used in the meta-analysis of triclosan in U.S. freshwater aquatic systems.
3
Reference*
Anderson P, Denslow N, Drewes JE, Olivieri A, Schlenk D,
Snyder S. 2010. Monitoring strategies for chemicals of emerging concern (CECs) in recycled water: Recommendation of a science advisory panel. California State Water Resources Control Board,
Sacramento, CA, USA. 180 p.
Water Type
LOD
(ng/L) N
Methods available?
(y/n)
Filtered, centrifuged or flocculated?
(y/n)
QC included?
(y/n)
Surrogate or internal standard added prefiltration?
(y/n)
Effluent* NR 19 N NR NR NR
N
Y
Y
Y
N
N
Barber LB, Murphy S, Verplanck P, Sandstrom M, Taylor H,
Furlong E. 2006. Chemical loading into surface water along a hydrological biogeochemical, and land use gradient: A holistic watershed approach.
Environ Sci and Technol 40:475-486.
Effluent
Environmental
Barnes, K.K., Kolpin, D.W., Furlong, E.T., Zaugg, S.D., Meyer,
M.T., and Barber, L.B., 2008, A national reconnaissance of pharmaceuticals and other organic wastewater contaminants in the United States--I. Groundwater: Science of the Total
Environment, v. 402, no. 2-3, p. 192-200.
Benotti MJ, Trenholm RA, Vanderford BJ, Holady JC, Stanford
BD, Snyder SA. 2009. Pharmaceuticals and endocrine disrupting compounds in U.S. drinking water. Environmental Science and
Technology 43:597-603.
Environmental
Environmental
1 4
1 24
1
1
47
44
Y
Y
Y
Y
Y
Y
Y
Y
NR
N
S2
Boyd GR, Palmeri JM, Zhang S, Grimm DA. 2004.
Pharmaceuticals and personal care products (PPCPs) and endocrine disrupting chemicals (EDCs) in stormwater canals and
Bayou St. John in New Orleans, Louisiana, USA.
Sci Total
Environ 333:137-148.
Finished
Environmental
1 62
0.2 34
Boyd GR, Reemtsma H, Grimm DA, Mitra S. 2003.
Pharmaceuticals and personal care products (PPCPs) in surface and treated waters of Louisiana, USA and Ontario, Canada. Sci
Total Environ 311:135-149.
Carter JM, Kingsbury JA, Delzer GC, Hopple JA. 2010.
Concentration data for anthropogenic organic compounds in groundwater, surface water, and finished water of selected community water systems in the United States, 2002 –10. U.S.
Geological Survey Data Series 544. United States Geological
Survey, Reston, VA, USA. 36 p.
City of Chicago Emerging Contaminant Study. 2010. Table A:
Lake Michigan and drinking water results: analysis of endocrine disrupting chemicals, pharmaceuticals, and personal care product. Final Report. City of Chicago Department of Water
Management, Chicago, IL, USA. 3 p.
Effluent 0.2 1
Environmental
Finished
Environmental
0.2
0.2
500
4
1
478
Finished
Environmental
500
5
241
60
Conn KE, Lowe KS, Drewes JE, Hoppe-Jones C, Tucholke MB.
2010. Occurrence of pharmaceuticals and consumer product chemicals in raw wastewater and septic tank effluent from singlefamily homes. Environ Eng Sci 27:1-10.
Finished
Untreated*
5
200
30
20
Coogan M, Edziyic R, La Point T, Venables B. 2007. Algal bioaccumulation of triclocarban, triclosan, and methyl-triclosan in a North Texas wastewater treatment plant receiving stream.
Chemosphere 67:1911-1918.
Effluent*
Effluent
200
10
16
1
Y
N
Y
Y
Y
Y
Y
Y
N
Y
Y
Y
Y
NR
NR
Y
Y
N
Y
Y
Y
Y
N
Y
Y
Y
Y N
NR
N
S3
Y
NR
N
N
N
N
N
Y
Y
Y
Y
Y
Y
Y
Y
Y
N
N
Coogan M, La Point T. 2008. Snail bioaccumulation of triclocarban, triclosan, and methyltriclosan in a north Texas, USA, stream affected by wastewater treatment plant runoff. Enviro
Toxicol Chem 27:1788-1793.
Effluent-impacted environmental
Environmental
Effluent
10
10
10
1
2
1
Des Moines Water Works. 2010. Pharmaceutical and EDC data summary finished drinking water. Table. Des Moines Water
Works, Des Moines, IA, USA.
Environmental 20 4
Duff B. 2006. Evaluation of pharmaceuticals and personal care products in Des Moines source and finished waters. Final Report.
Des Moines Water Works, Des Moines, IA, USA. 16 p.
Finished
Untreated
Illinois Environmental Protection Agency (IEPA). 2008. Report on pharmaceuticals and personal care products in Illinois drinking water. Final Report. Illinois EPA Bureau of Water, Springfield, IL,
USA. 10 p.
Fair PA, Lee HB, Adams J, Darling C, Pacepavicius G, Alaee M,
Bossart GD, Henry N, Muir D. 2009. Occurrence of triclosan in plasma of wild Atlantic bottlenose dolphins ( Tursiops truncatus and in their environment.
Environ Pollut 157:2248-2254.
Focazio M, Kolpin D, Barnes K, Furlong E, Meyer M, Zaugg S,
Barber LB, Thurman E. 2008. A national reconnaissance for
)
Effluent
Environmental
Environmental
Finished
Finished
Finished
Untreated
Untreated
Effluent
20 3
2
2
2
5
2
2
2
5
2
2
39
3.7
39
5
39
39
3.7
5
10
10
N
N
Y
Y
Y
N
Y
Y
Y
N
Y
Y
Y
Y
Y
N
N
N
NR
NR
Y
Y
Y
NR
Y
Y
Y
NR
Y
Y
Y
Y
Y
NR
NR
Y
Y
Y
NR
Y
Y
Y
NR
N
N
S4
NR
Y
Y
Y
NR
Y
Y
Y
NR
Y
Y
Y
Y
Y
NR
pharmaceuticals and other organic wastewater contaminants in the United States- II) untreated drinking water sources. Sci Total
Environ 402:201-216.
Environmental
Environmental
3 14
90 120
Glassmeyer S, Furlong E, Kolpin D, Cahill J, Zaugg S, Werner S,
Meyer M, Kryak D. 2005. Transport of chemical and microbial compounds from known wastewater discharges: potential for use as indicators of human fecal contamination. Environ Sci Techol
39:5157-5169.
Effluent-impacted environmental
97 31
Haggard B, Galloway J, Green W, Meyer M. 2006.
Pharmaceuticals and other organic chemicals in selected North-
Central and Northwestern Arkansas streams. J Environ Qual
35:1-11.
Environmental 97 b 9
Environmental 480 21
Halden RU, Paull DH. 2005. Co-occurrence of triclocarban and triclosan in U.S. water resources. Environ Sci Techol 39:1420-
1426.
Untreated* NR
Heidler J, Halden RU. 2009. Fate of organohalogens in U.S. wastewater treatment plants and estimated chemical releases to soils nationwide from biosolids recycling. J Environ Monit
11:2207 –2215.
Heidler J, Halden RU. 2007. Mass balance assessment of triclosan removal during conventional sewage treatment.
Chemosphere 66:362-369.
Effluent*
Untreated
Effluent-impacted environmental
Untreated
NR
250
20
250
Kolpin DW, Furlong ET, Meyer MT, Thurman EM, Zaugg SD,
Effluent-impacted environmental
20
3
55
22
3
72
69
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
N
Y
Y
Y
Y
Y
Y
N
Y
N
N
Y
Y
Y
Y
Y
Y
Y
Y
Y
S5
Barber LB, Buxton HT. 2002. Pharmaceuticals, hormones, and other organic wastewater contaminants in the U.S. streams,
1999-2000: a national reconnaissance. Environ Sci Techol
36:1202-1211.
Kolpin D, Skopec M, Meyer M, Furlong E, Zaugg S. 2004. Urban contribution of pharmaceuticals and other organic wastewater contaminants to streams during differing flow conditions.
Sci
Total Environ 328:119-130.
Effluent-impacted environmental
1000 a 88
Environmental 500 46
Y
Y
Untreated NR 5
Kumar KS, Priya SM, Peck AM, Sajwan KS. 2010. Mass loadings of triclosan and triclocarbon from four wastewater treatment plants to three rivers and landfill in Savannah, Georgia, USA.
Arch Environ Con Tox 58:275-285.
Effluent NR 4
Environmental* 0.001
c 12
Lee KE, Barber LB, Furlong E, Cahill J, Kolpin D, Meyer M,
Zaugg S. 2004. Presence and distribution of organic wastewater compounds in wastewater, surface, ground, and drinking waters,
Minnesota, 2000-02. Scientific Investigation Report 2004 –5138.
United States Geological Survey, Reston, VA, USA. 48 p.
Lee KE, Langer S, Barber LB, Writer J, Ferrer I, Schoenfuss H,
Furlong E, Foreman W, Gray J, ReVello R, Martinovic D,
Woodruff O, Keefe S, Brown G, Taylor H, Ferrer I, Thurman E.
2009. Endocrine active chemicals, pharmaceuticals, and other chemicals of concern in surface water, wastewater-treatment plant effluent, and bed sediment, and biological characteristics in selected streams, Minnesota-design, methods, and data, 2009.
U.S. Geological Survey Data Series 575. United States
Geological Survey, Reston, VA, USA. 55 p.
Untreated
Effluent
Environmental
Finished
Effluent
50
50
50
50
5
6
8
73
47
37
Y
Y
Y
Y
Y
Y
Y
Y
N
N
Y
Y
Y Y Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
N
S6
N
N
N
N
Y
Y
N
N
Effluent-impacted environmental
Loraine G, Pettigrove ME. 2006. Seasonal variations in concentrations of pharmaceuticals and personal care products in drinking water and reclaimed wastewater in Southern California.
Environ Sci and Technol 40:687-695.
Environmental
Effluent
5
5
Martinet MC, Dahm C. 2005. Presence of pharmaceuticallyactive compounds in the Rio Grande and Riparian groundwater.
WQCC No. 08-13 (R). Final Report. University of New Mexico,
Alburqerque, NM, USA. 30 p.
Environmental
Finished
Effluent
16
43
250
125
125
25
6
13
15
3
McAvoy DC, Schatowitx B, Jacob M, Hauk A, Eckhoff WS. 2002.
Measurment of triclosan in wastewater treatment systems.
Environ Toxicol Chem 21:1323-1329.
Environmental
Untreated
25
NR
Montgomery Watson Harza. 2007. City of San Diego Advanced
Water Treatment Research Studies. Scientific Investigational
Report. Montgomery Watson Harza, San Diego, CA, USA. 57 p., with appendices.
Effluent
Effluent
Morrall D, McAvoy D, Schatowitz B, Inauen J, Jacob M, Hauk A,
Eckhoff W. 2004. A field study of triclosan loss rates in river water
(Cibolo Creek, TX). Chemosphere 54:653-660.
National Water Research Institute (NWRI). 2010. Source, fate and transport of endorcrine disruptors, pharmaceuticals, and personal care products in drinking water sources in California.
07-WQ-004. Final Report. National Water Research Institute,
Effluent
Effluent-impacted environmental
Environmental
NR
1
10
10
10
2
5
10
3
1
1
3
Y
Y
Y
Y
Y
Y
Y
Y
Y
N
Y
Y
Y
Y
Y
N
N
N
Y
Y
Y
Y
Y
N
N
NR
S7
Y
Y
Y
N
N
N
N
N
Y
Y
NR
N
N
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Fountain Valley, CA, USA. 140 p.
Effluent
Oblinger C, Gill A, McPherson A, Meyer M, Furlong E. 2005.
Occurrence of selected pharmaceuticals, personal-care products, organic wastewater compounds, and pesticides in the lower
Tallapoosa River Watershed near Montgomery, Alabama, 2005.
Scientific Investigations Report 2007 –5266. Scientific
Investigations Report. United States Geological Survey, Reston,
VA, USA. 24 p.
Environmental
Environmental
5
5
16
111
480 20 Y
Y
Y
Schaider L, Rudel R, Dunagan S, Ackerman J, Perovich L, Brody
J. 2010. Emerging contaminants in Cape Cod drinking water.
Final Report. Silent Spring Institute, Cape Cod, MA, USA. 40 p.
Environmental 50 20 Y
Shelver WL, Kamp LM, Church JL, Rubio FM. 2007.
Measurement of triclosan in water using a magnetic particle enzyme immunoassay. J Agric Food Chem 55:3758-3763.
Snyder SA, Wert EC, Rexing DJ, Zegers RE, Drury DD. 2006.
Ozone oxidation of endocrine disurptors and pharmaceuticals in surface water and wastewater. Ozone-Sci Eng 28:445-460.
Standley LJ, Rudel RA, Swartz CH, Attfield KR, Christian J,
Erickson M, Brody JG. 2008. Wastewater-contaminated
Finished
Untreated
Effluent
Untreated
Effluent
Untreated
Effluent
50 2
20 26
20 4
20 2
20 13
1 1
1 3
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
N Y N
Y
Y
N
N
N
Y
Y
Y
Y
Y
Y
Y
Y
Y
S8
N
N
Y
Y
N
N
N
Y
Y
N
groundwater as a source of endogenous hormones and pharmaceuticals to surface water ecosystems. Environ Toxicol
Chem 27:2457-2468.
Environmental 16 16
Thomas PM, Foster GD. 2005. Tracking acidic pharmaceuticals, caffeine, and triclosan through the wastewater treatment process.
Environ Toxicol Chem 24:25-30.
Untreated 6 9
Y
Y
Wert EC, Rosario-Ortiz F, Snyder S. 2009. Effect of ozone exposure on the oxidation of trace organic contaminants in wastewater. Water Res 43:1005-1014.
Effluent 6 3
Effluent 1 3
Xu J, Wu L, Chang AC. 2009. Degradation and adsorption of selected pharmaceuticals and personal care products (PPCPs) in agricultural soils. Chemosphere 77:1299-1305.
Yu JT, Bouwer EJ, Coelhan M. 2006. Occurrence of biodegradability studies of selected pharmaceuticals and personal care products in sewage effluent. Agr Water Manage
86:72-80.
Effluent
Effluent-impacted environmental*
Untreated
6
6
NR
Effluent NR
Yu CP, Chu KH. 2009. Occurrence of pharmaceuticals and personal care products along the West Prong Little Pigeon River in east Tennessee, USA. Chemosphere 75:1281-1286.
Untreated 38
Yu Y, Wu L. 2012. Analysis of endocrine disrupting compounds, pharmaceuticals and personal care products in sewage sludge by gas chromatography –mass spectrometry. Talanta 89:258-263.
Effluent
Environmental
Untreated
38
38
420
1
36
1
1
2
2
4
4
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
Y
N
Y
N
N
Y
Y
Y
Y
Y
Y
Y
Y
Y
N
Y
Y
Y
Y
N
N
N
Y
N
N
S9
Zhang S, Zhang Q, Darisaw S, Ehic O, Wang G. 2007.
Simultaneous quantification of polycyclic aromatic hydrocarbons
(PAHs), polychlorinated biphenyls (PCBs), and pharmaceuticals and personal care products (PPCPs) in Mississippi River water, in New Orleans, Louisiana, USA. Chemosphere 66:1057-1069.
Environmental 1.7 14
Zimmerman MJ. 2005. Occurrence of organic wastewater contaminants, pharmaceuticals, and personal care products in selected water supplies, Cape Cod, Massachusetts. Scientific
Investigations Report 2005-1206. United States Geological
Survey and United States Department of the Interior, Reston, VA,
USA. 20 p.
Untreated 1000 6
Y
Y
Y
Y
Y
Y
Y
N
Finished 1000 10 Y Y Y N
Snyder, S.A., Trenholm, R.A., Snyder, E.M., Bruce, G.M., Pleus,
R.C., Hemming, J.D.C. Toxicological Relevance of EDCs and
Pharmaceuticals in Drinking Water. 2008. Awwa Research
Foundation. ISBN 978-1-60573-040-0, pp. 484
Not included in the analysis: good sample size, but only mean values reported; authors contacted, but would not provide additional data; did not pass QC criteria
Gibbons SE, Wang C, Ma Y. Determination of pharmaceutical and personal care products in wastewater by capillary electrophoresis with UV detection. Talanta 2011, 84, 1163-1168.
Not included in the analysis: authors report an IDL that is three orders of magnitude greater than the
MDL; the MDL is the highest reported of all the studies; methods in question
Snyder, S.A. Occurrence, treatment, and toxicological relevance of EDCs and pharmaceuticals in water. Ozone: Science and
Engineering, 2008, 30, 65-69.
Not included in the analysis: only max and median reported; authors contacted, but would not provide additional data; did not pass QC criteria
NR = not reported
S10
4 a Reporting limit b Lowest reported estimated concentration was used since no
LOD was available c Reported in nanograms only
*Includes composite samples
*References cited in Table 1 of the primary article
5
S11
6 Table S2. Percentage of total samples collected by state.
Minnesota
California
Massachusetts
Illinois
Maryland
Several across US
Iowa
Alaska
Georgia
Texas
Ohio
Oregon
South Carolina
Louisiana
Colorado
Indiana
North Carolina
Alabama
Arkansas
Nevada
New Jersey
N State/Commonwealth % Total Samples
61
60
59
55
78
65
62
55
54
54
48
44
44
43
322
201
142
138
124
106
99
3.55%
2.95%
2.82%
2.77%
2.73%
2.68%
2.50%
2.50%
2.45%
2.45%
14.64%
9.14%
6.45%
6.27%
5.64%
4.82%
4.50%
2.18%
2.00%
2.00%
1.95%
S12
Pennsylvania
Utah
North Dakota
New York
Nevada/ Arizona
Virginia
Florida
New Mexico
Arizona
Missouri
Tennessee
Idaho
California/ Arizona
South Dakota
Oklahoma
Kansas
Montana
Washington
Hawaii
Nebraska
Puerto Rico
Michigan
Connecticut
7
7
6
6
6
10
10
10
9
7
26
20
19
15
35
33
28
4
3
2
5
4
4
0.45%
0.45%
0.45%
0.41%
0.32%
0.32%
0.32%
0.27%
0.27%
0.27%
1.59%
1.50%
1.27%
1.18%
0.91%
0.86%
0.68%
0.23%
0.18%
0.18%
0.18%
0.14%
0.09%
S13
7
8
2
2
2
1
Wisconsin
Delaware
Maine
New Hampshire
0.09%
0.09%
0.09%
0.05%
S14
9 Statistical Analysis.
TCS data were tested for distribution fit using the Shapiro-Wilk
10 goodness-of-fit test for a normal, lognormal, and gamma distribution. All water types
11 were found to have lognormal distributions a 95% confidence level, with the exception
12 of the untreated water values. However, the distribution of untreated waters was
13 determined to be best approximated by a lognormal distribution when compared to
14 probability plots for the normal, lognormal and gamma distribution (Figure S1). In brief,
15 reported data, using the reported limit of detection or reporting limit for non-detect
16 values, were used for the ROS analysis in ProUCL. For ANOVA, the LnROS values
17 were transformed using the natural log prior to statistical analysis. The ROS method is
18 suited for datasets with multiple limits of detection and has been shown to produce
19 robust estimates of the mean and standard deviation, particularly in situations where
20 there is departure from a lognormal distribution {Baccarelli, 2005 #257;Huybrechts,
21 2002 #258;Lubin, 2004 #259}. Histograms using the LnROS imputed data for each
22 water classification are shown in Figure S2.
23
24
25
26
S15
27 Figure S1. Lognormal Q-Q Plot for normal, lognormal, and gamma ROS estimates
28 for untreated waters.
29
30
31
S16
32 Figure S2. Histograms of natural log transformed TCS sample concentration
33 including values imputed by the lognormal ROS method by water type.
34
50
40
30
20
10
0
4 6 8
Ln Untreated (ng/L)
10 12
25
20
15
10
5
0
-2 0 2 4
Ln Effluent (ng/L)
6 8
35
30
20
10
0
50
40
1 2 3 4 5
Ln Effluent-Impacted (ng/L)
6 7 8
140
120
100
80
60
40
20
0
-6 -4 -2 0 2
Ln Environmental (ng/L)
4 6
36
50
40
30
20
10
37
38
0
-20 -15 -10 -5
Ln Finished (ng/L)
0 5
S17
39
40
41
References
[1] Baccarelli A, Pfeiffer R, Consonni D, Pestatori AC, Bonzini M, Patterson Jr. DG,
42 Bertazzi PA, Landi MT. 2005. Handling of dioxin measurement data in the presence of
43 non-detectable values: Overview of available methods and their application in the
44 Seveso chloracne study. Chemosphere 60:898-906.
45 [2] Huybrechts T, Thas O, Dewulf J, Van Langenhove H. 2002. How to estimate
46 moments and quantiles of environmental data sets with non-detected observations? A
47 case study on volatile organic compounds in marine water samples. Journal of
48 Chromatography A 975:123-133.
49 [3] Lubin JH, Colt JS, Camann D, Davis S, Cerhan JR, Severson RK, Berstein L,
50 Hartge P. 2004. Epidemiologic evaluation of measurement data in the presence of
51 detection limits. Environmental Health Perspectives 112:1691-1696.
52 [4] Minnesota Department of Public Health (MDH). 2010. 2010 Health Based Value
53 for Water: Triclosan. Environmental Health Division, St. Paul.
54 [5] United States Environmental Protection Agency (USEPA). 1999. 5-chloro-2-(2,4-
55 dichlorophenoxy)phenol (triclosan): Request for dietary risk assessment. Office of
56 Prevention, Pesticides and Toxic Substances, Washington, D.C.
57 [6] Capdevielle M, Van Egmond R, Whelan M, Versteeg D, Hormann-Kamensky M,
58 Inauen J, Cunningham V, Woltering D. 2008. Consideration of exposure and species
59 sensitivity of triclosan in the freshwater environment. Integrated Environmental
60 Assessment and Management 4:15-23.
S18
61 [7] Lyndall J. 2010. Probabilistic risk evaluation for triclosan in surface water,
62 sediments, and aquatic biota tissues. Integrated Environmental Assessment and
63 Management 6:419-440.
64 [8] Wilson BA, Smith VH, De Noyelles FJ, Larive CK. 2003. Effects of three
65 pharmaceutical and person care products on natural freshwater algal assemblages.
66 Environmental Science and Technology 37:1713-1719.
67 [9] Orvos D, Versteeg D, Inauen J, Capdevielle M, Rothenstein A, Cunningham V.
68 2002. Aquatic toxicity of triclosan. Environmental Toxicology and Chemistry 21:1338-
69 1349.
70 [10] Singer H, Muller S, Tixier C, Pillonel L. 2002. Triclosan: Occurence and fate of a
71 widely used biocide in the aquatic environment: Field measurements in wastewater
72 treatment plants, surface waters, and lake sediments. Environmental Science and
73 Technology 36:4998-5004.
74 [11] Veldhoen N, Skirrow R, Osachoff H, Wigmore H, Clapson D, Gunderson M,
75 Aggelen G, Helbing C. 2006. The bactericidal agent triclosan modulates thyroid
76 hormone-associtated gene expression and disrupts postembryonic anuran
77 development. Aquatic Toxicology 80:217-227.
78 [12] von der Ohe PC, Schmitt-Jansen M, Slobodnik J, Brack W. 2011. Triclosan
—the
79 forgotten priority substance? Environmental Science and Pollution Research 9:585-589.
80
81
S19
82
S20