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Science of the Total Environment 491–492 (2014) 51–59

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Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Atmospheric concentrations of persistent organic pollutants over the

Pacific Ocean near southern Taiwan and the northern Philippines
How-Ran Chao a, Ding-Yan Lin a, Kuang-Yu Chen b,⁎⁎, Yan-Yu Gou a, Tsyr-Huei Chiou c, Wen-Jhy Lee d,
Shui-Jen Chen a, Lin-Chi Wang e,⁎
a
Emerging Compounds Research Center, Department of Environmental Science and Engineering, National Pingtung University of Science and Technology, Neipu, Pingtung County 912, Taiwan
b
Taiwan Ocean Research Institute, National Applied Research Laboratories, Kaohsiung City 852, Taiwan
c
Department of Life Sciences, National Cheng Kung University, Tainan City 701, Taiwan
d
Department of Environmental Engineering, National Cheng Kung University, Tainan City 701, Taiwan
e
Department of Civil Engineering and Geomatics, Cheng Shiu University, Kaohsiung City 833, Taiwan

H I G H L I G H T S

• The world's first data on PBDD/Fs, PCDEs, and PBBs in the oceanic atmosphere
• Atmospheric POP TEQ levels over the target ocean were one order lower.
• PCBs and PBDEs were the dominant POPs in the global oceanic atmosphere.
• Atmospheric POPs over the target ocean were influenced by combustion sources.

a r t i c l e i n f o a b s t r a c t

Article history: This study investigates the atmospheric occurrence of persistent organic pollutants (POPs) over the Pacific Ocean
Received 13 November 2013 near southern Taiwan and the northern Philippines. We determined sixty-six compounds, including
Received in revised form 7 March 2014 polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), dioxin-like polychlorinated biphenyls
Accepted 7 March 2014
(DLPCBs), polybrominated diphenyl ethers (PBDEs), as well as polychlorinated diphenyl ethers (PCDEs),
Available online 28 March 2014
polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs), and polybrominated biphenyls (PBBs), in air
Editor: D. Barcelo samples simultaneously collected from the offshore oceanic atmosphere (n = 6) and over a rural area (n = 2).
We calculated the atmospheric World Health Organization 2005 toxic equivalency levels (WHO2005-TEQ), for
Keywords: the total dioxin-like POPs, including PCDD/Fs, DLPCBs, and PBDD/Fs, being 0.00612 pg WHO2005-TEQ/m3 and
Ocean 0.0138 pg WHO2005-TEQ/m3 over the ocean and land, respectively. We found unexpected lower averaged
Atmosphere atmospheric PBDE concentrations in the rural area (15.9 pg/m3) than over the ocean (31.1 pg/m3) due to higher
Persistent organic pollutants (POPs) levels of the BDE209 congener, although the difference was not statistically significant. We have compared and
Dioxins reported our field results with previously published datasets over the global oceans, which suggest PCBs and
Polybrominated diphenyl ethers (PBDEs)
PBDEs are the dominant chemical contaminants in the global oceanic atmosphere among these halogenated
Polychlorinated biphenyls (PCBs)
POPs (e.g. PCBs and Σdi-hepta PBDEs could be found in the range of 0.09–48.7 and 8.07–94.0 pg/m3, respectively,
including our dataset). However, there are still very few investigations on the global atmospheric levels of
PBDD/Fs, PCDEs and PBBs and our data sums to these earlier studies. Finally, we point out that the halogenated
POPs originated from Taiwan or the continental East Asia which could easily reach remote ocean sites via
atmospheric transport.
© 2014 Elsevier B.V. All rights reserved.

1. Introduction

Halogenated persistent organic pollutants (POPs) are a global con-

⁎ Correspondence to: L.-C. Wang, Department of Civil Engineering and Geomatics,
Cheng Shiu University, 840 Chengcing Road, Kaohsiung City 833, Taiwan. Tel.: +886 7
7310606x3045; fax: +886 7 7332204.
⁎⁎ Correspondence to: K.-Y. Chen, No 219 Sec 1 Dongfang Road, Taiwan Ocean Research
Institute, Kaohsiung City 852, Taiwan. Tel.: +886 7 6986886x124; fax: +886 7 6986656.
E-mail addresses: littlefish3@short.idv.tw (K.-Y. Chen), lcwang@csu.edu.tw (L.-C. Wang).
cern because of their negative impacts on the environment and health
of humans and other animals. Halogenated POPs, including poly-
chlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), dioxin-
like polychlorinated biphenyls (DLPCBs), polychlorinated diphenyl
ethers (PCDEs), polybrominated dibenzo-p-dioxins and dibenzofurans

http://dx.doi.org/10.1016/j.scitotenv.2014.03.017
0048-9697/© 2014 Elsevier B.V. All rights reserved.
 Author's personal copy
52 H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59
(PBDD/Fs), polybrominated biphenyls (PBBs), and polybrominated
diphenyl ethers (PBDEs), are ubiquitous in the environment. PCDD/Fs
and PBDD/Fs are incomplete-combustion byproducts or chemical
impurities that are released into the environment (Chang et al.,
2014; Lee et al., 2004; Wang et al., 2010a). PCBs are manufactured
for industrial purposes and used in capacitors and dielectric fluids in
transformers. PBBs and PBDEs are brominated flame retardants
(BFRs) used as additives in electronic appliances, paints, textiles, and
furnishings (Schenker et al., 2008). A number of studies have shown
the importance of the combustion source when considering the
release of PBDEs into the atmosphere (Wang et al., 2010b, 2011,
2010c). PCDEs spread into the environment through the use of
chlorophenols and as emissions from combustion sources (Wu et al.,
2014). Except for PCDEs, the previously mentioned halogenated
chemical compounds are all listed as POPs under the Stockholm
Convention (Stockholm Convention, 2013).
These organochlorines and organobromines are linked to many
adverse health effects (Chao et al., in press; Van den Berg et al., 2006),
related to reproductive (Chao et al., 2010, 2007b; Hsu et al., in press),
developmental (Chao et al., 2007a; Nishijo et al., 2012), neurological
(Chao et al., 2011; Shy et al., 2011; Tai et al., 2013), and immunological
toxicities (Lin et al., 2011; Shy et al., 2012), the disruptions of endocrine
secretions (Shy et al., 2012; Wang et al., 2006), and the development of
cancers (Manuwald et al., 2012; Van den Berg et al., 2006). Their
negative impacts are possibly the result of their persistence in the envi-
ronment, resistance to physical and chemical degradations, and lipophi-
licity, which means that they accumulate in the fatty tissues of humans
and other animals.
The atmosphere is the major transportation pathway for POPs,
and long-range atmospheric transport (LRAT) is a rapid method of
transporting such chemicals to other locations or remote regions, in-
cluding oceans, the Arctic, and Antarctica (Booth et al., 2013; Möller
et al., 2011a, 2011b; Montone et al., 2005). Oceans are a naturally
cumulative reservoir for POPs; therefore, they are associated with the
exposure of aquatic organisms to these substances. Oceans act as sinks
for the accumulation of airborne POPs through dry and wet deposition
and air and water gas exchange, although studies have also suggested
that oceans may contribute to the presence of POPs in the oceanic atmo-
sphere via the volatilization of POPs in seawater (Lohmann et al., 2012;
Zhang and Lohmann, 2010).
Marine environmental scientists have examined the presence of
organochlorines, such as organochlorine pesticides and PCBs, in the
oceanic atmosphere (Gioia et al., 2012; Montone et al., 2005; Wurl
et al., 2006b; Zhang and Lohmann, 2010). An investigation of PCBs
and hexachlorobenzene (HCB) in the surface ocean-lower atmosphere
of the open Pacific Ocean revealed that the levels of these substances
in the Northern Hemisphere were significantly higher than in the
Southern Hemisphere, although no notable differences were found in
the seawater between these two areas (Zhang and Lohmann, 2010).
Recently, several studies were conducted on the levels of BFRs in the
oceanic atmosphere, especially PBDEs, to determine the related spatial
and latitudinal distributions and time trends for different oceans (Li
et al., 2011; Möller et al., 2011a; Xie et al., 2011). Möller et al. (2012a,
2012b) indicated that elevated levels of atmospheric PBDEs were gener-
ally observed in the marginal seas, such as the East China Sea or North
Sea, and among the global oceans, such as the Pacific, Atlantic, Indian,
Arctic, and Antarctic Oceans. Although a considerable number of oceanic
studies of airborne PBDE and PCB contamination have been conducted,
very few works have focused on investigations of PCDEs and dioxin-like
POPs, such as PCDD/Fs, PBDD/Fs and DLPCBs, in the oceanic atmosphere
(Lohmann et al., 2001).
Taiwan and the Philippines are located in the marginal sea of the
West Pacific Ocean. Background levels of POPs in these countries may
be influenced by LRAT during specific events (e.g., the burning of bio-
mass in Southeast Asia) (Chang et al., 2012) or the monsoon season
(e.g., the winter or northeast monsoon from Siberia, Mongolia, and
northern China) (Huang and Liang, 2011). During biomass burning in
Southeast Asia, atmospheric PCDD/F and PBDE levels were shown to
be significantly increased at a high-altitude background station in cen-
tral Taiwan, which was most likely a result of the LRAT of PCDD/Fs
and PBDEs from various Southeast Asian countries (Chang et al.,
2012). Li et al. (2011) reported that Σ21PBDE (the sum of BDE17, 28,
32, 35, 37, 47, 49, 51, 66, 71, 75, 77, 99, 100, 126, 128, 138, 153, 154,
166, and 183) in the oceanic atmosphere of the East and South China
Seas was 10.8 pg/m3, which is higher than the figures given in other
published marine atmospheric studies of the open oceans (Möller
et al., 2012b). To the best of our knowledge, no reports to date have in-
vestigated the oceanic atmospheric levels of halogenated POPs in the
West Pacific Ocean between Taiwan and the northern Philippines.
Therefore, it is still unknown whether the marine atmosphere over
the Pacific Ocean near these areas is influenced by the LRAT of POPs
from continental East Asia or Taiwan Island.
Our previous studies have established the levels of PCDD/Fs, PBDD/
Fs, DLPCBs, PBDEs, and PBBs in different atmospheric environments in
Taiwan (Chang et al., 2012; Lee et al., 2004; Shih et al., 2006; Wang
et al., 2007, 2010d, 2011); however, there is still a lack of data on the
levels of POPs in the marine atmosphere surrounding this island. This
study was the first to investigate atmospheric levels of PCDD/Fs,
PBDD/Fs, DLPCBs, PBBs, PCDEs and PBDEs over the Pacific Ocean near
southern Taiwan and the northern Philippines. Although the halogenat-
ed POP concentrations in the oceanic atmosphere are considered to be
at global background levels, as a result of the extremely low levels in
the atmosphere over the ocean compared to such levels over the land,
only PBDEs and indicator PCBs in the oceanic atmosphere have received
much research attention. This study presents details of the background
levels of halogenated POPs in the oceanic atmosphere over the West
Pacific Ocean to compensate for part of the current lack of data on the
oceanic atmosphere for the area from Aomori to Okinawa, Japan, to
Taiwan and the northern Philippines.
2. Materials and methods
2.1. Air sample collection
The ambient air of the atmospheric boundary layer over the ocean
was sampled between November 1 and November 6, 2012 by two
high-volume air samplers installed on the compass deck of the Research
Vessel Ocean Researcher V (R/V OR5), which is a 2700-tonne research
vessel from the Taiwan Ocean Research Institute, National Applied
Research Laboratories (TORL/NARL). The R/V OR5 sailed to the target
ocean from Kaohsiung (Kaohsiung Harbor, 22.60° N, 120.29° E) and
returned to Tainan (Anping Harbor, 22.97° N, 120.17° E). The atmo-
spheric air samples were collected along three routes, A (22.49° N,
120.13° E), B (20.05° N, 123.57° E), and C (19.26° N, 123.09° E), which
were over the Pacific Ocean near southern Taiwan and the northern
Philippines between 22.49° N, 120.13° E and 17.94° N, 124.63° E
(Fig. 1). Concurrently, the ambient air in a rural area (D) was sampled
by two high-volume air samplers deployed on the top floor (4 F) of
the Engineering College Building of National Pingtung University
of Science and Technology (NPUST) in southern Taiwan (22.65° N,
120.61° E). The rural area was far from the seacoast and industrial and
urban areas and has historically provided background levels of POPs in
southern Taiwan.
Each air sample was collected for approximately 40 h (1–2 days,
~600 m3) using a PS-1 sampler (Graseby Andersen, GA, USA) following
US EPA Reference Method TO9A. A quartz fiber filter was followed by a
glass cartridge containing polyurethane foam (PUF) to capture the
particle and gas phases. After the collection, the quartz fiber filter and
PUF of each air sample were combined and analyzed for PCDD/Fs,
DLPCBs, PCDEs, PBDD/Fs, PBBs, and PBDEs.
One of PS-1 samplers did not work on the NPUST campus after
November 2. Consequently, only eight air samples were collected in
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H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59 53

Fig. 1. The R/V OR5 cruising route in the present study was conducted between 1 and 6 November 2012. The OR5 sailed from Kaohsiung Harbor in Kaohsiung and returned to Anping
Harbor in Tainan. The oceanic atmosphere samples were collected along A–B between 1 and 2 November, B–C between 3 and 4 November, and C–A between 5 and 6 November. The
background levels of halogenated POPs in the ambient air over the land were collected on the campus of NPUST from 1 to 6 November (D).

the present study, including six oceanic atmosphere samples from the
Pacific Ocean and two ambient air samples over land from the NPUST
campus.
The meteorological conditions in the sampling periods were strong-
ly influenced by the winter or northeast monsoon, which features
cool and dry winds that originate in a vast anticyclone from Siberia,
Mongolia, and northern China during each winter in Taiwan and the
northern Philippines.
2.2. Extraction, cleanup and chemical analysis
The analytical method for atmospheric halogenated POPs was de-
scribed in our previous reports and used with minor modifications
(Chang et al., 2014; Wu et al., 2014). Briefly, an identified amount of
surrogate standards pre-labeled with isotopes (see Table S2 of Supple-
mentary data) were spiked to verify the collection efficiency of the sam-
pling process prior to sampling. After the collection of air samples,
internal standards were spiked into the samples to be well mixed
with toluene before Soxhlet extraction and were used to monitor the
extraction and cleanup procedures. The sample mixture was extracted
in a Soxhlet extractor with toluene for 24 h. The extracts were sequen-
tially concentrated, treated with concentrated sulfuric acid, and then
underwent a series of sample cleanup and fractionation procedures,
including the use of a multi-layered silica column, alumina column
and activated carbon column. The compounds of biphenyls, such as
non-planar PCBs and PBBs, were eluted with 15 mL hexane during the
alumina column cleanup. The activated carbon column was used for
the further cleanup procedure. After the elution of 25 mL DCM/hexane
(1/24, v/v), the activated carbon column was sequentially eluted with
5 mL toluene/methanol/ethyl acetate/hexane (1/1/2/16, v/v) for
PCDEs, PBDEs, planar PCBs and PBBs, which was followed by 40 mL
of toluene for PCDD/Fs and PBDD/Fs. The planar and non-planar
PCBs/PBBs eluates were mixed together to represent the PCB and PBB
samples. The eluate was concentrated to approximately 1 mL and
transferred to a vial. The concentrate was further concentrated to near
dryness using a stream of nitrogen. Immediately prior to injection,
10 μL of the standard solution for recovery checking was added to the
sample extract to minimize the possibility of loss.
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2.3. Instrumental analysis Table 1

Atmospheric POP levels over the rural area and Pacific Ocean near Taiwan and the
northern Philippines.
Sixty-six halogenated POPs, including the seventeen 2,3,7,8-
substituted PCDD/F, twelve 2,3,7,8-substituted PBDD/F, twelve DLPCB, Compounds Ocean (n = 6) Land (n = 2) p values
five PBB, fourteen PBDE, and six PCDE congeners, were analyzed by a Mean ± SD Mean
high-resolution gas chromatograph/high-resolution mass spectrometer
Dioxin-like POPsa 0.00612 ± 0.00591 0.0138 0.137
(HRGC/HRMS). The detailed instrumental analysis parameters for
the PCDD/Fs, PCBs, PCDEs, PBDD/Fs, PBBs and PBDEs were given in our Organochlorinesa 0.107
PCDD/Fs 0.00438 ± 0.00453 0.0113 0.11
previous studies (Chang et al., 2014; Wu et al., 2014). The HRGC
PCDDs 0.00322 ± 0.00335 0.00857 0.144
(Hewlett–Packard 6970 Series gas, CA) was equipped with a silica PCDFs 0.00116 ± 0.00117 0.00276 0.117
capillary column (J&W Scientific, CA) and splitless injector, whereas Dioxin-like PCBs 0.000439 ± 0.000230 0.00122 0.028⁎
the HRMS (Micromass Autospec Ultima, Manchester, UK) was equipped Non-ortho PCBs 0.000430 ± 0.000225 0.00118 0.028⁎
with a positive electron impact (EI+) source. Selected ion monitoring Mono-ortho PCBs 0.00000897 ± 0.00000526 0.0000303 0.020⁎
PCDEsb 0.00875 ± 0.0077 0.0144 0.333
(SIM) was used with a resolving power of 10,000. The electron energy CDE28 0.00860 ± 0.00762 0.0138 0.359
and source temperature were specified at 35 eV and 250 °C, respectively.
The quality assurance and quality control (QA/QC) of the samplings Organobrominesa
PBDD/Fs 0.00130 ± 0.00113 0.00129 0.838
and analyses, including recoveries of precision and recovery (PAR), PBDDsc bLOD bLOD –
surrogate, internal and alternate standards, spiked concentrations of PBDFsd 0.777 ± 1.04 0.198 0.438
surrogate and internal standards, laboratory and field blanks, and limits PBBse 0.0265 ± 0.0108 0.144 0.003⁎⁎
of detection (LOD) values can be found in the Supplementary data. PBB15 0.0265 ± 0.0108 0.136 0.003⁎⁎
PBDEsf 31.1 ± 16.5 15.9 0.253
diBDEs to heptaBDEs 0.903 ± 0.0381 4.70 b0.001⁎⁎⁎
2.4. Statistical analysis BDE209 27.0 ± 15.5 9.50 0.19
a
Unit: dioxins-like POPs: pg WHO2005-TEQ/m3; other POPs: pg/m3; Dioxin-like POPs
The toxic equivalency (TEQ) values of PCDD/Fs and DLPCBs were including PCDD/Fs, PBDD/Fs, and dioxin-like PCBs.
calculated using the World Health Organization 2005 toxic equivalent fac- b
PCDEs are the sum of CDE28, 77, 99, 141, 180, and 209.
c
tors (WHO2005-TEF) as previously described (Van den Berg et al., 2006). PBDDs are the sum of 2,3,7,8-TeBDD, 1,2,3,7,8-PeBDD, 1,2,3,4,7,8-HxBDD, 1,2,3,7,8,9-
The WHO2005-TEFs of PCDD/Fs were used as tentative TEFs for PBDD/Fs HxBDD, 1,2,3,4,6,7,8-HpBDD, and OBDD.
d
PBDFs are the sum of 2,3,7,8-TeBDF, 1,2,3,7,8-PeBDF, 2,3,4,7,8-PeBDF, 1,2,3,4,7,8-
to evaluate their toxicity. The differences in atmospheric POP levels
HxBDF, 1,2,3,4,6,7,8-HpBDF, and OBDF.
between the ocean and land were examined by one-sample T tests. The e
PBBs are the sum of PBB15, 52, 153, 180, and 194.
ranges of PBDEs and PCBs in the global oceanic atmosphere were obtain- f
PBDEs are the sum of BDE28, 47, 99, 100, 153, 154, 183, 196, 197, 203, 206, 207, 208,
ed from 17 published articles and the present study. The significance level and 209.
⁎ p b 0.05.
in the present study was set at 0.05 (α = 0.05). Analyses were carried out
⁎⁎ p b 0.01.
using the Statistical Package for Social Science (SPSS), version 12.0. ⁎⁎⁎ p b 0.001.

3. Results
3.1. Concentrations of dioxin-like POPs
The atmospheric dioxin-like POP levels (PCDD/Fs, PBDD/Fs and
DLPCBs) over the rural area and Pacific Ocean near Taiwan and the
northern Philippines are shown in Table 1. The detailed concentrations
of the individual dioxin-like POP congeners are shown in Tables S6-S9.
The mean levels of total dioxin-like POPs were 0.00612 (standard devi-
ation (SD) = 0.00591) and 0.0138 pg WHO2005-TEQ/m3 in the atmo-
sphere over the ocean and land, respectively. The mean PCDD/F level
in the oceanic atmosphere (0.00438 pg WHO2005-TEQ/m3) was lower
than in the ambient air over the land (0.0113 pg WHO2005-TEQ/m3);
however, the difference was not statistically significant (p = 0.110).
The mean atmospheric PBDD/F levels for the ocean and land were
comparable (0.0013 vs. 0.00129 pg WHO2005-TEQ/m3, respectively,
p = 0.0838). The levels of DLPCBs, non-ortho PCBs and mono-ortho
PCBs (0.000439, 0.000430 and 0.00000897 pg WHO2005-TEQ/m3, re-
spectively) in the atmosphere over the ocean were significantly lower
than those over the land (DLPCBs 0.00122, p = 0.028; non-ortho PCBs
0.00118, p = 0.028, and mono-ortho PCBs 0.0000303 pg WHO2005-
TEQ/m3, p = 0.020).
PCDD/F contributed 71.6% and 81.9% of the total WHO2005-TEQ levels
in the atmosphere for the ocean and land, respectively, whereas the con-
tribution of DLPCBs was minor, particularly for mono-ortho PCBs. Similar
distribution patterns for the atmospheric dioxin-like POP concentrations
were found for both the ocean and land (Fig. 2). Compared to the
PCDD/Fs and DLPCBs, the mean PBDD/F concentration in the oceanic at-
mosphere (0.777 pg/m3) was higher than in the ambient air of the rural
area (0.198 pg/m3, p = 0.438). No significant differences in atmospher-
ic concentrations of 2,3,7,8-substituted PCDD/Fs and PBDD/Fs were
found between the ocean and rural area in southern Taiwan.
3.2. Concentrations of other halogenated POPs
The mean atmospheric PBB, PBDE and PCDE levels over the rural
area and Pacific Ocean near Taiwan and the northern Philippines are
also shown in Table 1, with the detailed concentrations of their individ-
ual congeners shown in Table S10. Elevated mean levels of PCDEs
(0.0144 pg/m3) and PBBs (0.144 pg/m3) were found in the ambient
air of the rural area compared with those found in the oceanic atmo-
sphere (PCDEs 0.00875 pg/m3; PBBs 0.0265 pg/m3); however, a signifi-
cant difference was only found for PBBs.
A higher mean level of PBDEs (31.1 pg/m3) was found for the oceanic
atmosphere compared to that in the ambient air collected from the rural
area (15.9 pg/m3), although the difference was not significant. The
mean Σdi-hepta PBDEs in the oceanic atmosphere (0.903 pg/m3) were
significantly lower than that in the ambient air from the rural area
(4.7 pg/m3, p b 0.001). There was no significant difference in the
atmospheric BDE209 levels between the ocean and land (27.0 pg/m3
vs. 9.5 pg/m3, respectively, p = 0.19). The predominant congeners of
CDE28, PBB15, and BDE209 accounted for 98.3%, 100%, and 86.8%,
respectively, of the oceanic atmosphere, and 95.8%, 94.4%, and 59.7%,
respectively, of the ambient air on the land based on the total PCDEs,
PBBs, and PBDEs.
3.3. Current levels of halogenated POPs in the oceanic atmosphere of the
global oceans
The results of various ship-based studies are listed in Tables 2 and 3.
The current levels of PBDEs, PBDD/Fs, and PBBs, which are presented in
Table 2, were recorded in the atmosphere over the open waters of the
Pacific, Arctic, Indian, Atlantic, and Southern Oceans, and in that over
marginal seas, including the Far East Asia, East and South China Seas,
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H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59
Fig. 2. Distributions of halogenated POPs in the oceanic atmosphere and ambient air over
the land.
the East Indian Archipelago, the Bay of Bengal, and the Andaman and
North Seas (Li et al., 2011; Möller et al., 2011a, 2011b, 2012a; Wang
et al., 2005; Wurl et al., 2006a; Xie et al., 2011). The dominant congeners
in the oceanic atmosphere among the brominated POPs listed in Table 2
are BDE47 or BDE209. However, few published articles have reported
the atmospheric levels of PBBs and PBDD/Fs over the ocean.
Table 3 lists the atmospheric levels of PCDD/Fs, PCBs (including
DLPCBs), and PCDEs over the oceans. Most investigations have focused
on the atmosphere over the Atlantic Ocean (Gioia et al., 2008, 2012;
Jaward et al., 2004; Lohmann et al., 2001, 2012; Montone et al., 2005;
Zhang and Lohmann, 2010), and few works have considered the atmo-
spheric PCDD/Fs and PCBs over the Indian, Southern, and Arctic Oceans
or the marginal seas in East and South Asia (Gioia et al., 2012; Lohmann
et al., 2001; Montone et al., 2005; Wurl et al., 2006b). In addition, little
research has been conducted on the levels of PCDD/Fs, DLPCBs, and
PCDEs in the global oceanic atmosphere.
4. Discussions
4.1. Halogenated POPs in the atmosphere over the ocean and land
The halogenated POP levels in the rural area of this study were close
to the background levels. More specifically, our PCDD/F concentration
(0.0113 pg WHO2005-TEQ/m3) was comparable to that (Lee et al.,
55
2004) in the background of Taiwan (0.0063 pg I-TEQ/m3) and notably
lower than those in the atmosphere of the industrial, urban, and rural
areas in southern Taiwan, which were 0.0492, 0.0568, and 0.0318 pg
I-TEQ/Nm3, respectively (Mi et al., 2012). The atmospheric DLPCB con-
centrations in different areas of southern Taiwan (industrial 0.00329,
urban 0.00567, and rural 0.00230 pg WHO2005-TEQ/Nm3) reported by
Mi et al. (2012) were significantly higher than what was found in the
present study (0.000439 pg WHO2005-TEQ/m3). The PBDD/F concentra-
tions found in different atmospheric environments in Taiwan (Wang
et al., 2007) (rural 0.0027, urban 0.0064, industrial 0.012, science park
0.031 pg TEQ/Nm3) were at least two-fold higher than what was
found in the current report (0.00129 pg WHO2005-TEQ/m3). In addition,
the averaged atmospheric PBDE concentration in the rural area
(15.9 pg/m3) found in this study was lower than that in earlier articles
that also examined various environments in Taiwan (heavy steel
complex area 165, metals complex area 93.3, urban 35.3 pg/m3 in
Taipei City in 2009 from Wang et al. (2011); industrial: 58.5, urban:
88, rural: 55.4 pg/Nm3 in Tainan City in 2010–2011 from Lin et al.
(2012)). Few studies have reported the atmospheric levels of PBBs,
although Wang et al. (2010d) reported that the mean PBB level was
0.341 pg/Nm3 (ranged from 0.149 to 0.556 pg/Nm3) in a rural area
near a municipal solid waste incinerator (MSWI) in Kaohsiung City in
2009. To the best of our knowledge, no studies have reported PCDE
data for Taiwanese atmospheric environments.
Except for PBDD/Fs and PBDEs from octa to deca, the levels of atmo-
spheric halogenated POPs over the target oceans were all lower than the
background levels over the land in this study. For the PBDD/Fs, only
three congeners of 1,2,3,4,7,8-HxBDF, 1,2,3,4,6,7,8-HpBDF, and OBDF
were found in the atmosphere over both the ocean and land. Although
the mean PBDD/F mass concentration in the oceanic atmosphere was
higher than in the ambient air of the rural area, the TEQ levels of
atmospheric PBDD/Fs over the ocean and land were comparable,
which was mainly a result of the high atmospheric levels of 1,2,
3,4,6,7,8-HpBDF and OBDF over the target ocean, which had low TEF
values (1,2,3,4,6,7,8-HpBDF of 0.001 and OBDF of 0.0003).
4.2. Characteristic patterns of halogenated POPs over the ocean and land
POPs in the oceanic atmosphere or marine environment have histor-
ically been recognized as the global background levels. Although it is
difficult to identify the persistence and atmospheric transport behaviors
in the environment for halogenated POPs, scientific models have shown
that these halogenated compounds can move to the oceanic atmo-
sphere via LRAT (Booth et al., 2013; Ono et al., 2012). Booth et al.
(2013) estimated that the annual PCDD/F deposition to surface seawa-
ter was 115 kg-TEQ in the East China Sea near Japan and South Korea,
which is the highest value that has been reported for all of the oceans
in the world (consisting of 40% of the total global PCDD/F emissions).
The characteristic distribution patterns of atmospheric halogenated
POPs were similar for the rural area over the land and target ocean
except for the distribution pattern of PBDEs (Fig. 2). BDE209 accounted
for a greater fraction (86.8%) of the total PBDEs in the oceanic atmo-
sphere than in the ambient air over the land (59.7%). Our previous
study found that PBDEs could form through de novo synthesis and
precursor mechanisms (Artha et al., 2011). Furthermore, PBDE and
PBDD/F formation through combustion prefers the generation of highly
brominated congeners, such as BDE-209, -208, -207, -206, and -183,
1,2,3,4,6,7,8-HpBDF and OBDF (Chang et al., 2013, 2014; Wang et al.,
2010b). These highly brominated congeners dominate in the stack flue
gasses (or exhausts) of various important combustion sources, such as
incinerators, metallurgical processes, power-heating systems and
vehicles (Chang et al., 2013, 2014; Wang et al., 2010a, 2010b, 2010c).
The elevated mass concentration of PBDD/Fs (only the highly brominat-
ed PBDF congeners were detectable) and PBDEs, especially octa- to
deca-PBDEs, in the oceanic atmosphere compared to those in the ambi-
ent air of the rural area revealed that during the winter monsoon
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56 H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59

Table 2
Current data for the mean levels (gaseous and particulate phase) of brominated POPs in the oceanic atmosphere (unit: pg/m3).

Sampling location (years) BDE47 BDE99 BDE100 BDE153 BDE183 BDE209 PBDEs PBDD/Fs PBBs References

Pacific Ocean
Near Southern Taiwan (2012) 0.490 0.133 0.0526 0.0407 0.0795 27.0 31.1(0.903)a 0.0013b 0.0265 This study
Near Siberia (2003)c 6.00 2.24 0.56 0.1 0.04 3.62 12.8 –d – Wang et al. (2005)
Near Siberia (2010) 0.0533 0.182 0.0083 0.0033 0.0083 0.592 0.852 – – Möller et al. (2011a)
Near East Philippines (2010/11) 0.14 bLODe bLOD bLOD bLOD bLOD 0.14 – – Möller et al. (2012a)
Far East Asia Sea (2003)c 28.0 14.4 3.62 0.54 0.03 9.63 58.3 – – Wang et al. (2005)
Far East Asia Sea (2010) 0.278 0.338 0.02 0.25 0.243 1.58 2.85 – – Möller et al. (2011a)
East and South China Sea (2008) 4.09 1.76 0.37 0.26 0.56 – 10.8 – – Li et al. (2011)
East Indian Archipelago (2010/11) 0.233 0.163 0.005 0.045 bLOD 1.05 1.67 – – Möller et al. (2012a)
Bay of Bengal and Andaman Sea (2008) 1.44 0.47 0.24 0.05 0.23 – 3.22 – – Li et al. (2011)

Arctic Ocean
Near Alaska (2003)c 7.21 4.95 0.98 0.26 0.03 3.01 17.3 – – Wang et al. (2005)
Near Alaska (2010) 0.03 0.0529 0.0011 bLOD 0.0043 0.823 0.911 – – Möller et al. (2011a)
East Greenland Sea (2009) 0.339 0.148 0.035 0.0072 0.0044 0.0144c 0.523 – – Möller et al. (2011b)

Indian Ocean
North (2009) 3.21 0.89 0.39 0.03 bLOD – 5.12 – – Li et al. (2011)
Near Indonesia (2004/05) 3.69 1.17 0.1 0.144 bLOD bLOD 5.22 – – Wurl et al. (2006a)
East and South (2010/11) 0.121 0.131 0.0071 0.0129 0.045 1.35 1.90 – – Möller et al. (2012a)

Atlantic Ocean
Near Africa (2008) 3.21 0.89 0.39 0.03 bLOD – 5.12 – – Li et al. (2011)
Near Europe (2008) 1.48 0.405 0.05 0.55 0.11 – 2.22 – – Xie et al. (2011)
Near Northwestern and Western Africa (2008) 1.16 0.335 0.08 0.0175 0.015 – 1.70 – – Xie et al. (2011)
Near Southwestern Africa (2008) 0.327 0.31 0.07 0.02 0.03 – 0.83 – – Xie et al. (2011)
North Sea (2010) 0.306 0.178 0.023 0.002 0.550 1.62 2.10 – – Möller et al. (2012b)

Southern Ocean
Near South Africa (2008) 0.58 0.11 0.03 0.01 0.01 – 0.78 – – Xie et al. (2011)
Near Australia (2010/11) 0.08c 0.06c bLOD bLOD bLOD bLOD 0.14 – – Möller et al. (2012a)

PBDEs in our study: BDE28, 47, 99, 100, 153, 154, 183, 196, 197, 203, 206, 207, 208, and 209; in Wang et al. (2005): BDE28, 47, 66, 85, 99, 100, 138, 153, 154, 183, and 209; in Möller et al.
(2011a): BDE47, 99, 100, 153, 154, 183, and 209; in Li et al. (2011): BDE17, 28, 32, 35, 37, 47, 49, 51, 66, 71, 75, 77, 99, 100, 126, 128, 138, 153, 154, 166, and 183; Xie et al. (2011): BDE28, 47,
66, 85, 99, 100, 153, 154, and 183; in Möller et al. (2011b): BDE28, 47, 66, 85, 99, 100, 153, 154, and 183; in Möller et al. (2012a): BDE28, 47, 66, 85, 99, 100, 153, 154, 183, and 209; in Möller
et al. (2012a): BDE28, 47, 66, 85, 99, 100, 153, 154, 183, and 209; Measurements lower than LOD recognized as zero.
a
PBDEs (Σdi-hepta PBDEs); Σdi-hepta PBDEs was the sum of BDE28, 47, 99, 100, 153, 154, and 183.
b
pg WHO2005 TEQ/m3.
c
Particulate phase.
d
No data.
e
Low than detection of limits.

season, the POPs in the oceanic atmosphere of the Pacific Ocean near
Taiwan and the northern Philippines may be influenced by the POPs
emitted from combustion sources in Taiwan or China via atmospheric
transport. This can be verified by the significantly lower concentration
of Σdi-hepta PBDEs in the oceanic atmosphere (0.903 pg/m3) than in the
ambient air from the rural area (4.7 pg/m3), which was the result of
the lighter brominated PBDEs produced by the evaporative release of
the commercial penta- and octa-PBDE mixtures used in many common
products (Wang et al., 2011).
The target ocean in the current study was listed in Booth et al. (2013)
as having the second highest level of severe marine PCDD/F deposition.
Furthermore, extremely high concentrations of PCDD/Fs, PBDD/Fs, and
PBDEs were found in air samples near e-waste recycling areas (Taizhou
in Zhejiang and Guiyu in Guangdong) in China (Li et al., 2007; Zhang
et al., 2012) close to East and South China Seas and our sampling area
by the Taiwan Strait. Therefore, longitudinal and long-term monitoring
of halogenated POPs in this ocean is required.
4.3. The current investigation of halogenated POPs in the
oceanic atmosphere
This study is the first report to show the levels of PCDD/Fs, DLPCBs,
PBDD/Fs, PBBs, and PCDEs in the oceanic atmosphere over the Pacific
Ocean (Tables 2 and 3). Few previous studies have reported data on
dioxin-like POPs, PCDEs, and PBBs in the oceanic atmosphere, with the
literature being particularly sparse for PBDD/Fs, PCDEs, and PBBs.
In general, atmospheric POP concentrations over the open ocean are
lower than those over marginal seas near continents or islands; howev-
er, factors such as the geographical and meteorological conditions can
affect the characteristic distribution of POP concentrations and should
be carefully considered. The spatial distributions of POPs, especially
PBDEs, are most likely related to the proximity of the sampling sites to
the source regions, whether of land or air mass origin (Li et al., 2011).
Furthermore, a German research team indicated that the concentrations
of halogenated POPs, such as PBDEs, in the oceanic atmosphere are in-
fluenced during sampling by various environmental or meteorological
parameters, including wind speed and direction and temperature
(Möller et al., 2012a).
Therefore, comparing the PBDE levels in the oceanic atmosphere
found in the current work with those in the literature does not appear
to be useful, because of the large number of confounding factors, such
as temperature, pressure, humidity or moisture, geography, longitude,
latitude, wind speed and direction, monsoon, ocean current, and instru-
ments for sampling and analysis. However, additional data are required
to determine if halogenated POPs emitted from the land have serious
impacts on the contamination of marine environments, including the
atmosphere, seawater, and sediments in remote oceans. The collection
of the data from papers published within the last two decades that
show the ranges of various halogenated POPs may offer additional
detailed information regarding marine contamination, and such a
collection is one of the aims of the current work.
To the best of our knowledge, all of the published data for atmo-
spheric levels of PCDD/Fs, DLPCBs, PCBs, and PBDEs over the global
oceans and marginal seas are listed in Tables 2 and 3. The spatial and
latitudinal distributions of PCDD/Fs, PCBs, non-ortho PCBs, and PBDEs
in the oceanic atmosphere presented in several studies (Gioia et al.,
2012; Lohmann et al., 2001, 2012; Möller et al., 2011a, 2012a) were col-
lected and analyzed in this work to examine the levels of halogenated
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H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59 57

Table 3
Current data for the mean levels (gaseous and particulate phase) of chlorinated POPs in the oceanic atmosphere (unit: pg WHO-TEQ/m3 or pg/m3).a

Sampling location (years) PCDD/Fs Non-ortho PCBs Mono-ortho PCBs PCBs PCDEs References

Pacific Ocean
Near southern Taiwan (2012) 0.00438b 0.000430b 0.00000897b 0.349 0.00875 This study
East and South China Sea (2007/08) –c – – 77 – Gioia et al. (2012)
Andaman Sea and Bay of Bengal (2004/05) – – – 53.2 – Wurl et al. (2006b)
Andaman Sea and Bay of Bengal (2007/08) – – – 30 – Gioia et al. (2012)

Indian Ocean
North (2004/05) – – – 39.4 – Wurl et al. (2006b)
North (2007/08) – – – 42 – Gioia et al. (2012)

Atlantic Ocean
Near Southern South America (1995) – – – 203 – Montone et al. (2005)
Near Western Europe and North Africa 30–60° N (1998) 0.0056d 0.00263d – 2.32 – Lohmann et al. (2001)
Near North Africa 0–30° N (1998) 0.0058d 0.00601d – 2.16 – Lohmann et al. (2001)
Near Brazil 0–30° S (1998) 0.0035d 0.00401d – 1.14 – Lohmann et al. (2001)
Near Argentina 30–60 oS (1998) 0.0019d 0.00077d – 0.707 – Lohmann et al. (2001)
Northern Hemisphere (2001) – – – 31 – Jaward et al. (2004)
Southern Hemisphere (2001) – – – 22 – Jaward et al. (2004)
Northern Hemisphere (2005) – – – 53 – Gioia et al. (2008)
Southern Hemisphere (2005) – – – 16 – Gioia et al. (2008)
Northern Hemisphere (2006/07) – – – 94 – Zhang and Lohmann (2010)
Southern Hemisphere (2006/07) – – – 25 – Zhang and Lohmann (2010)
Northern Hemisphere (2007/08) – – – 23 – Gioia et al. (2012)
Southern Hemisphere (2007/08) – – – 20 – Gioia et al. (2012)
Northern Hemisphere (2009) – – – 8.07 – Lohmann et al. (2012)
Southern Hemisphere (2009) – – – 8.56 – Lohmann et al. (2012)

Southern Ocean
Near South America (1995) – – – 62.4 – Montone et al. (2005)
Near South America (1998) 0.00095d 0.00077d – 0.786 – Lohmann et al. (2001)

Arctic Ocean
Near Scandinavia (1998) 0.00099d 0.000658d – 0.786 – Lohmann et al. (2001)

PCBs in this study: PCB 77, 81, 105, 114, 118, 123, 126, 156, 157, 167, 169, and 189; in Gioia et al. (2012): PCB 28, 31, 52, 90, 101, 118, 132, 138, 153, and 180; in Montone et al. (2005): 18,
28, 44, 52, 101, 118, 128, 138, 153, 180, and 187; in Lohmann et al. (2001): PCB77 and PCB126; in Jaward et al. (2004): PCB 28, 52, 101, 118, 138, 153, and 180; in Gioia et al. (2008): PCB 28,
31, 52, 90, 101, 118, 132, 138, 153, and 180; in Zhang and Lohmann (2010): PCB3, 8, 18, 28, 44, 52, 66, 101, 118, 138, 153, 180, 189, 206, and 209; in Lohmann et al. (2012): PCB 28, 52, 101,
153, and 180; Measurements lower than LOD recognized as zero.
a
The unit of PCDD/Fs, non-ortho PCBs, and mono-ortho PCBs is pg WHO-TEQ/m3. The units of PCBs and PCDEs are pg/m3.
b
Unit: pg WHO2005-TEQ/m3.
c
No data.
d
pg WHO1998-TEQ/m3; non-ortho PCBs only included in PCB77 and PCB126.

POPs in the global oceanic atmosphere. Data for PBDEs and PCBs were
included; however, DLPCBs were excluded.
Based on the available PBDE data, which is listed in Table 2, the most
frequently detected congeners are BDE47, 99, 100, and 209, whereas
the most infrequently detected congeners are BDE28, 153, 154, and
183. The mean Σdi-hepta PBDEs concentrations ranged from 0.09 to
48.7 pg/m3 in the atmosphere over the global oceans (our mean value
was 0.903 pg/m3). The highest and lowest values of Σdi-hepta PBDEs in
the oceanic atmosphere were found for the Far East Asia Sea (collected
in 2003) (Wang et al., 2005) and Arctic Ocean near Alaska (collected in
2010) (Möller et al., 2011a), respectively. Data for BDE209 were avail-
able in six papers, including the present study, and are shown in
Table 2 (Möller et al., 2011a, 2011b, 2012a, 2012b; Wang et al., 2005).
Atmospheric levels of PBDEs, including BDE209, over the global oceans
ranged between 0.14 and 58.3 pg/m3. Our values for the PBDEs, includ-
ing BDE209, were slightly higher than the other figures listed in Table 2
except for the PBDEs in the atmosphere over the Far East Asia Sea collect-
ed in 2003 (Möller et al., 2011a). From the current available data for the
global oceans, the mean atmospheric levels of Σdi-hepta PBDEs ranged be-
tween 0.14 and 48.7 pg/m3 over the Pacific Ocean, 0.09 and 14.3 pg/m3
over the Arctic Ocean, 0.55 and 5.22 pg/m3 over the Indian Ocean, 0.48
and 5.12 pg/m3 over the Atlantic Ocean, and 0.14 and 0.78 pg/m3 over
the Southern Ocean. Therefore, our findings were consistent with the
conclusions in Möller et al. (2012a), which stated that the highest
PBDE concentrations in the global oceanic atmosphere were over the
marginal seas, such as the East China Sea for the Pacific Ocean or the
North Sea for the Atlantic Ocean, and the Southern Ocean, with lower
magnitudes found over the Arctic Ocean (Möller et al., 2012a).
With regard to the PCB congeners in the global oceanic atmosphere,
the dominant PCBs were PCB28, 52, 101, 118, 138, 153, and 180, as
shown in Table 3. It should be noted that indicator PCBs were not inves-
tigated in the present study. Six published articles were selected for data
analysis because of their investigations of atmospheric indicator PCBs
over oceans (Gioia et al., 2008, 2012; Jaward et al., 2004; Lohmann
et al., 2012; Montone et al., 2005; Wurl et al., 2006a; Zhang and
Lohmann, 2010). The reports of Montone et al. (2005) and Lohmann
et al. (2001) were excluded because of the sampling time period
(1995 in Montone et al. (2005) and 1998 in Lohmann et al. (2001)),
analytical instrument for PCBs (GC-ECD was used in Montone et al.
(2005)), and type of PCB congener (only PCB-77 and 126 were detected
in Lohmann et al. (2001)). The mean PCB concentrations ranged from
8.07 to 94.0 pg/m3 and were based on all the statistics for PCBs in the
global oceanic atmosphere. The average atmospheric PCB levels ranged
from 30.0 to 77.0 pg/m3 over the Pacific Ocean, 39.4 to 42.0 pg/m3 over
the Indian Ocean, and 8.07 to 94.0 pg/m3 over the Atlantic Ocean.
With regard to the atmospheric PCBs in the Northern and Southern
Hemispheres of the Atlantic Ocean, these were between 8.07 and
94.0 pg/m3 and between 8.56 and 25.0 pg/m3, respectively, and slightly
higher in the former than in the latter (Gioia et al., 2008, 2012; Jaward
et al., 2004; Zhang and Lohmann, 2010).
The atmospheric WHO-TEQ levels of PCDD/F and non-ortho PCBs
found over the ocean in the present study were comparable to those re-
ported along a North-South Atlantic transect in 1998 (Lohmann et al.,
2001). To the best of our knowledge, no further information on PCDD/
Fs and DLPCBs in the oceanic atmosphere has been published since
Lohmann et al. (2001). However, continuous monitoring of dioxin-like
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58 H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59
POPs in the seawater of East Asia is essential because of severe PCDD/F
deposition in these remote oceans.
5. Conclusions
This study is valuable because few previous studies have reported
the levels of PBDD/Fs, PCDEs, and PBBs in the global oceanic atmo-
sphere. Except for PBDEs, similar congener profiles for the atmospheric
halogenated POPs were found for the ocean and land, and the atmo-
spheric POP concentrations were higher over the land than ocean.
Atmospheric TEQ levels of dioxin-like POPs over the target ocean were
one order of magnitude lower than those over the land. The halogenat-
ed POPs originating from the land could reach our target ocean via
atmospheric transport. According to data from 17 published references
and the present study, the levels of Σdi-hepta PBDEs and PCBs in the global
oceanic atmosphere ranged between 0.09 and 48.7 pg/m3 and 8.07 and
94.0 pg/m3, respectively. The results showed that PCBs and PBDEs are
the major halogenated POPs in the global oceanic atmosphere.
Conflict of interest
The authors declare no conflict of interest with regard to this study.
Acknowledgments
The study was supported by the National Science Council of Taiwan
under Grant NSC 100-2628-E-230-001-MY3 and partially under NSC
101-2628-E-020-001. We also acknowledge the support this study
received from the crew of the R/V Ocean Researcher V (R/V OR5) and
staff of the Taiwan Ocean Research Institute, National Applied Research
Laboratories (TORL/NARL). We thank Mr. Wen-Kai Wu, Chien-Yu Chen,
and Bao-An Chiang from the National Pingtung University of Science
and Technology for assisting with sample collection and data analysis.
Appendix A. Supplementary data
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.scitotenv.2014.03.017.
References
Artha AA, Wu EM-Y, Wang L-C, Chen C-H, Chang-Chien G-P. Thermal formation of
polybrominated diphenyl ethers in raw and water-washed fly ash. Aerosol Air Qual
Res 2011;11:393–400.
Booth S, Hui J, Alojado Z, Lam V, Cheung W, Zeller D, et al. Global deposition of airborne
dioxin. Mar Pollut Bull 2013;75:182–6.
Chang S-S, Lee W-J, Wang L-C, Lin N-H, Chang-Chien G-P. Influence of the Southeast Asian
biomass burnings on the atmospheric persistent organic pollutants observed at near
sources and receptor site. Atmos Environ 2012;78:184–94.
Chang S-S, Lee W-J, Wang L-C, Chang-Chien G-P, Wu C-Y. Energy recovery and emissions
of PBDD/Fs and PBDEs from co-combustion of woodchip and wastewater sludge in an
industrial boiler. Environ Sci Technol 2013;47:12600–6.
Chang YC, Lee WJ, Wang LC, Yang HH, Cheng MT, Lu JH, et al. Effects of waste cooking oil-
based biodiesel on the toxic organic pollutant emissions from a diesel engine. Appl
Energy 2014;113:631–8.
Chao H-R, Wang S-L, Lee W-J, Wang Y-F, Päpke O. Levels of polybrominated diphenyl
ethers (PBDEs) in breast milk from central Taiwan and their relation to infant birth
outcome and maternal menstruation effects. Environ Int 2007a;33:239–45.
Chao HR, Wang SL, Lin LY, Lee WJ, Päpke O. Placental transfer of polychlorinated dibenzo-
p-dioxins, dibenzofurans, and biphenyls in Taiwanese mothers in relation to
menstrual cycle characteristics. Food Chem Toxicol 2007b;45:259–65.
Chao HR, Shy CG, Wang SL, Chih-Cheng Chen S, Koh TW, Chen FA, et al. Impact of non-
occupational exposure to polybrominated diphenyl ethers on menstruation charac-
teristics of reproductive-age females. Environ Int 2010;36:728–35.
Chao HR, Tsou TC, Huang HL, Chang-Chien GP. Levels of breast milk PBDEs from southern
Taiwan and their potential impact on neurodevelopment. Pediatr Res 2011;70:
596–600.
Chao H-R, Huang H-L, Hsu Y-C, Lin C-W, Lin D-Y, Gou Y-Y, et al. Impact of brominated
pops on the neurodevelopment and thyroid hormones of young children in an indoor
environment—a review. Aerosol Air Qual Res 2014. http://dx.doi.org/10.4209/aaqr.
2013.05.0156. [in press].
Gioia R, Nizzetto L, Lohmann R, Dachs J, Temme C, Jones KC. Polychlorinated biphenyls
(PCBs) in air and seawater of the Atlantic Ocean: sources, trends and processes.
Environ Sci Technol 2008;42:1416–22.
Gioia R, Li J, Schuster J, Zhang Y, Zhang G, Li X, et al. Factors affecting the occurrence and
transport of atmospheric organochlorines in the China sea and the northern Indian
and south east Atlantic oceans. Environ Sci Technol 2012;46:10012–21.
Hsu P-C, Guo YL, Smith DR, Lin Y-S, Tseng L-H, Lee C-W, et al. Airborne persistent organic
pollutants and male reproductive health. Aerosol Air Qual Res 2014. http://dx.doi.
org/10.4209/aaqr.2013.03.0066. [in press].
Huang CK, Liang JJ. Effects of basin topography and monsoon conditions on transport and
occurrence of atmospheric PCDD/Fs in the Taichung Basin. Environ Sci Pollut Res
2011;18:1305–15.
Jaward FM, Barber JL, Booij K, Dachs J, Lohmann R, Jones KC. Evidence for dynamic air–
water coupling and cycling of persistent organic pollutants over the open Atlantic
ocean. Environ Sci Technol 2004;38:2617–25.
Lee W-S, Chang-Chien G-P, Wang L-C, Lee W-J, Tsai P-J, Wu K-Y, et al. Source identifica-
tion of PCDD/Fs for various atmospheric environments in a highly industrialized
city. Environ Sci Technol 2004;38:4937–44.
Li H, Yu L, Sheng G, Fu J, Pa Peng. Severe PCDD/F and PBDD/F pollution in air around an
electronic waste dismantling area in China. Environ Sci Technol 2007;41:5641–6.
Li J, Li Q, Gioia R, Zhang Y, Zhang G, Li X, et al. PBDEs in the atmosphere over the Asian
marginal seas, and the Indian and Atlantic oceans. Atmos Environ 2011;45:6622–8.
Lin S-M, Chen F-A, Huang Y-F, Hsing L-L, Chen L-L, Wu L-S, et al. Negative associations
between PBDE levels and thyroid hormones in cord blood. Int J Hyg Environ Health
2011;214:115–20.
Lin L-F, Chang K-L, Liao W-T, Lai Y-C, Lee Y-Y, Wang L-C, et al. Atmospheric concentrations
and dry deposition of polybrominated diphenyl ethers in southern Taiwan. Aerosol
Air Qual Res 2012;12:1135–45.
Lohmann R, Ockenden WA, Shears J, Jones KC. Atmospheric distribution of poly-
chlorinated dibenzo-p-dioxins, dibenzofurans (PCDD/Fs), and non-ortho biphenyls
(PCBs) along a north–south Atlantic transect. Environ Sci Technol 2001;35:4046–53.
Lohmann R, Klanova J, Kukucka P, Yonis S, Bollinger K. PCBs and OCPs on a east-to-west
transect: the importance of major currents and net volatilization for PCBs in the
Atlantic Ocean. Environ Sci Technol 2012;46:10471–9.
Manuwald U, Garrido MV, Berger J, Manz A, Baur X. Mortality study of chemical workers
exposed to dioxins: follow-up 23 years after chemical plant closure. Occup Environ
Med 2012;69:636–42.
Mi H-H, Wu Z-S, Lin L-F, Lai Y-C, Lee Y-Y, Wang L-C, et al. Atmospheric dry deposition of
polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) and polychlorinated
biphenyls (PCBs) in southern Taiwan. Aerosol Air Qual Res 2012;12:1016–29.
Möller A, Xie Z, Cai M, Zhong G, Huang P, Cai M, et al. Polybrominated diphenyl ethers vs
alternate brominated flame retardants and dechloranes from East Asia to the Arctic.
Environ Sci Technol 2011a;45:6793–9.
Möller A, Xie Z, Sturm R, Ebinghaus R. Polybrominated diphenyl ethers (PBDEs) and
alternative brominated flame retardants in air and seawater of the European Arctic.
Environ Pollut 2011b;159:1577–83.
Möller A, Xie Z, Caba A, Sturm R, Ebinghaus R. Occurrence and air–seawater exchange of
brominated flame retardants and Dechlorane Plus in the North Sea. Atmos Environ
2012a;46:346–53.
Möller A, Xie Z, Cai M, Sturm R, Ebinghaus R. Brominated flame retardants and dechlorane
plus in the marine atmosphere from Southeast Asia toward Antarctica. Environ Sci
Technol 2012b;46:3141–8.
Montone RC, Taniguchi S, Boian C, Weber RR. PCBs and chlorinated pesticides (DDTs,
HCHs and HCB) in the atmosphere of the southwest Atlantic and Antarctic oceans.
Mar Pollut Bull 2005;50:778–82.
Nishijo M, Nakagawa H, Maruzeni S, Anh NTN, Van Luong H, Anh TH, et al. Impact of
perinatal dioxin exposure on infant growth: a cross-sectional and longitudinal
studies in dioxin-contaminated areas in Vietnam. PLoS One 2012;7:e40273.
Ono J, Takahashi D, Guo X, Takahashi S, Takeoka H. A numerical study on the seasonal
variability of polychlorinated biphenyls from the atmosphere in the East China Sea.
Chemosphere 2012;89:389–97.
Schenker U, Soltermann F, Scheringer M, Hungerbühler K. Modeling the environmental
fate of polybrominated diphenyl ethers (PBDEs): the importance of photolysis for
the formation of lighter PBDEs. Environ Sci Technol 2008;42:9244–9.
Shih M, Lee WS, Chang-Chien GP, Wang LC, Hung CY, Lin KC. Dry deposition of
polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in ambient air.
Chemosphere 2006;62:411–6.
Shy C-G, Huang H-L, Chang-Chien G-P, Chao H-R, Tsou T-C. Neurodevelopment of infants
with prenatal exposure to polybrominated diphenyl ethers. Bull Environ Contam
Toxicol 2011;87:643–8.
Shy CG, Huang HL, Chao HR, Chang-Chien GP. Cord blood levels of thyroid hormones and
IGF-1 weakly correlate with breast milk levels of PBDEs in Taiwan. Int J Hyg Environ
Health 2012;215:345–51.
Stockholm ConventionIn: Stockholm C (Hrsg.), editor. What are POPs?; 2013.
Tai PT, Nishijo M, Anh NTN, Maruzeni S, Nakagawa H, Van Luong H, et al. Dioxin exposure
in breast milk and infant neurodevelopment in Vietnam. Occup Environ Med 2013;
70:656–62.
Van den Berg M, Birnbaum LS, Denison M, De Vito M, Farland W, Feeley M, et al. The 2005
World Health Organization reevaluation of human and mammalian toxic equivalency
factors for dioxins and dioxin-like compounds. Toxicol Sci 2006;93:223–41.
Wang XM, Ding X, Mai Bx, Xie Zq, Xiang Ch, Sun Lg, et al. Polybrominated diphenyl ethers
in airborne particulates collected during a research expedition from the Bohai Sea to
the Arctic. Environ Sci Technol 2005;39:7803–9.
Wang SL, Chang YC, Chao HR, Li CM, Li LA, Lin LY, et al. Body burdens of polychlorinated
dibenzo-p-dioxins, dibenzofurans, and biphenyls and their relations to estrogen
metabolism in pregnant women. Environ Health Perspect 2006;114:740–5.
 Author's personal copy
H.-R. Chao et al. / Science of the Total Environment 491–492 (2014) 51–59
Wang LC, Tsai CH, Chang-Chien GP, Hung CH. Characterization of polybrominated
dibenzo-p-dioxins and dibenzofurans in different atmospheric environments.
Environ Sci Technol 2007;42:75–80.
Wang L-C, Hsi H-C, Wang Y-F, Lin S-L, Chang-Chien G-P. Distribution of polybrominated
diphenyl ethers (PBDEs) and polybrominated dibenzo-p-dioxins and dibenzofurans
(PBDD/Fs) in municipal solid waste incinerators. Environ Pollut 2010a;158:
1595–602.
Wang L-C, Lee W-J, Lee W-S, Chang-Chien G-P. Emission estimation and congener-
specific characterization of polybrominated diphenyl ethers from various stationary
and mobile sources. Environ Pollut 2010b;158:3108–15.
Wang L-C, Wang Y-F, Hsi H-C, Chang-Chien G-P. Characterizing the emissions of
polybrominated diphenyl ethers (PBDEs) and polybrominated dibenzo-p-dioxins
and dibenzofurans (PBDD/Fs) from metallurgical processes. Environ Sci Technol
2010c;44:1240–6.
Wang MS, Chen SJ, Huang KL, Lai YC, Chang-Chien GP, Tsai JH, et al. Determination of
levels of persistent organic pollutants (PCDD/Fs, PBDD/Fs, PBDEs, PCBs, and PBBs)
in atmosphere near a municipal solid waste incinerator. Chemosphere 2010d;80:
1220–6.
59
Wang L-C, Lee W-J, Lee W-S, Chang-Chien G-P. Polybrominated diphenyl ethers in various
atmospheric environments of Taiwan: their levels, source identification and influence
of combustion sources. Chemosphere 2011;84:936–42.
Wu EM-Y, Wang L-C, Lin S-L, Chang-Chien G-P. Validation and characterization of persis-
tent organic pollutant emissions from stack flue gases of an electric arc furnace by
using a long-term sampling system (AMESA®). Aerosol Air Qual Res 2014;14:185–96.
Wurl O, Potter JR, Durville C, Obbard JP. Polybrominated diphenyl ethers (PBDEs) over the
open Indian Ocean. Atmos Environ 2006a;40:5558–65.
Wurl O, Potter JR, Obbard JP, Durville C. Persistent organic pollutants in the equatorial
atmosphere over the open Indian Ocean. Environ Sci Technol 2006b;40:1454–61.
Xie Z, Möller A, Ahrens L, Sturm R, Ebinghaus R. Brominated flame retardants in seawater
and atmosphere of the Atlantic and the Southern Ocean. Environ Sci Technol 2011;
45:1820–6.
Zhang L, Lohmann R. Cycling of PCBs and HCB in the surface ocean-lower atmosphere of
the open Pacific. Environ Sci Technol 2010;44:3832–8.
Zhang T, Huang YR, Chen SJ, Liu AM, Xu PJ, Li N, et al. PCDD/Fs, PBDD/Fs, and PBDEs in the
air of an e-waste recycling area (Taizhou) in China: current levels, composition
profiles, and potential cancer risks. J Environ Monit 2012;14:3156–63.