The uncertainty of the entire method (sampling, sample preparation, detection) was calculated according to Eurachem CITAC guidelines (EURACHEM / CITAC guide CG 04, 2000). Uncertainties were only calculated for the frequently detected analytes (ADBI, AHMI, HHCB, AHTN and BDE183). Method uncertainties for PFCs were reported by Dreyer et al. (2009).
Table S14: Combined and expanded uncertainty (pg m-3) on the basis of high-concentration samples from waste water treatment plants (n=10).
Table S15: PFC concentrations (pg m-3) in gas-phase samples collected at WA and WB and the corresponding reference sites. n.d.: not detected, a values were corrected by average recovery rates of 13C 6:2 FTOH. Asterisks mark the 3-day samples.
4:2 FTOH
6:2 FTOH
8:2 FTOH
10:2 FTOH
12:2 FTOH
6:2 FTA
8:2 FTA
10:2 FTA
Me2FOSA
EtFOSA
MeFBSA
MeFOSA
PFOSA
MeFOSE
MeFBSE
EtFOSE
WA1
n.d.
16
59
27
55
11
4
21
n.d.
4
n.d.
9
n.d.
1
n.d.
2
WA2
7
29
85
22
33
8
4
15
n.d.
11
n.d.
10
n.d.
2
n.d.
3
WA3
n.d.
15
41
11
6
10
3
2
n.d.
3
n.d.
4
n.d.
1
3
n.d.
WA4*
n.d.
n.q.
36
19
6
n.d.
n.d.
2
n.d.
18
n.d.
5
n.d.
2
5
3
WA5
n.d.
25
91
22
12
11
3
3
n.d.
3
n.d.
n.q.
n.d.
6
7
2
WB1
n.d.
112 a
216
51
34
n.d.
20
28
n.d.
55
27
16
n.d.
7
n.d.
3
WB2*
n.d.
12 a
124
35
14
n.d.
3
4
n.q.
51
23
6
n.d.
4
5
9
WB3
n.d.
120 a
143
31
17
n.d.
7
8
n.d.
31
34
8
n.d.
2
n.d.
n.d.
WB4
n.d.
225 a
419
66
29
n.d.
35
33
n.d.
69
61
10
n.d.
4
7
3
WB5
n.d.
259 a
350
77
30
n.d.
49
56
n.d.
61
60
54
n.d.
2
5
n.d.
RA1
n.d.
13
34
14
8
n.d.
3
3
n.d.
3
n.d.
6
n.d.
1
5
n.d.
RA2
n.d.
9
130
19
8
4
4
3
n.d.
3
n.d.
4
n.d.
1
5
1
RA3
n.d.
7
62
11
6
5
1
2
n.d.
3
n.d.
4
n.d.
1
3
n.d.
RA4*
n.d.
8
31
12
3
9
1
1
n.d.
2
n.d.
n.q.
n.d.
3
3
1
RA5
n.d.
8
26
9
5
n.d.
n.d.
n.d.
n.d.
9
n.d.
10
n.d.
1
5
3
RB2*
n.d.
34 a
75
48
20
n.d.
3
2
n.d.
1
3
3
n.d.
2
3
n.d.
RB3
n.d.
4 a
45
14
7
7
4
2
n.d.
2
3
4
n.d.
n.d.
n.d.
n.d.
RB4
n.d.
45
176
58
24
13
6
3
n.d.
3
4
9
n.d.
4
n.d.
2
RB5
n.d.
4 a
7
3
2
n.d.
3
n.d.
n.d.
1
n.d.
n.d.
n.d.
2
n.d.
n.d.
Table S16: PFC concentrations (pg m-3) in particle-phase samples collected at WA and WB and the corresponding reference sites. n.d.: not detected, n.q.: not quantified. Asterisks mark the 3-day samples.
PFBS
PFHxS
PFOS
PFBA
PFPA
PFHxA
PFHpA
PFOA
PFNA
PFDA
PFUnDA
PFDoDA
PFOSA
WA2
n.d.
n.d.
0.2
8.4
n.q.
0.5
0.1
1.3
n.d.
0.2
0.1
0.2
1.9
WA3
n.d.
n.d.
0.5
6.5
0.1
0.2
n.d.
1.1
0.1
0.1
0.1
0.1
1.5
WA4*
n.d.
n.d.
0.4
1.4
n.d.
n.d.
n.d.
n.d.
0.1
n.d.
n.d.
0.1
0.6
WA5
0.2
0.7
0.9
6.5
0.2
0.4
0.1
0.5
0.3
0.0
0.1
0.1
0.9
WB1
n.d.
n.d.
0.0
0.5
n.d.
n.q.
n.d.
n.d.
0.2
0.3
n.d.
n.d.
0.6
WB3
0.1
n.d.
0.2
2.8
n.d.
n.d.
n.d.
0.6
0.3
0.2
n.d.
n.d.
0.9
WB4
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WB5
0.2
n.d.
0.5
n.q.
n.d.
n.d.
n.d.
1.1
0.5
0.6
n.d.
n.d.
0.9
RA2
n.d.
0.0
0.1
2.6
0.4
0.3
0.1
0.3
0.3
0.1
0.1
0.2
0.2
RA3
0.1
0.2
0.6
5.6
0.4
0.3
0.1
0.2
n.q.
0.1
0.1
0.1
0.3
RA4*
n.d.
n.d.
0.1
n.d.
n.d.
n.d.
n.d.
n.d.
n.q.
n.d.
n.d.
n.d.
n.q.
RA5
0.9
2.0
1.8
5.4
1.8
1.6
1.0
3.4
0.9
2.1
0.8
1.1
1.7
RB1
1.9
n.d.
2.9
5.7
4.7
3.3
2.8
2.1
1.9
1.7
n.d.
n.d.
n.d.
RB3
0.2
n.d.
0.6
7.2
n.d.
0.5
0.1
0.4
n.d.
n.d.
n.d.
n.d.
n.d.
RB4
n.d.
n.d.
1.0
6.6
1.2
0.6
n.d.
0.5
n.d.
n.d.
n.d.
n.d.
n.d.
RB5
n.q.
n.d.
n.d.
1.7
n.d.
n.q.
n.d.
n.q.
n.d.
n.d.
n.d.
n.d.
n.d.
c
d
Figure S3: Concentrations (pg m-3) of ionic PFCs in particle-phase samples taken at two WWTPs WA (a) and WB (b) and at the corresponding reference sites (b, d). Sampling periods: 0.4.08.-11.08.2009 (WA) and 20.08.- 27.08.2009 (WB). Samples WA1, RA1, WB2 and RB2 were not analysed because of breaking of measurement vials during centrifugation. WB4 is
a
b
Table S17: Musk fragrance concentrations (pg m-3) in gas-phase samples collected at WA and WB and the corresponding reference sites. n.d.: not detected. Asterisks mark the 3-day samples.
ADBI
AHMI
HHCB
ATII
MX
AHTN
MK
WA1
48
16
5157
n.d.
n.d.
304
n.d.
WA2
76
142
66715
n.d.
n.d.
3972
n.d.
WA3
11
20
8621
n.d.
n.d.
556
n.d.
WA4*
97
880
119644
n.d.
n.d.
6106
n.d.
WA5
348
90
45128
n.d.
n.d.
2539
n.d.
WB1
454
1760
55181
n.d.
n.d.
17967
n.d.
WB2*
181
88
190216
n.d.
n.d.
44126
n.d.
WB3
1328
4213
406625
n.d.
n.d.
45556
n.d.
WB4
1576
5164
264112
n.d.
n.d.
44831
n.d.
WB5
1741
6551
407194
n.d.
n.d.
65063
n.d.
RA1
n.d.
n.d.
250
n.d.
n.d.
46
n.d.
RA2
n.d.
n.d.
308
n.d.
n.d.
44
n.d.
RA3
n.d.
n.d.
63
n.d.
n.d.
10
n.d.
RA4*
n.d.
n.d.
831
n.d.
n.d.
131
n.d.
RA5
n.d.
n.d.
179
n.d.
n.d.
33
n.d.
RB1
n.d.
n.d.
104
n.d.
n.d.
12
n.d.
RB2*
8
n.d.
296
n.d.
n.d.
47
n.d.
RB3
6
n.d.
300
n.d.
n.d.
38
n.d.
RB4
n.d.
n.d.
226
n.d.
n.d.
34
n.d.
RB5
12
n.d.
718
n.d.
n.d.
96
n.d.
Table S18: Musk fragrance concentrations (pg m-3) in particle-phase samples collected at WA and WB and the corresponding reference sites. n.d.= not detected. Asterisks mark the 3-day samples.
ADBI
AHMI
HHCB
ATII
MX
AHTN
MK
WA1
14
13
169
n.d.
n.d.
60
n.d.
WA2
9
8
75
n.d.
n.d.
18
n.d.
WA3
3
3
34
n.d.
n.d.
8
n.d.
WA4*
11
8
436
n.d.
n.d.
59
n.d.
WA5
14
9
404
n.d.
n.d.
108
n.d.
WB1
7
6
272
n.d.
n.d.
30
n.d.
WB2*
n.d.
n.d.
6
n.d.
n.d.
11
n.d.
WB3
11
9
850
n.d.
n.d.
115
n.d.
WB4
12
11
467
n.d.
n.d.
70
n.d.
WB5
22
20
1362
n.d.
n.d.
211
n.d.
RA1
n.d.
n.d.
3
n.d.
n.d.
4
n.d.
RA2
n.d.
n.d.
11
n.d.
n.d.
12
n.d.
RA3
n.d.
n.d.
9
n.d.
n.d.
11
n.d.
RA4*
n.d.
n.d.
7
n.d.
n.d.
8
n.d.
RA5
n.d.
n.d.
8
n.d.
n.d.
16
n.d.
RB1
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB2*
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB3
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB4
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB5
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
Table S19: PBDE concentrations (pg m-3) in gas-phase samples collected at WA and WB and the corresponding reference sites. n.d.: not detected. Asterisks mark the 3-day samples.
BDE28
BDE47
BDE100
BDE99
BDE153
BDE154
BDE183
WA1
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WA2
n.d.
n.d.
n.d.
n.d.
n.d.
1.9.
2.1
WA3
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WA4*
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WA5
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WB1
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WB2*
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WB3
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WB4
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
WB5
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RA1
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RA2
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RA3
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
4.3
RA4*
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RA5
n.d.
n.d.
n.d.
n.d.
n.d.
2.3
3.9
RB1
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB2*
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB3
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB4
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
RB5
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
n.d.
Table S20: PBDE concentrations (pg m-3) in particle-phase samples collected at WA and WB and the corresponding reference sites. n.d.: not detected. Asterisks mark the 3-day samples.