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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

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S18

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S19

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S20

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