Distribution, Fate and Risk Assessment of Antibiotics in Five Wastewater Treatment Plants

Appendix

Distribution, fate and risk assessment of antibiotics in five wastewater treatment plants in Shanghai, China

Minghong Wu a,b, Chenjing Que a, Liang Tang a, Hui Xu a, Jiajia Xiang a, Jiajun Wang a, Wenyan Shi a,*, Gang Xu a,*

a School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, Shanghai 200444, China

b Shanghai Applied Radiation Institute, Shanghai University, 99 Shangda Road, Shanghai 200444, China

* Corresponding author at: School of Environmental and Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, China. Tel.: +86 21 66137801; fax: +86 21 66137801

E-mail addresses: (M. Wu), (C. Que), (L. Tang), (H. Xu), (J. Xiang), (J. Wang), (W. Shi), (G. Xu).

Table S1Information of five WWTPs in this study

WWTP / Servedpopulation / Average dailyflow (m3/day) / Primary treatment process / Biological treatment process / Disinfection process
Plant A / 453000 / 240000 / Grit Chamber / Oxidation ditch / Ultraviolet
Plant B / 123000 / 60000 / Grit Chamber, Primary Clarifier / Anaerobic-Anoxic-Oxic / Ultraviolet
Plant C / 931600 / 400000 / Grit Chamber / Sequencing batch / Without tertiary treatment
Plant D / 931600 / 138000 / Grit Chamber, Primary Clarifier / Anaerobic-Anoxic-Oxic / NaClO
Plant E / 45000 / 20000 / Grit Chamber / Oxidation ditch / NaClO

Table S2LC-MS/MS parameters and Limits of quantification for 14 antibiotics and 1 surrogate standard

* The MRM transitions were used for quantification

Compound / Retention time(min) / MRM-transitions(m/z) / Fragment(V) / Collision energy(eV) / Limits of quantification(S/N=10)(ng/L)
Sulfadiazine / 1.95 / 251.1→108.1 / 114 / 21 / 1.87
251.1→156.0* / 14
Sulfamethoxazole / 4.67 / 254.1→92.1 / 118 / 34 / 0.76
254.1→156.1* / 14
Sulfamethazine / 2.92 / 279.1→92.1 / 118 / 26 / 0.48
279.1→124.1* / 30
Cefalexin / 2.36 / 348.2→106.0 / 82 / 29 / 4.80
348.2→158.0* / 5
Enrofloxacin / 6.33 / 360.2→245.1 / 148 / 29 / 0.71
360.2→342.2* / 22
Ofloxacin / 1.96 / 362.1→261.2* / 100 / 28 / 1.71
362.1→443.2 / 10
Amoxicillin / 1.11 / 366.1→113.9 / 91 / 17 / 2.56
366.1→349.0* / 5
Tetracycline / 2.56 / 445.2→410.1* / 132 / 18 / 2.37
445.2→427.2 / 20
Oxytetracycline / 2.10 / 461.2→426.1* / 123 / 18 / 1.37
461.2→443.2 / 20
Erythromycin / 15.35 / 734.5→116.1 / 140 / 54 / 0.01
734.5→158.1* / 35
Roxithromycin / 15.04 / 837.5→158.2* / 178 / 38 / 0.01
837.5→576.4 / 18
Spiramycin / 4.74 / 875.7→174.1 / 135 / 35 / 1.36
875.7→318.2* / 30
Chloramphenicol / 3.01 / 321.0→151.9* / 110 / 14 / 0.55
321.0→256.9 / 10
Thiamphenicol / 1.63 / 354.0→184.9 / 118 / 18 / 0.26
354.0→289.9* / 10
C13-Caffeine / 1.69 / 198.1→112.0 / 116 / 25 / 1.47
198.1→140.0* / 18

Table S3 Concentrations (ng/L) of 12 investigated antibiotics in fiveWWTPs in Shanghai, China

Plant A / Plant B / Plant C / Plant D / Plant E
IFa / EFb / IF / EF / IF / EF / IF / EF / IF / EF
SD / Winc,
Sumd / 58.39,
20.17 / 8.83,
2.22 / 105.79,
31.20 / 22.35,
13.79 / 411.32,
44.67 / 210.06,
8.04 / 189.23,
11.19 / 18.55,
8.17 / 91.29,
8.15 / 41.08,
8.52
SMX / Win,
Sum / 178.39,
85.17 / 56.78,
36.17 / 258.49,
98.72 / 41.86,
36.61 / 112.95,
132.78 / 28.05,
38.17 / 267.08,
85.84 / 33.58,
10.56 / 959.13,
9.17 / 106.60,
7.37
SMZ / Win,
Sum / 21.41,
54.56 / 0.69,
3.16 / 49.26,
10.09 / 31.35,
8.09 / 538.87,
42.16 / 127.08,
9.30 / 49.52,
11.62 / 17.25,
10.06 / 70.46,
5.65 / 34.20,
12.68
CFX / Win,
Sum / 96.10,
NDe / 11.12,
ND / 225.43,
ND- / 30.89,
ND / 126.47,
ND / 36.00,
ND / 341.80,
36.16 / 39.53,
25.16 / 316.22,
22.26 / 52.96,
20.24
AMOX / Win,
Sum / 675.25,
ND / 79.60,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND
ENR / Win,
Sum / ND,
ND / ND,
ND / ND,
ND / 3.87,
ND / 19.95,
ND / 35.11,
ND / 10.67,
ND / 14.28,
ND / ND,
20.53 / ND,
21.34
OFL / Win,
Sum / 587.50,
ND / 126.13,
ND / 1208.20,
ND / 800.37,
ND / 321.39,
ND / 916.88,
ND / 969.37,
ND / 290.08,
ND / 290.72,
821.16 / 159.03,
853.53
TC / Win,
Sum / 117.03,
ND / ND,
ND / 29.40,
ND / 26.15,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / 31.11,
ND
OTC / Win,
Sum / 537.57,
162.84 / ND,
16.70 / 153.26,
170.18 / 59.22,
72.64 / 346.21,
277.28 / 337.81,
125.17 / 564.30,
236.16 / 261.57,
151.52 / ND,
ND / ND,
ND
ERY / Win,
Sum / 27.78,
25.16 / 0.11,
1.66 / 1.77,
49.71 / 10.61,
10.08 / 37.62,
184.74 / 8.56,
47.40 / 2.01,
64.17 / 2.52,
25.16 / 3.25,
48.68 / 4.64,
53.28
ROX / Win,
Sum / 144.58,
63.16 / 21.38,
14.46 / 47.91,
112.96 / 78.85,
30.91 / 87.97,
186.16 / 54.50,
46.84 / 44.50,
79.20 / 28.54,
18.56 / 52.03,
17.12 / 29.26,
10.86
SPI / Win,
Sum / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / ND,
ND / 10.01,
ND / ND,
ND / ND.
ND / ND,
ND

a Influent.

b Effluent.

c Winter.

d Summer.

e Not Detected.

Table S4Concentrations of antibiotics in WWTPs of different countries/regions

Antibiotic / Cin(ng/L)a / Cef(ng/L)b / Country or region / Reference
SD / 58.39-411.32 / 8.83-210.06 / Shanghai / Current study
2.3-36 / 1.46-28.4 / Fujian, China / (Zhang et al. 2015)
NAc / 34.3 / Spain / (Diaz-Cruz et al. 2008)
3.7 / 1.9-3.8 / Japan / (Chang et al. 2008a)
Ndd-2900 / Nd-960 / Beijing, China / (Chang et al. 2008b)
SMX / 112.95-959.13 / 28.05-143.95 / Shanghai / Current study
<3-150 / <3-23 / UK / (Kasprzyk-Hordern et al. 2009)
<3 / 12 / UK / (Kasprzyk-Hordern et al. 2008)
80-1250 / 50-210 / USA / (Karthikeyan &Meyer 2006)
360-500 / 270-320 / Australia / (Watkinson et al. 2007)
250-3000 / 50-200 / Australia / (Watkinson et al. 2009)
380-2400 / 500-2600 / China / (Chang et al. 2008b)
230-570 / 270-320 / Switzerland / (Gobel et al. 2005)
5.41-11.5 / 2.96-137 / Fujian, China / (Zhang et al. 2015)
SMZ / 21.41-538.87 / 0.69-127.08 / Shanghai / Current study
Nd-251 / Nd-184 / Fujian, China / (Zhang et al. 2015)
CFX / 96.10-341.80 / 11.12-52.96 / Shanghai / Current study
670-2900 / 240-1800 / Hong Kong / (Gulkowska et al. 2008)
1563-4367 / 10-994 / Taiwan / (Lin et al. 2009)
4600e / ND / Australia / (Watkinson et al. 2007)
2800e / Nd-250 / Australia / (Watkinson et al. 2009)
AMOX / Nd-675.25 / Nd-79.60 / Shanghai / Current study
ND-280 / Nd-30 / Australia / (Watkinson et al. 2007)
NA / <1.80-120.4 / Italy / (Andreozzi et al. 2004)
ENR / Nd-20.53 / Nd-35.11 / Shanghai / Current study
Nd-11 / Nd-10.9 / Fujian, China / (Zhang et al. 2015)
10-100 / 10 / Australia / (Watkinson et al. 2007)
Nd-40 / 2-50 / Australia / (Watkinson et al. 2009)
OFL / 290.72-1208.20 / 126.13-1274.23 / Shanghai / Current study
91.5-129 / 12-24.6 / Fujian, China / (Zhang et al. 2015)
470 / 110 / USA / (Brown et al. 2006)
22.5 / 10 / Sweden / (Zorita et al. 2009)
TC / Nd-117.03 / Nd-85.23 / Shanghai / Current study
Nd-175 / Nd-34.8 / Fujian, China / (Zhang et al. 2015)
240-790 / 50-850 / USA / (Karthikeyan &Meyer 2006)
Nd-35 / Nd-30 / Australia / (Watkinson et al. 2007)
NA / 92-210 / Hongkong / (Minh et al. 2009)
OTC / Nd-564.30 / Nd-337.81 / Shanghai / Current study
Nd-75.8 / Nd-34.8 / Fujian, China / (Zhang et al. 2015)
Nd / Nd-20 / Australia / (Watkinson et al. 2007)
NA / <5-100 / Hongkong / (Minh et al. 2009)
ERY / 1.77-37.62 / 0.11-15.52 / Shanghai / Current study
1.12-1.67 / 1.2-4.4 / Fujian, China / (Zhang et al. 2015)
830 / 620 / Germany / (Ternes et al. 2007)
71-141 / 145-290 / UK / (Roberts &Thomas 2006)
ROX / 44.50-144.58 / 21.38-60.16 / Shanghai / Current study
Nd-175 / Nd-100 / Australia / (Watkinson et al. 2007)
NS / <85-120 / Hongkong / (Minh et al. 2009)
10-40 / 10-30 / Switzerland / (Gobel et al. 2005)

a Concentration of antibiotic in influent (ng/L).

b Concentration of antibiotic in effluent (ng/L).

c Not analyzed.

d Not detected.

eMedian concentration

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