Zhiqiang Nie
1
, Qingqi Die
1
, Yufei Yang
1
, Zhenwu Tang
2
, Qi Wang
1
, Qifei Huang
1*
1.
Key Laboratory of Environmental Criteria and Risk Assessment, Chinese
Research Academy of Environmental Sciences, Beijing 100012, China
2.
MOE Key Laboratory of Regional Energy and Environmental Systems
Optimization, Resources and Environmental Research Academy, North China
Electric Power University, Beijing 102206, China
1.
Table S1 Comparative concentrations of PCDD/PCDF in air, water soils and sediments measured in this study and reported for other areas in China and other countries
2.
Table S2 Meteorological information and collecting data for the five air sampling sites around the upper reaches of Haihe River basin, China
3.
Table S3 Air and water concentrations of PCDD/PCDF surrounding the upper reaches of Haihe River basin, China (fg/m 3 or pg/L)
4.
Table S4 Average concentrations of PCDD/PCDF and TOC in the different soils used for the ff s
calculation (pg/g)

Fugacity is a measure of the chemical potential or partial pressure of a particular compound
to escape from one medium to another (Mackay 2001); it has been used to investigate the
air-water/soil equilibrium status of many POPs, such as organochlorine pesticides (OCPs) and
polychlorinated biphenyls (PCBs) (Li et al. 2009, Lin et al. 2012, Ru
Žic ková et al. 2007). To
estimate the equilibrium status using fugacity, measurements of the chemical’s gaseous concentration near the atmospheric boundary layer and its corresponding concentration in surface water or soil are needed. Fugacity values can be calculated using the fugacity capacities and the
concentrations in the two compartments (Backe et al. 2004, Bidleman &Leone 2004, Meijer et al.
2003)
.
1.1 Air-water exchange
The dynamics of air–water exchange for semi-volatile compounds can be explored by rationing the fugacity of the chemical in the respective water and air phases, with knowledge of the temperature-dependent Henry's Law constant (H) and ambient air and surface water
temperatures (Falconer et al. 1995). Air–water fugacity ratios were calculated from relationships
given in equation: ff w
= ff w ff w
+ ff a
=
C w
H
C w
H+ C a
RT
Where C a
is the gaseous concentration (mol/m 3 ), C w
is the dissolved aqueous concentration
(mol/m 3 ), R is the gas constant (8.314 Pa·m3/mol·K), T is the ambient air temperature (K) and H is the Henry's law constant of PCDD/PCDF homologues (Pa·m 3
/mol) (Srogi 2008).
1.2 Air-soil exchange
Air ( f a
) and soil ( f s
) fugacity (Pa) of PCDD/PCDF were calculated using the following equations
(Bidleman &Leone 2004, Mackay 2001):
f a
= C a
R T (1) f s
= C s
R T /(0.411
ρ s
φ soc
K oa
) (2) where C a
and C s
are the PCDD/PCDF concentrations in the air and soil (mol/m 3 ), respectively,
R is gas constant (8.314 Pa m 3 /mol/K), T is the average absolute air temperature (K), ρ s
is the soil density (assuming 2.5 kg/L), φ soc
is the organic carbon fraction in the soil, and K oa
is the
octanol-air partition coefficient of congener. Empirical studies (Meijer et al. 2003)
have proved that a coefficient of 0.411
can improve the correlation between the soil-air partition coefficient
( K sa
) and K oa
. The K oa
for all of the PCDD/PCDF were taken from (Meylan &Howard 2005)
at the actual average temperature is 25 ºC.
Meijer et al. (2003), as well as Bidleman and Leone (2004), have used the fugacity fraction
( ff s
, defined as a ratio of soil fugacity to the sum of soil fugacity and air fugacity, equation (3)) as an indication of the net direction of air-soil exchange. ff s
= f s
/( f s
+ f a
) = C s
/( C s
+ 0.411
ρ s
φ soc
K oa
C a
) (3)
A fugacity fractions equal to 0.5 indicates equilibrium; ff >0.5 indicates net volatilization

from the soil into air, whereas ff < 0.5 indicates net transport from air to soil. If the ff value is close to 0 or 1, there will be a tendency for the chemical to move from one compartment to the other to establish equilibrium. However, due to uncertainties and the propagation of potential errors in the calculation, ff in the range of 0.3-0.7 was not considered to differ significantly from equilibrium
(Harner et al. 2001, Meijer et al. 2003, Ru
Žic ková et al. 2007).

Table S1 Comparative concentrations of PCDD/PCDF in air, water soils and sediments measured in this study and reported for other areas in China and other countries
Table S2 Meteorological information and collecting data for the five air sampling sites around the upper reaches of Haihe River basin, China
Table S3 Air and water concentrations of PCDD/PCDF surrounding the upper reaches of Haihe River basin, China (fg/m
3
or pg/L)
Table S4 Average concentrations of PCDD/PCDF and TOC in the different soils used for the ff s
calculation (pg/g)

Concentrations of PCDD/PCDF in air, water, soils and sediments measured in this study and reported for other rivers, coasts, and lakes in China and other countries
Matrix Location Concentration TEQ References
Air
(fg/m 3 )
Beiyun River, China
Thau lagoon, France
Lake Maggiore (LM) in Northern Italy
589-13,680 (4,855)
300-1,400
31.2-560 (203)
16-26
25
Malopolska Region, southern Poland northern Algeria
Ispra EMEP site, Northern Italy
Shanghai, China
Beijing, China
Guangzhou, China
Tangshan, China
Dalian, China
Hong Kong
Taiwan
600-37,000
3520-16,280 (9,635)
50 – 3,080
99-20,760 (5,388)
275-10,780 (4,355)
2023-22619 (8,447)
612-3,819 (2,005)
5,258-5,563 (5,411)
-
-
37–2,900
214-775 (474)
1–215
2.2-1214.9 (283.4)
18–644 (268)
56.7-1279.6 (364.3)
44.2-394.1 (169.9)
459.3-478.7 (469)
Winter: 32-430 , Summer: 18-25
Winter: 188-348 , Summer: 56-166
In this study
(Castro-Jiménez et al. 2008a)
(Castro-Jiménez et al.
2008b)
(Umlauf et al. 2010)
(Moussaoui et al. 2012)
(Castro-Jiménez et al. 2012)
(Li et al. 2008a)
(Li et al. 2008b)
(Yu et al. 2006)
(Ren et al. 2011)
(Wang et al. 2011)
(Sin et al. 2002)
(Chang et al. 2003)
Water
(pg/L)
Beiyun River, China
Thau lagoon, France
River Vene (Thau Lagoon), France
Coastal areas, Japan
Coastal area in Matsuyama, Japan
Rivers area in Matsuyama, Japan
Ponds in Matsuyama, Japan
Venice Lagoon, Italy
Raritan Bay/Houdson River Estuary, USA
4.9–22.4 (9.5)
0.16–0.48
2.78
1.3–2.9
15–170 (51)
ND a –1,500 (180)
44–530 (260)
3–31
2.35
0.12–1.1 (0.46)
0.004–0.009
0.053
--
--
--
--
--
0.085–0.16
In this study
(Castro-Jiménez et al. 2008a)
(Hashimoto et al. 1995)
(Seike et al. 1998)
(Dalla Valle et al. 2003)
(Lohmann et al. 2000)

Port Jackson (Sydney Harbour), Australia
Elbe River, Germany
Lake Rotorua (Utuhina upstream and downstream), New Zealand
Lake Rotorua (Puarenga Stream), New Zealand
Xijiang River, China
Beijiang River, China
Three Gorges Reservoir, China
Ya-Er Lake, China
Yangtze River basin, China
Beiyun River, China
Haihe River, North China
PCDDs: 2.4–84
PCDFs: 0.15–7.2
0.12–0.28
--
--
2.7–4.6
1.4–114
2–96 (11.9)
17.2–22.5 (19.9)
10.7–131 (34.3)
10.7
– 302 (99.2)
11.6–1,180,924
Sediments
(pg/g dw)
Haihe River, North China
Dagu Drainage River, North China
Nanpaiwu River, North China
Daliao River, Northeast China
Liaohe River, Northeast China
Yellow Sea region of China
Shandong Peninsula, China
Pearl River Delta, South China
Pearl River Delta, South China
Dongjiang River, South China
Taihu Lake, China
151–11,546 (2013)
1,962–556,961 (201290)
430–8,714,500 (895449)
29.1–3,039 (864)
13.7–458.5 (121.9)
ND–166.8
6.2–27.4
--
2,003–4,314 (2,794)
2,100–5,400 (3,600)
120.1–1315
Ya-Er Lake, China 5,713–13,845
0.07–1.85
0.004–0.017
1.2–1.3
5.4
0.012–0.075 (0.39)
--
0.0008–0.32 (0.063)
0.11–0.4 (0.25)
0.45–10.0 (2.34)
0.17
– 7.7 (2.2)
0.3–3,319 (sum of PCDD/PCDF and PCBs)
1.3–26 (8.6)
19–1,264 (525.7)
21–22,000 (3,056)
0.28–29.0 (7.45)
0.17–14.9 (2.15)
0.11–0.8
0.6–17.5 (6.4)
0.45–9.46 (5.31)
4.3–10.6 (7.1)
0.83–17.7 (sum of PCDD/PCDF and PCBs)
10–420
(Roach et al. 2009)
(Götz et al. 1994)
(Gifford et al. 1996)
(Liu et al. 2008)
(Mou 2010)
(Chen et al. 2008)
(Wu et al. 2001a)
(Nie et al. 2013)
In this study
(Li et al. 2012)
(Liu et al. 2007)
(Hu et al. 2005)
(Zhang et al. 2008)
(Zhang et al. 2010)
(Naile et al. 2011)
(Pan et al. 2010)
(Zheng et al. 2001)
(Zhang et al. 2009a)
(Ren et al. 2009)
(Zhang &Jiang 2005)
(WU et al. 2001b)

Soils
(pg/g)
Yangtze River basin, China
Beiyun River, China
Haihe River, China
Yoneshiro River basin, Japan
Trondheim, Norway
Pearl River Delta, China
Daliao River Basin, China
Chuang-Zhu-Tan urban agglomeration, China a ND: Not detected
42.4–928 (355)
11.4-275 (56.4)
0.31–51 (5.25)
0.29-5.90 (1.25)
77.9-9,095 (1884) 0.75-33.6 (8.67)
15,000-230,000 (83,000) 3.0-380 (87.1)
0.16 - 14
97.6 - 9,600 (2,299) 0.28–15.2 (3.62)
21.8-8,744 (1,005)
268-7,510 (2,156)
0.31 - 53.05
0.9-10 (4.8)
(Nie et al. 2013)
In this study
(Kobayashi et al. 2008)
(Andersson &Ottesen 2008)
(Zhang et al. 2009b)
(Zhang et al. 2008)
(Yang et al. 2012)

Table S2 Meteorological information and collecting data for the five air sampling sites around the upper reaches of Haihe River basin, China
Sampling site
Sampling date
Latitude (N°)
Longitude (E°)
Time (h)
Volume (m 3 )
Average temperature (
℃
)
TSP (μg/m 3 )
A1
39°55.430′
116°39.724′
72
2304
25
335
A2 A3
7/7/2011-20/7/2011
A4 A5
39°44.895′ 39°37.424′ 39°15.759′ 39°13.167′
116°46.492′ 116°59.084′ 117°05.804′ 117°07.616′
72
2046
72
2066
72
2152
72
2226
27
480
28
458
24
507
22
770

Table S3 Air and water concentrations of PCDD/PCDF surrounding the upper reaches of Haihe
River basin, China (fg/m 3 or pg/L)
Homologues
TeCDF
PeCDF
HxCDF
HpCDF
OCDF
TeCDD
PeCDD
HxCDD
HpCDD
OCDD
Air and water concentrations (fg/m 3 or pg/L)
A1 A2 A3 A4 A5 W1 W2 W3 W4 W5
291 957 275 1572 2183 0.69
0.69
0.58
0.68
2.44
200 799 134 1667 2505 0.72
1.19
0.54
1.17
2.56
223 1113 226 2245 4241 1.27
0.76
0.63
3.28
6.91
184 1057 246 2188 4941 1.37
1.50
0.74
2.84
6.04
131 872 171 1094 2817 0.98
1.08
0.72
4.44
1.61
58.1
179 45.6
406 448 0.54
1.90
0.31
0.60
4.76
84.9
259 61.7
999 1403 0.52
1.39
0.19
0.91
1.89
129 546 165 1985 3332 0.99
0.93
0.67
3.10
3.77
103 538 155 1661 3391 1.19
2.18
1.18
3.56
3.43
92.2
649 140 983 2083 1.54
2.93
2.8
7.95
1.99

Table S4 Average concentrations of PCDD/PCDF and TOC in the different soils used for the ff s calculation
Soil Site
TeCDF
PeCDF
S1-S4
6.6
± 2.1
a
2.8
± 2.8
S5-S6
13.3
6.4
±
±
Soil Concentrations (pg/g)
6.7
2.0
S7-S10
9.0
4.5
±
±
4.6
2.7
S11-S12 S13-S14
22.4
± 2.5 58.2
± 44.3
20.0
± 3.7 38.6
± 35.9
HxCDF
HpCDF
OCDF
TeCDD
3.9
± 0.9
2.6
± 0.7
3.8
± 0.8
3.0
± 0.8
5.3
5.5
9.4
4.6
±
±
±
±
2.8
3.4
6.8
2.7
4.3
3.4
4.7
3.2
±
±
±
±
1.9
1.7
4.0
1.7
18.9
15.3
24.4
10.6
±
±
±
±
1.2
2.8
6.3
2.7
29.5
24.4
39.0
18.2
±
±
±
±
26.7
22.6
32.6
14.0
PeCDD
HxCDD
HpCDD
OCDD
TOC (g/kg)
1.3
± 0.5
2.2
± 0.6
2.9
± 1.0
1.7
± 0.6
3.7
± 1.8
5.9
± 2.5
2.3
± 1.2
2.6
± 1.2
4.1
± 1.1
6.7
± 0.1 12.6
± 11.8
10.1
± 1.0 17.1
± 17.7
9.5
± 0.7 20.9
± 21.4
6.6
± 8.1 13.3
± 0.2 9.0
± 12.4 22.4
± 0.8 58.2
± 45.6
1.6
± 0.6 3.9
± 0.5 3.1
± 0.3 2.5
± 0.1 3.0
± 1.6
Air sampling site a
Standard deviation
A1 A2 A3 A4 A5

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