Chemosphere 191 (2018) 990e1007

Contents lists available at ScienceDirect

Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere

Review

Pyrethroid pesticide residues in the global environment: An overview

Wangxin Tang, Di Wang, Jiaqi Wang, Zhengwen Wu, Lingyu Li, Mingli Huang, Shaohui Xu,
Dongyun Yan*
College of Environmental Sciences and Engineering, Qingdao University, Qingdao, 266071, China

h i g h l i g h t s

 Pyrethroid pesticides have been widely detected at the global scale.

 Sediment samples from developed regions revealed high levels of pyrethroids.
 Pesticide residues in residential environments and the human body should be given more attention.

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

Article history: Pyrethroids are synthetic organic insecticides with low mammalian toxicity that are widely used in both
Received 12 July 2017 rural and urban areas worldwide. After entering the natural environment, pyrethroids circulate among
Received in revised form the three phases of solid, liquid, and gas and enter organisms through food chains, resulting in sub-
17 October 2017
stantial health risks. This review summarized the available studies on pyrethroid residues since 1986 in
Accepted 20 October 2017
different media at the global scale and indicated that pyrethroids have been widely detected in a range of
Available online 23 October 2017
environments (including soils, water, sediments, and indoors) and in organisms. The concentrations and
Handling Editor: Frederic Leusch detection rates of agricultural pyrethroids, which always contain a-cyanogroup (a-CN), such as cyper-
methrin and fenvalerate, decline in the order of crops > sediments > soils > water. Urban pyrethroids
Keywords: (not contain a-CN), such as permethrin, have been detected at high levels in the indoor environment, and
Pyrethroids 3-phenoxybenzoic acid, a common pyrethroid metabolite in human urine, is frequently detected in the
Residue distributions human body. Pyrethroid pesticides accumulate in sediments, which are a source of pyrethroid residues in
Transport pathways aquatic products.
Ecological risks
© 2017 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 991
2. Spatiotemporal variation in pyrethroids in species and their frequency of detection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 991
3. Pyrethroid residues in environmental media . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 992
3.1. Pyrethroid residues in soils . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 992
3.2. Pyrethroid residues in surface water . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 993
3.3. Pyrethroid residues in sediments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 995
3.4. Indoor pyrethroid residues . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 996
3.5. Pyrethroid residues in crops . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 998
3.6. Pyrethroid residues in aquatic organisms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 998
3.7. Pyrethroid residues in land organisms and their secretions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 999
3.8. Pyrethroids and their metabolite residues in the human body . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 999
4. Pathways of pyrethroid transportation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1001
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1002
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1002

* Corresponding author. No. 308 Ningxia Road, College of Environmental Sciences

and Engineering, Qingdao University, Qingdao, China.
E-mail address: yandongyun666@hotmail.com (D. Yan).

https://doi.org/10.1016/j.chemosphere.2017.10.115
0045-6535/© 2017 Elsevier Ltd. All rights reserved.
 W. Tang et al. / Chemosphere 191 (2018) 990e1007 991

Supplementary data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1002

References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1002

1. Introduction provide a technical basis for future ecological risk assessments and
pollution management.
Pyrethroids are a class of synthetic organic insecticides derived
from pyrethrins. They have been used worldwide since the 1980s
2. Spatiotemporal variation in pyrethroids in species and
because of their high level of effectiveness and low toxicity
their frequency of detection
compared to other insecticides, such as organophosphorus and
carbamic ester compounds (Yoo et al., 2016). Pyrethroid pesticides
We reviewed the reported levels of pyrethroids and their me-
had become one of the three major kinds of pesticides (Xiao et al.,
tabolites in various environmental media (soils, water, and sedi-
2012), and the global synthetic pyrethroids market is valued at
ments) and organisms (plants, animals, and humans). In total, 31
$1633.03 million in 2016 (QYResearch Group, 2017). Based on their
pyrethroids and 8 metabolites were reported in these media.
molecular structure, they can be divided into agricultural pyre-
Cypermethrin was the most frequently detected pyrethroid (102
throids (alpha-, with medium toxicity) and urban pyrethroids (not
times: see Table $1), followed by permethrin (73 times), delta-
containing alpha-, with low toxicity), which are primarily used for
methrin (66 times), fenvalerate (59 times), and bifenthrin (57
agriculture and nonagricultural pest control, respectively. Pyre-
times), all of which are commonly used. Cyphenothrin, kadethrin,
throids also play a vital role in personal care products such as
tefluthrin, and bioallethrin were reported only once in water
shampoo and mosquito-repellent perfume. Cypermethrin, delta-
samples. b-cyfluthrin was reported only once in sediments. Fur-
methrin, fenpropathrin, fenvalerate, bifenthrin, permethrin, l-
amethrin, transfluthrin, and metofluthrin were reported only once
cyhalothrin, and cyfluthrin have been widely used in recent years
in and around homes, while 3-PBA was the main pyrethroid
(Gong, 2013). Compared to traditional pesticides, pyrethroid pes-
metabolite reported in the human body.
ticides have less potential to pollute the environment, but can enter
Annual variation: Based on 176 published papers, we produced
organisms through food chains. They are very toxic to aquatic or-
graphs of the number of studies of pyrethroid residues and the
ganisms and may cause long-term adverse effects in aquatic envi-
highest concentrations reported in various media over the past
ronments (Zhao, 2014). Due to the lipophilicity of pyrethroids, it is
three decades (Fig. 1). Concentrations of water, indoor environment
difficult to remove them once they enter an organism. Long-term,
and human body were not included because of differences in the
low-dose exposure to pyrethroids can cause chronic diseases and
units. It should be noted that most of the studies included in this
have toxic effects on the nervous, immune, cardiovascular, and
review were published in the last 10 years (from 2007 to the pre-
genetic systems of organisms, inducing teratogenicity, carcinoge-
sent); therefore, the situation before 2007 may not have been
nicity, and mutagenicity (Ma, 2009). Koureas et al. (2012) provided
accurately represented. The number of studies of pyrethroid resi-
evidence that pyrethroid exposure is associated with adverse ef-
dues in the environment has increased over time. The two earliest
fects on the male reproductive system. Radwan et al. (2015) found
datasets were from indoor investigations in China (low concen-
that urinary pyrethroid metabolite levels are significantly related to
trations). Highest concentrations (trans-permethrin,
sperm aneuploidy. In case-control studies in Shanghai and Shanxi
375700.00 ng g 1) were detected in bed sediments in Osun, Nigeria,
provinces in China, the geometric mean concentrations of urinary
in 2016.
pyrethroid metabolites of patients were higher than those of
Fig. 2 shows the overall increasing trend in the detection of
healthy children, indicating that exposure to pyrethroid pesticides
pyrethroid residues over the past three decades. Between 2006 and
may be associated with an increased risk of childhood brain tu-
2016, not including 2007 and 2010, more than or equal to 10 py-
mors, childhood acute lymphocytic leukemia, and coronary heart
rethroids were detected every year, and 2014 had the largest fre-
disease (Ding et al., 2012; Chen et al., 2016; Han et al., 2017). In
quencies of detection of 16 pyrethroids, as shown in Fig. 2. The
addition, children with urinary 3-phenoxybenzoic acid (3-PBA)
frequency of detection of agricultural pyrethroids was greater than
levels above the limit of detection (LOD) are twice as likely to have
that of urban pyrethroids, but the frequency of detection of both
attention deficit hyperactivity disorder compared to those with
groups increased during the past three decades. Annual variation
urinary 3-PBA levels below the LOD. Moreover, hyperactive-
over the past decade is not obvious, probably because the degra-
impulsive symptoms increased by 50% for every 10-fold increase
dation rate of pyrethroid pesticides changes with different envi-
in 3-PBA levels (Wagner-Schuman et al., 2015). In 2015, pesticides
ronmental conditions and environmental regulations. The
were measured in carpet dust from the houses of 277 children with
difference in pyrethroid residence time in different environments
leukemia and 306 controls in northern and central California,
might be another important reason for the lack of obvious annual
United States, where pyrethroid residues were derived from home
variation.
and garden pest treatments. Cyfluthrin and cypermethrin were
Regional differences: Pyrethroids have been widely detected at
detected in 25.0% and 49.0% of the homes, respectively, and
the global scale, with most reports being from China (41.8%) and the
permethrin had the highest median concentration of 1062 ng g 1
United States (21.2%). These two countries have the first and second
(Deziel et al., 2015).
largest production and use of pesticides in the world, respectively.
Many studies have investigated pyrethroid insecticides at the
However, the fact that the available research reports are written in
global scale. Li et al. (2017) reported the global occurrence of py-
English and Chinese may be another reason for the dominance of
rethroid insecticides in sediments and the associated toxicological
reported detection in these two countries. In China, there are more
effects on benthic invertebrates. However, reports are lacking on
research data for pyrethroid residues in economically developed
pyrethroid pollution in a range of media at the global scale. The
areas than in those undeveloped regions. In the United States, py-
objectives of this review were to summarize the available studies
rethroid residues in water and sediments have been reported most
on pyrethroid residues in different media at the global scale, and to
frequently in California. Because there are more available data for
992 W. Tang et al. / Chemosphere 191 (2018) 990e1007

Fig. 1. Numbers of studies in which pyrethroids were detected and the highest concentrations of pyrethroids over time (Not including concentrations of water, indoor environment
and human body because of different units).

China, the discussion of pyrethroid residues in different media in
this study first considers the situation in China and then other
countries and regions.
There are 33 countries that reported pyrethroid residues in
the environment in this review, with 10 from Asian and Europe
each. This is obviously related to the large number of countries in
these two continents. In Africa, pyrethroids are usually used to
treat mosquito nets to control malaria. In 2001, when a major
dengue epidemic occurred in Brazil, the National Health Foun-
dation used pyrethroid insecticides to control it instead of
organophosphorus (OP) insecticides because mosquitoes had
developed resistance to OP (Corcellas et al., 2012). There are too
many such studies to list; however, there are few statistics or
experimental data regarding pyrethroid residues. Data for South
America are limited, but are widespread in terms of their
regional coverage. In North America (except the United States),
there is one published dataset in each of Canada and Mexico,
respectively. Only one dataset has been reported in Oceania
(Australia).
China: China has the largest production and consumption of
pesticides in the world, which has resulted in serious pesticide
pollution. The highest frequency of detection of pyrethroid
pesticides reported has been in Guangdong in southern China,
including the Pearl River Basin, which is an extremely active eco-
nomic area. In addition, a mature agricultural economy has devel-
oped in Sichuan and Jiangsu. The development of advanced
agriculture and cities has resulted in high levels of pesticide con-
sumption. Pesticide companies are usually located in well-
developed cities and their suburbs. More monitoring and decon-
tamination programs have been undertaken in well-developed
regions with serious pesticide pollution issues by government
and institutes, resulting in more available data.
3. Pyrethroid residues in environmental media
3.1. Pyrethroid residues in soils
Pyrethroid concentrations in soils worldwide are shown in
Table 1; eight pyrethroids were detected in soils worldwide, with
all eight reported in China, of which six were found in other
countries and regions. Cypermethrin was the pyrethroid most
frequently detected in China (11 times), but it was detected only
twice in other countries and regions. Fenpropathrin and cyfluthrin
were detected only in China.

Fig. 2. Numbers of agricultural and urban pyrethroid detections reported over time.
 W. Tang et al. / Chemosphere 191 (2018) 990e1007 993

Table 1
Pyrethroid residue concentrations in soils worldwide.
1
Samples type Region Concentration (ng g )

China
tea garden soils (Li, 2007) Chongqing 9.00e52.00
tea garden soils (Tan et al., 2008b) Sichuan 17.00e312.00
lei bamboo forest soils (Guo et al., 2008) Zhejiang 1.75e92.96
litchi orchard soils (Yao et al., 2010) Guangdong 7.83a
litchi orchard soils (Yao et al., 2011) Guangxi NDe60.30
Fujian NDe0.89
framland soils (Yin et al., 2011) Yunnan NDe44.90
vegetable soils (Dai et al., 2012) Yunnan NDe63.60
grapes soils (Qiang et al., 2013) Jiangsu 5.00e36.00
framland soils (Gong, 2013) Chongqing NDe906.05
tea garden soils (Liu et al., 2015b) Jiangsu 7.50e38.00
orchard soils (Zhu et al., 2015) Chongqing NDe2.50
persimmons, jujubes soils (Liu et al., 2016) e NDe400.10
Other countries and regions
soils (Fernandez-Alvarez et al., 2008) Spain 4.00e60.00
framland soils (Kumari et al., 2008) India (Haryana) NDe35.00
soils (Riederer et al., 2010) The United States (Atlanta) 1.97e724.19
soils (Murugan et al., 2013) India (Andaman Islands) NDe19.17
framland soils (Mawussi et al., 2014) Togo NDe3.73
farmland soils (Rafique et al., 2016) Pakistan (Punjab) 0.07e1184.00

Note: a: average; ND: not detected or below the detection limit.

Through analysis of the maximum concentrations of pyrethroids
(Table 1: average concentrations are not listed because of their
absence from most reports), it was apparent that Chongqing was
the most polluted location in China, with the highest pyrethroid
residue concentration (906.05 ng g 1) being detected in cropland
soils in the Liang Tan River Basin (Gong, 2013). The Liang Tan River
Basin is a major producer of grains, vegetables, oilseeds, and silk-
worm cocoons in Chongqing, with well-developed agriculture,
forestry, livestock, and tertiary industries (Gong, 2013). The same
study also detected high concentrations (503.70 ng g 1) of pyre-
throids in sediments. Sichuan, Yunnan, Guangxi, and Zhejiang had
relatively high levels of contamination, while Jiangsu, Guangdong,
and Fujian had lower levels; there were few data for other regions.
Both Sichuan and Jiangsu are agricultural regions, but the levels of
pollution in each region were very different. Yunnan and Guangxi
had lower levels of agricultural modernization than Guangdong
and Fujian, which may explain why pesticide pollution is reportedly
higher in the former than the latter region. Compared to China,
there are few reports of pyrethroid residues in soils in other
countries and regions. The highest concentration reported was in
the farmland soils of Okara, in the Punjab in Pakistan (Rafique et al.,
2016), which is well known for its fertile land. The second-highest
concentration reported was in residential soils from 11 homes in
Atlanta, Georgia, United States, with pyrethroid insecticides (cis-
and trans-permethrin, bioallethrin) being the most commonly
detected analytes (Riederer et al., 2010).
In general, concentrations of pesticide residues were higher in
regions with developed agriculture than in other areas. It was also
found that the spatiotemporal variation of pyrethroid residues in
soils varied greatly; residues were detected in some regions at very
high concentrations, which should be given more attention. The
trends in spatiotemporal distribution and annual changes in pyre-
throid residues were not obvious, which may have resulted from a
lack of relevant data.
3.2. Pyrethroid residues in surface water
Pyrethroid concentrations in surface water worldwide ranged
from not detected (ND) to 13000.00 mg L 1 (Table 2). In total, 23
pyrethroids were reported in global surface water, with 16 reported
from China and 11 from other countries and regions. Cypermethrin
was the most frequently detected pyrethroid (22 times), but was
detected only five times in China. Allethrin, prallethrin, cypheno-
thrin, tetramethrin, tefluthrin, and bioallethrin were detected only
once in China. Kadethrin, tralomethrin, and two pyrethroid me-
tabolites (3-PBA and 3-(2,2-dichlorovinyl)-2,2-dimethylycycl
opropanecarboxylic acid [DCCA]) were ND in China.
Levels of pyrethroid residues were lower in surface water than
in other media. Compared to soils, more studies have been con-
ducted on water bodies, involving a wider range of geographical
regions, with most studies focusing on the economically developed
areas of southern, eastern, and central China. More data are avail-
able regarding pyrethroid residues in water bodies than for other
environmental media. The highest concentration (29.72 mg L 1)
reported was in the Pearl River in the south of China (Wang et al.,
2013b). In another study (Zhao, 2014) of the same river, seven py-
rethroid compounds were detected, but at lower concentrations.
Permethrin was the dominant pyrethroid in this study, while
bifenthrin was detected in the two studies referred to above.
Guangdong Province, particularly the Pearl River Delta in southern
China, is one of the most economically advanced regions of China,
where high exposure to residues of urban pyrethroids, such as
bifenthrin and permethrin, may result from their common use in
urban areas for the management of structural and landscape pests.
By contrast, agricultural pyrethroids such as fenpropathrin and
cypermethrin had a high frequency of detection in Hu'nan and
Zhejiang, which may be due to their wide agricultural distribution
and high grain output, and the ease of transportation of pesticides
from soils or plants to water bodies through groundwater, rain, or
surface runoff. Pollution levels in Anhui, Jiangsu, and Heilongjiang
were reported to be lower. Wu (2015), who studied pyrethroid
residues in water samples from four rivers running into Chao Lake
in Anhui, reported that permethrin was the dominant pyrethroid,
with the highest frequency of detection (100%), followed by bio-
allethrin. Pyrethroid pollution in the Nanfei River, which is the
main river in Anhui, was much higher than in the other three rivers.
Moreover, pyrethroid residues were also detected in rural drinking
water sources in Yantai, Shandong Province (Xu et al., 2015). Un-
fortunately, no detailed concentration data were reported in that
study.
Pyrethroid residues have also been frequently reported in water
bodies in California. The pyrethroid residue detected at the highest
994 W. Tang et al. / Chemosphere 191 (2018) 990e1007

Table 2
Pyrethroid residue concentrations in water worldwide.
1
Samples type Region Concentration (ng L )

China
surface water, fish pond water (Hu and Liu, 2001) Jiangsu 2.50e30.00
sewage (Chen et al., 2005) Beijing 13.00e1246.00
river water (Zang et al., 2008) Hebei 160.00e210.00
river water (Zhao, 2009) Zhejiang NDe16400.00
river water (Zong et al., 2009) Guangdong 70.00e110.00
seawater (Zhao, 2009) Zhejiang NDe16200.00
seawater (Chen et al., 2009) Fujian present
seawater (Wang et al., 2010) Fujian NDe6360.00
seawater (Song et al., 2012) Fujian 4.68e29.72
river water (Li and Chen, 2013) Heilongjiang 52.00
river water (Gong, 2013) Chongqing NDe409.11
river water (Wang et al., 2013b) The Yangtze River 2700.00
The Pearl River 4680.00e29720.00
river water (Zhao, 2014) The Pearl River NDe730.00
river water (Liu and Zhang, 2014) Anhui ND-13.90
river water (Wu, 2015) Anhui 0.05e13.86
water source (Xu et al., 2015) Shandong present
polluted pond water (Chen et al., 2015) Hu'nan 12470.00; 19080.00
Other countries and regions
ground water (Kumari et al., 2008) India (Haryana) 17.00e90.00
river water (Nigam et al., 2008) India (Ganga) present
river water (Feo et al., 2010a) Spain (Tarragona) 4.94e30.50
river water (Feo et al., 2010b) Spain (Ebro River) 0.73e58.78
river water (Elfman et al., 2011) Philippines (Leyte) 0.50e1400.00
river water (Moreno-Villai et al., 2012) Mexico (Sonora) 29400.00max
lake water (Yurtkuran and Saygi, 2013) Turkey (Kızılırmak Delta) 1.00e8.00
river water (Toan et al., 2013) Vietnam (Mekong delta) 3550.00
river water (Fernandez-Ramos et al., 2014) East of the Czech Republic (Hradec Kr

)
alove 26110.00
lake water 34530.00
seawater (Langford et al., 2014) Norway <10.00 D
river water (Chau et al., 2015) Vietnam (Mekong delta) 770.00
river water (Mahboob et al., 2015) Pakistan (River Ravi), 2015 4.20e2680.00
lake water (Hossain et al., 2015) Bangladesh (Savar), 2015 ND-80500.00a
lake water (Papadakis et al., 2015) Greece (Macedonia, Thrace, Thessaly), 2015 present
raw wastewater from WWTPs (Rousis et al., 2016) Italy (Cremona, Milan, Merano, Florence, Terni, Bari, Palermo), 2016 3-PBA(180.00max)
trans-DCCA/cis-DCCA(7.00e220.00)
river water (Nesser et al., 2016) Sudan (White Nile water), 2016 ND-926.50
wetland near the farm (Mimbs et al., 2016) The United States (Nebraska), 2016 260.00max
river water (Hapke et al., 2016) The United States (Oregon), 2016 0.14max; Present
The United States (California)
river water (Woudneh and Oros, 2006b) ND-0.26
runoff of Nursery (Lao et al., 2008) present
urban runoff (Weston et al., 2009) <3.00u-252.00
river water (Hladik and Kuivila, 2009) ND-15.00
constructed wetlands; Tailwaters (Budd et al., 2009) ND-470000.00
urban runoff (Weston and Lydy, 2010) 3.50max-45.80max
POTWs 1.70max-17.20max
agricultural drains 3.90max-17.50max
river water (Ensminger et al., 2011) 5.00e21.00
river water (Delgado-Moreno et al., 2011) 500.00e13000000.00max
river water (Xu et al., 2016) 2011act 11.00max
urban runoff (Ensminger et al., 2013) 20.00 a
municipal wastewater (Weston et al., 2013) 200.00e500.00

Note: u: usually; o: occasionally; max: maximum; D: dry weight; W: wet weight.

concentration (13000.00 mg L 1) was trans-permethrin in the
coastal watersheds of southern California. This was also the highest
concentration of this residue reported at the global scale (not
including China). The unusually high concentration was primarily
due to an accident, but may have also been enhanced by spray drift
during application, cleaning of spray equipment, or improper
disposal of spray waste (Delgado-Moreno et al., 2011). From 2006 to
2013, there was continuous monitoring of pyrethroid pesticides in
California. However, the data collected indicated no significant
trend in pyrethroid residues. The most ubiquitous pyrethroid
detected was Bifenthrin, which could have originated from use by
private consumers or professional pest controllers (Weston et al.,
2009). The highest concentration (80.50 mg L 1) of cypermethrin
other than in China and the United States was reported in Savar,
Bangladesh, where agriculture is the main economic activity
(Hossain et al., 2015). High concentrations of pyrethroid residues
were also reported in the east of the Czech Republic (fenvalerate,
34.53 mg L 1) (Fernandez-Ramos et al., 2014) and at Sonora in
Mexico (cypermethrin, 29.40 mg L 1) (Moreno-Villai et al., 2012).
Other than the countries or regions listed above, reported pyre-
throid concentrations were all below 5.00 mg L 1.
Pyrethroids are primarily transported downstream from agri-
cultural or urban areas to surface water through surface runoff or
drainage channels. In the Mekong Delta of Vietnam, cypermethrin
has been infrequently detected in water samples, whereas after
heavy rainfall, cypermethrin concentrations have occasionally
reached 3.55 mg L 1 (Toan et al., 2013). Most pyrethroids will be
transported into sediments after entering water bodies, while some
 W. Tang et al. / Chemosphere 191 (2018) 990e1007 995

will evaporate into the atmosphere or enter the ocean. Zhao (2009)
analyzed pyrethroid residues in seawater and fresh water in the Ao
river basin in Zhejiang, China. The study found that pyrethroid
levels were always lower in the river mouth than in the fresh water
of the river due to dilution by seawater. Pyrethroid residues in
surface water can also enter organisms through food chains, which
should not be ignored.
3.3. Pyrethroid residues in sediments
Pyrethroid concentrations in sediments worldwide are shown
in Table 3, and were found to range from ND to 375700.00 ng g 1. In
general, levels of pyrethroids were higher in sediments than in
surface water. Most sediment samples were collected from surface
sediments, with only a few samples being suspended solids

Table 3
Pyrethroid residue concentrations in sediments worldwide.
1
Samples type Region Concentration (ng g )

China
costal sediments (Yang et al., 2010) Fujian 5.60e9.50
river sediments (Li et al., 2011a) Pearl River Delta D 0.65e384.00
river sediments (Fang et al., 2012) Liaohe River Basin NDe19.60
lake sediments (Fang et al., 2012) Taihu Lake Basin D NDe2.91
estuarine sediments (Zhao et al., 2013) The Pearl River D NDe94.00
river sediments (Gong, 2013) Chongqing NDe503.70
lake sediments (Qi et al., 2015) Taihu Lake Basin D 0.11e0.21
river sediments (Wu, 2015) Chaohu Lake Basin 0.06e66.01
sediments core 1.09ae10.60a
urban waterways (Sun et al., 2015) Guangdong 50.00e4960.00
lake and river sediments (Zhao et al., 2016) Taihu Lake Basin NDe562.00
Chaohu Lake Basin NDe991.00
lake and river sediments (Ding et al., 2016) Chaohu Lake Basin 0.08e2.95
sediments cores of a rural river (Sun et al., 2016) Fujian 1.70e1631.00
sediments cores of suburban river (Sun et al., 2016) Guangdong NDe29.80
Other countries and regions
river sediments (Yasin et al., 1996) British (Meltham) NDe309.50
river sediments (Feo et al., 2010b) Spain (Ebro River) 8.27e71.90
lake sediments (Yurtkuran and Saygi, 2013) Turkey (Kızılırmak Delta) 9.50e385.00
river sediments (Toan et al., 2013) Vietnam (Mekong delta) 34.80a
riverine suspended solids (Sangchan et al., 2014) Thailand (Chiang Mai) 0.20e52.90
river sediments (Duong et al., 2014) Vietnam (Hanoi, ho chi minh city) D NDe59741.00
marine sediments (Langford et al., 2014) Norway D <15
wetland sediments (Allinson et al., 2015) Australia (Melbourne) D 59.00max
river sediments (Mahboob et al., 2015) Pakistan (River Ravi) 660.00e5580.00
river sediments (Jabeen et al., 2015) Pakistan (Indus River) W 183.00e318.00
stream sediments (Hunt et al., 2016) Argentina (Buenos Aires) D <0.25e8.32max
Paraguay <0.25e16.57max
Brazil <0.25e4.94max
bed sediments (Olutona et al., 2016) Nigeria (Osun) 770.00maxe375700.00max
bed sediments (Kuivila et al., 2012) The United States (Atlanta, Boston, Milwaukee-Green Bay, 11.20max
Dallas-Fort Worth, Denver, Salt Lake City, Seattle-Tacoma)
(Atlanta, Dallas-Fort Worth, Milwaukee-Green Bay, 3.00max
Seattle-Tacoma, Salt Lake City)
Dallas-Fort Worth 8.90max
Dallas-Fort Worth, Denver 9.30max
Boston, Denver, Seattle-Tacoma 38.30max
wetland sediments (Belden et al., 2012) The United States (Nebraska) 17.00
(Kansas, Nebraska, Colorado) 1.10
(Oklahoma, New Mexico, Texas) 6.10
The United States (California)
river sediments (Xu et al., 2016) 2004act D
183.00max
2005act 21.80maxe993.00max
2009act 8.59maxe512.00max
2010act 8.48max
2011act 112.00max
lake sediments 2009act 2.47max
irrigation canal and river sediments (Weston et al., 2004) 16.80e459.00
river sediments (Weston et al., 2005) D NDe736.00
river sediments (Woudneh and Oros, 2006a) 17.60
river sediments (Amweg et al., 2006) 2.00maxe430.00max
commercial nursery (Lao et al., 2008) 1.40e486.60
urban waterways (Holmes et al., 2008) D NDe219.00
river sediments (Weston et al., 2009) D NDe1211.00
riverine suspended solids (Hladik and Kuivila, 2009) (NDe870.00) ng L 1
river sediments (Ensminger et al., 2011) D NDe74.40
river sediments (Delgado-Moreno et al., 2011) 0.50e1100.00
riverine suspended solids (Ng et al., 2012) 21.60maxe83.00max
estuarine sediments 19.70; 35.60
marine sediments 10.60max
river sediments (Ensminger et al., 2013) present
suspended solids (Chinen et al., 2016) 27.15maxe1407.63max
996 W. Tang et al. / Chemosphere 191 (2018) 990e1007

(marked in Table 3). In total, 13 pyrethroid compounds were
detected in sediments worldwide, of which 8 were reported from
China and all 13 reported from other countries and regions. b-
cyfluthrin, ethofenprox, cyhalothrin, resmethrin, and tralomethrin
were ND in China. Permethrin was the most frequently detected
pyrethroid (28 times), followed by cypermethrin (26 times),
bifenthrin (25 times), and fenvalerate (20 times). Generally, pyre-
throids were detected less frequently in China than in other
countries. However, fenpropathrin was detected six times more
frequently in China than in other countries.
The regions where pyrethroids were detected in sediments were
similar to those where they were detected in water. For example,
Gong found that fenpropathrin and permethrin were the dominant
pyrethroids in both water and sediment samples in the Liang Tan
River, Chongqing (Gong, 2013). Pesticides from other environ-
mental media can become concentrated in sediments, as demon-
strated by studies conducted in Guangdong. The highest reported
concentration (4960.00 ng g 1) of pyrethroids in any environ-
mental media in China was in sediments from Guangzhou College
City and the adjacent area in Guangdong (Sun et al., 2015). The use
of pesticides is reduced when farmland is converted to suburban
land (Sun et al., 2016). However, traces of pesticides remain in
suburban sediments. In general, the mildly toxic agricultural py-
rethroids, which always contain a-CN, were the dominant pyre-
throids in Guangdong. Permethrin is not an agricultural pyrethroid,
but has been frequently reported in such locations. This phenom-
enon is worthy of attention because it indicates that the application
of pesticides changes with urbanization. In addition, permethrin
was detected with the highest frequency in Chaohu Lake Basin,
Taihu Lake Basin and Liaohe River Basin. Studies conducted in Taihu
Lake Basin and Liaohe River Basin (Fang et al., 2012; Qi et al., 2015)
showed that permethrin was the dominant pyrethroid, followed by
cypermethrin and fenvalerate. Risk assessment studies in Chaohu
Lake Basin and Taihu Lake Basin showed that permethrin strongly
affected the aquatic environment of Chaohu Lake Basin, while
esfenvalerate strongly impacted both lakes (Zhao et al., 2016).
Studies in China have indicated that pyrethroid residues in sedi-
ments have increased over time.
Among other countries and regions, Osun of Nigeria had the
highest reported concentration of pyrethroid residues, with a trans-
permethrin concentration of 375.70 mg g 1 (Olutona et al., 2016);
lower cis-permethrin concentrations were reported in the same
study. This was the only report from Nigeria, and such high pyre-
throid residue concentrations were probably related to the high
population. In California, the reports of pyrethroid residues in
sediments are as plentiful as the reports in water samples. A study
in Los Angeles showed that the likely emissions of total pyrethroids
from the Upper Ballona Creek watershed were within the range of
4000 to 10,000 g y 1 (Chinen et al., 2016). Another study in Salton
Sea and its primary tributaries from 2002 to 2012 found that py-
rethroid concentrations in sediments increased consistently after
2009 (Xu et al., 2016). From the available data for California, it was
apparent that bifenthrin was the most commonly detected pyre-
throid in sediments, followed by cypermethrin, cyfluthrin,
permethrin, and fenvalerate. It is likely that pyrethroid residue
concentrations are higher in developed regions. For example, the
highest concentration reported in California (1407.63 ng g 1) was
close to that reported in Fujian, China, while the highest reported
concentration in China was in Guangdong. From Table 3, it can be
seen that some pyrethroid concentrations reported in underde-
veloped regions (e.g., Nigeria, Vietnam, and Pakistan) were higher
than in Guangdong, while low levels of residues were reported in
Norway and some areas of America. Attention should be given to
these areas, but more evidence is needed to draw a firm conclusion.
The impact of population and level of development on pesticide
degradation are important factors influencing pesticide residue
concentrations in environmental media. Compared to China, the
pyrethroid concentrations in sediments in other countries and re-
gions displayed no obvious trend over time. The earliest published
report of pyrethroid pollution in sediments was of cis-permethrin
in Meltham, United Kingdom, in 1996, at a high concentration of
309.50 ng g 1.
3.4. Indoor pyrethroid residues
Pyrethroid pesticides are widely used indoors, accounting for

Table 4
Pyrethroid residue concentrations indoor worldwide.

Samples Type Region Pesticide Type and Concentration

China
3
air (He et al., 1986) Hebei (0.01e0.06) mg m
3
air (China preventive medicine academy of sciences institute Beijing (0.01e0.08) mg m
of labor hygiene and occupational disease, 1990)
3
air (Huang et al., 2000) Guangdong (0.01e2.69) mg m
3
air (Tan et al., 2008a) Guangdong (0.01e0.04) mg m
air (Zhang et al., 2009) Shandong present
Other countries and regions
air (Berger-preieß et al., 1997) Germany (Berlin) (0.10e2000.00) mg m 3
air (Rudel et al., 2003) The United States (<3.70) ng m 3
air (Leng et al., 2005) Germany (Berlin) (4.90e45.70) ng m 3
air (Morgan et al., 2007) The United States (North Carolina and Ohio) (<11.90) ng m 3
air (Yoshida, 2009) Japan (0.15e148.00) mg m 3
dust (Berger-preieß et al., 1997) Germany (Berlin) (50.00e800.00) mg g 1
dust (Rudel et al., 2003) The United States (7.04e16.50) mg g 1
dust (Leng et al., 2005) Germany (Berlin) (1.00e70.00) mg g 1
dust (Obendorf et al., 2006) The United States (New York states) (0.03e9.40) mg m 3
dust (Morgan et al., 2007) The United States (North Carolina and Ohio) (0.14e84.23) mg g 1
dust (Regueiro et al., 2007) Italy (Bergamo) (0.02e5.13) mg g 1
dust (Harnly et al., 2009) The United States (California) (>5.00) mg g 1
dust (Stout et al., 2009) The United States (Washington, D.C.) (2.22e2.90) ng cm 2
dust (Quiros-Alcala et al., 2011) The United States (California) (0.05e13.50) mg g 1
dust (Deziel et al., 2015) The United States (California) (<1.06) mg g 1
 W. Tang et al. / Chemosphere 191 (2018) 990e1007 997

more than 80% of the total market of public health insecticides. The
degradation rates of pyrethroid pesticides are much lower in indoor
than outdoor environments. In total, 19 pyrethroids have been re-
ported in the indoor environment worldwide (Table 4), among
which permethrin was the most frequently detected (18 times),
followed by deltamethrin and cypermethrin (six times each).
Compared to levels in soils, water, and sediments, pyrethroid res-
idue concentrations were higher indoors, which can result in
adverse health effects on human beings. For example, in a health
examination of 199 workshop workers packing pesticides in
Xingtai, China (He et al., 1986), after being exposed to contaminated
air for 0.5e4.5 months, two-thirds who already had a certain de-
gree of skin infection suffered facial discomfort, while one-third of
them suffered from sneezing and runny noses. The number of
workers who had adverse reactions was greater in summer than in
winter. Similar symptoms were also reported in air-monitoring
studies at other workshops in China (China preventive medicine
academy of sciences institute of labor hygiene and occupational
disease, 1990).
Studies of indoor air pollution in Beijing and Guangdong, China,
have shown that fenvalerate and deltamethrin were relatively
frequently detected, but in low concentrations. This is probably
because the vapor pressure of pyrethroids is low, and it is therefore
unlikely that they will become concentrated in air. The scarcity of
reports of indoor pyrethroid residues in China may be related to the
structure of Chinese housing and the living habits of the popula-
tion. Most of the huge urban population of China resides in apart-
ments that are typically small, and only a few people have a
courtyard. Because pest infestations are rare, few insecticides are
used inside residences. Moreover, it is difficult to gather accurate
information from national censuses for such large populations. By
contrast, there have been many reports of indoor pyrethroid resi-
dues in other countries and regions. Pyrethroids were detected in
the indoor environment in Germany at a maximum concentration
of 800.00 mg g 1, with levels of residues being much larger in dust
samples than in air samples. This may be a consequence of their
chemical properties, which increase their binding affinity towards
particles and their tendency to adsorb onto household surfaces
such as carpet or dust. The density of dust samples is also greater
than that of air samples. In both 2011 (Quiros-Alcala et al., 2011)
and 2015 (Deziel et al., 2015), pyrethroid residues were detected in
residential environments in California. Only permethrin and
cypermethrin were detected in each study, and the concentrations
of cypermethrin were very different (the maximum in 2011 was
168-fold larger than that in 2015). As the second biggest agricul-
tural producer and user at the global scale, the United States makes
considerable use of insecticides. Furthermore, California is one of
the most agriculturally developed states in the United States,
resulting in a close connection between pesticides and human
livelihoods, which could potentially lead to high indoor pesticide
residue concentrations. In addition, pyrethroid residues have also
been detected in residential environments in New York (Obendorf
et al., 2006), Washington (Stout et al., 2009), North Carolina, and
Ohio (Morgan et al., 2007) of the United States, whereas they have
rarely been reported in Africa.

Table 5
Pyrethroid residue concentrations in cash crops worldwide.
1
Samples Type Region Concentration (ng g )

China
vegetables (Li et al., 2006) Jilin 5.00e641.60
vegetables (Li et al., 2006) Jiangxi 570.00max
tea products (Li, 2007) Chongqing 67.00e95.00
oolong tea (Yang et al., 2007) Yunnan 0.91e15.70
medicinal leeches (Wang et al., 2007) Anhui, Shaanxi, Beijing, Jiangxi, Shandong 4.00e352.00
tobacco (Mou et al., 2008) Yunnan 10.00e230.00
vegetables (Yan and Jin, 2008) Beijing 11.00e1980.00
vegetables (Zou et al., 2009) Guangdong 16.50e1540.00
agrocybe cylindracea (Zhang et al., 2011b) Guangdong 23.00, 31.00
mushroom 16.00
vegetables (Ding et al., 2011) Zhejiang 330.00max
vegetables (Li et al., 2011b) Shanghai 1.70e450.00
fruits (Li et al., 2011b) Shanghai 1.60e52.80
vegetables (Hu and Yan, 2012) Hubei 12.00e501.00
vegetables (Qin and He, 2013) Guangxi Present
vegetables (He et al., 2013) Zhejiang Present
tobacco leaf (Wang et al., 2013a) Hu'nan 147.00e930.00
herbal medicine decoction pieces (Cheng et al., 2013) Guizhou 0.40ae3.20a
herbal medicines (Tong et al., 2014) Major markets in China 0.80e102.40
vegetables (Li et al., 2014) Hebei 8.00e260.00
vegetables (Zheng et al., 2015) Tianjin Present
tea fresh leaves (Liu et al., 2015a) Jiangsu 23.50e51.10
honeysuckle (Tian et al., 2015) 9 provinces of China 20.00e400.00
dried dates (Yun et al., 2015) Hubei 3.30e1100.00
persimmons Hebei, Shaanxi, Shandong 15.40e222.40
jujubes (Liu et al., 2016) 59.40e2945.00
fruits (Li et al., 2016) Shandong, Shaanxi, Hebei, Henan, Liaoning, Xinjiang 5.00e1208.00
Other countries and regions
eggplant (Lu, 2011) Philippines 20.00e30.00
vegetables (Aldana-Madrid et al., 2011) Mexico 4.00e573.00
fruits, vegetables (Wongsa and Burakham, 2012) Thailand 10.00e770.00
okra (Essumang et al., 2013) Ghana (West African) 100.00e4100.00
eggplant, tomato, okra (Akoto et al., 2015) Ghana (Kumasi) 3.00ae133.00a
apple, blackcurrant, peking cabbage (Szpyrka, 2015) The region of southeastern Poland 20.00e300.00
sweet pepper (Kemmerich et al., 2015) Brazil 53.60
vegetables (Yu and Yang, 2017) Singapore 4.17
998 W. Tang et al. / Chemosphere 191 (2018) 990e1007
3.5. Pyrethroid residues in crops
Pyrethroid concentrations in crops worldwide from 2006 to
2015 are shown in Table 5. In general, pyrethroid residues were
detected much less in China than in other countries and regions,
and cypermethrin was extensively used in vegetable cultivation.
Cypermethrin was the most frequently detected pyrethroid in crops
(22 times, including 18 times from China and 4 times from other
regions), followed by deltamethrin (13 times: 9 times from China
and 4 times from other regions), while the other pyrethroids were
detected less than 10 times.
Pyrethroid residues have been widely detected in vegetables
and fruits in China. In total, eight pyrethroids (cypermethrin,
pemethrin, bifenthrin, deltamethrin, fenvalerate, l-cyhalothrin,
fenpropathrin, and cyfluthrin) were detected in China, with con-
centrations ranging from 1.60 to 1980.00 ng g 1. Cypermethrin was
the most frequently detected pyrethroid, followed by fenvalerate
and l-cyhalothrin. There were at least two pyrethroids detected in
every vegetable sample, and the highest total pyrethroid concen-
tration (1540.00 ng g 1) was detected in Guangdong in 2009, fol-
lowed by Beijing and Hubei. Pyrethroid levels were highest in leaf
vegetables (Feng and Jin, 2007), followed by melons, beans, and
root vegetables. This phenomenon may be related to the different
spraying methods used for pesticides. Although most of the resi-
dues were below the maximum residue limits (MRLs) (GB 2763-
2012) set by China, some excessive concentrations of almost all of
the pyrethroids were apparent. Pyrethroids were also detected in
edible fungus (Zhang et al., 2011b; Qin and He, 2013), tobacco (Mou
et al., 2008; Wang et al., 2013a), tea (Li, 2007; Yang et al., 2007; Liu
et al., 2015a), honeysuckle (Tian et al., 2015), and traditional Chi-
nese medicine (Wang et al., 2007; Cheng et al., 2013; Tong et al.,
2014), with respective maximum concentrations of 31.00 ng g 1
for cepermethrin, 930.00 ng g 1 for fenvalerate, 73.00 ng g 1 for
fenpropathrin, 400.00 ng g 1 for deltamethrin, and 352.00 ng g 1
for cepermethrin. Cepermethrin was the pyrethroid most
frequently detected in traditional Chinese medicine. Tong et al.
(2014) collected a total of 132 samples of Chinese herbal medi-
cines from major markets in China and found pesticide residues in
74 of them, with a frequency of detection of 4.6% for cyhalothrin,
2.3% for bifenthrin, 1.5% for cepermethrin and permethrin, and 0.8%
for fenpropathrin and cyfluthrin. Cheng et al. (2013) found pesti-
cide residues in 23 of 121 batches of 30 different Chinese herbal
Table 6
Pyrethroid residue concentrations in aquatic organisms worldwide.
Samples type
China
leech (Wang et al., 2007)
aquatic products (fish,shrimp,crab) (Jiang et al., 2007)
vivipara (Huang et al., 2008)
wild crucian (Cai et al., 2011)
aquatic products (fish,mussels) (Wang et al., 2012)
tilapia mossambica (Wang, 2013)
shrimp (Zhao, 2014)
cowry
fish
rass carp (Chen et al., 2015)
Other countries and regions
fish and shellfish (Rawn et al., 2010)
franciscana dolphins (Alonso et al., 2012)
Catla (Mahboob et al., 2015)
channa marulius (Jabeen et al., 2015)
cyprinus carpio
pooled edible fish (Corcellas et al., 2015)
fish (Dallegrave et al., 2016)
Note: L: lipid weight.
medicines produced in Guizhou, with cypermethrin having the
highest rate of detection (13.22%, 13 batches), while deltamethrin
had the lowest (0.83%, one batch).
In total, 10 pyrethroids (cypermethrin, pemethrin, bifenthrin,
deltamethrin, fenvalerate, l-cyhalothrin, fenpropathrin, cyfluthrin,
allethrin, and tetramethrin) were detected in studies of crops in
countries other than China, with concentrations ranging from 3.00
to 573.00 ng g 1. Cypermethrin and deltamethrin were frequently
detected, and cypermethrin concentrations were much higher than
those of other pyrethroids. The pyrethroid with the highest con-
centration (573.00 ng g 1) in vegetables was cyfluthrin, which was
reported in Mexico in 2011, followed by cypermethrin, which was
detected in vegetables and fruits at a concentration of 570.00 ng g 1
in Thailand in 2012. Excessive amounts of allethrin, deltamethrin,
and cypermethrin in crops have been reported. Levels of allethrin
and deltamethrin residues have been reported to exceed the Eu-
ropean Union MRLs in eggplant samples from Kumasi, Ghana. In
southeastern Poland, cypermethrin was detected in high concen-
trations of 120.00 and 300.00 ng g 1 in blackcurrants, and bifen-
thrin, which has been banned since 2011, was detected in apple and
Peking cabbage at concentrations of 20.00 and 80.00 ng g 1,
respectively.
3.6. Pyrethroid residues in aquatic organisms
There have been few reports of pyrethroid residues in aquatic
organisms at the global scale, but the available data are shown in
Table 6, with ranges from ND to 9901.40 ng g 1. In total, 10 pyre-
throid compounds have been detected in aquatic organisms, with 9
compounds reported from China and 5 compounds reported from
other countries and regions. Cypermethrin was the most frequently
detected pyrethroid, being reported four times both in China and
other regions, followed by deltamethrin, which was reported seven
times globally. Cypermethrin, deltamethrin, and bifenthrin were
detected in both China and other countries. Fenpropathrin, fen-
valerate, cyfluthrin, tetramethrin, and a-phenothrin were detected
only in China, while permethrin and cyhalothrin were ND in China.
The highest concentrations of pyrethroid residues in China and
other countries were 9901.40 ng g 1 (aquatic products from Ningbo
of Zhejiang, China) (Jiang et al., 2007) and 4938.00 ng g 1 (fish in
the Iberian River Basin, Spain) (Corcellas et al., 2015), respectively.
These were also the highest concentrations among all
1
Region Concentration (ng g )
e NDe243.00
Zhejiang W NDe9901.40
Shanghai 15.57e56.18
Zhejiang 0.30e416.23
Jiangsu NDe4.68
Hu'nan 8.57e13.41
the Pearl River 0.05e1.13
0.69e1.20
NDe3.05
Hunan 3.27e74.29
Canada 0.30e6.50
Brazil (S~
ao Paulo and Rio Grande do Sul) L
4.48e68.40
Pakistan (River Ravi) L 350.00ae3470.00a
Pakistan (Indus River) W 52.00e283.00
490.00e839.00
Spain (Iberian river) 12.00e4938.00
L
Brazil (rio grande do sul) NDe26.10
 W. Tang et al. / Chemosphere 191 (2018) 990e1007
environmental media in the two regions. Pyrethroid residues were
also frequently detected in the Ravi River, Pakistan (3470.00 ng g 1
in Cutler fish) (Mahboob et al., 2015), at levels slightly lower than in
sediments at the same location. The levels detected in other regions
were much lower. Pyrethroids are lipophilic and it is therefore easy
for them to enter the gills and blood of fish directly. In an investi-
gation of a massive die-off of fish following an accidental release of
pyrethroid pesticides in Hu'nan Province, China (Chen et al., 2015),
fenpropathrin was detected in both the internal organs and gills of
the grass carp that died from poisoning. The residue concentrations
were 22.7 times higher in the internal organs than in gills. Aquatic
organisms are impacted by pesticide residues in sediments that
have accumulated from other environmental media. These results
are in agreement with those of previous studies in the Pearl River
Delta in China, in which pyrethroid residues were detected. The
concentrations were much higher in shrimp and shellfish than in
the water and sediments, suggesting that pyrethroid levels were
enriched in aquatic organisms (Zhao, 2014). Wang et al. (2007)
investigated pyrethroid residues in leech and seahorse in tradi-
tional Chinese medicine, obtained from markets in China, and
detected cypermethrin in leech samples but not in seahorse sam-
ples. Leeches inhabit rivers, lakes, paddy fields, and swamps, and
hibernate in soils during the winter, which suggests that the high
residue concentrations found in aquatic organisms may originate
from sediments.
3.7. Pyrethroid residues in land organisms and their secretions
Studies have shown that pyrethroid residues in livestock and
their products mainly originate from residues in the feed (Cai and
Dai, 1994; Cai et al., 2003; Salas et al., 2003; Aulakh et al., 2006).
Wang et al. (2016b) found that four pyrethroid compounds in
Boehmeria nivea, which is used as livestock feed, and soils, were
positively associated with their spray dosage, but were negatively
associated with the interval between harvests. Pyrethroid residues
in land organisms and their secretions are shown in Table 7, with
little data available from outside China. In a study in Guizhou,
China, Gao et al. (2012) reported that tetramethrin and cyhalothrin
residues differed in different mutton tissues, with residues being
much lower in muscles than in internal organs (liver and kidney)
due to the lipophilic characteristics of pyrethroids. Among the
other countries and regions, the highest reported concentrations
were from Brazil, where allethrin, cyhalothrin, cypermethrin, del-
tamethrin, and tetramethrin were detected in adipose tissue
Table 7
Pyrethroid residue concentrations in land organisms and their secretions worldwide.
Samples Type
China
loquat honey, date honey, acacia honey, honey
of various flowers (Jin et al., 2006)
lime tree honey (Zhang et al., 2011a)
vitex honey (Zhang et al., 2011a)
acacia honey (Zhang et al., 2011a)
mutton tissue (Gao et al., 2012)
Other countries and regions
honey bee (Johnson et al., 2010)
female dogs (Andrade et al., 2010)
frog (Kittusamy et al., 2014)
honey (Paradis et al., 2014)
honey (Malhat et al., 2015)
honey (Pacifico de Silva et al., 2015)
honey bee (Malhat et al., 2015)
bovine milk (Bedi et al., 2015)
partridge eggs (Bro et al., 2016)
999
adjacent to malignant mammary tumors in nine female dogs, with
no predilection for breed or age, and with a contamination level of
33.3% (Andrade et al., 2010). In addition, pyrethroid pesticides are
widely used for pest control in agricultural fields, homes, restau-
rants, hospitals, schools, and farm buildings in India (Bedi et al.,
2015). Pyrethroid residues, such as cyhalothrin, cypermethrin,
fenvalerate, and deltamethrin, were detected in bovine milk in the
Punjab, India. The presence of pyrethroid residues was also re-
ported in a recent study of human breast milk samples (Sereda
et al., 2009; Corcellas et al., 2012; Feo et al., 2012; Bedi et al., 2013).
From Table 7, the highest reported concentrations of pyrethroids
in land organisms and their secretions were in female dogs in
Brazil, followed by bees in the United States, while the lowest were
in partridge eggs in France. Permethrin was detected in honey from
both the United States and Egypt, but the frequency of detection
was much higher in the United States than in Egypt. Pyrethroid
residues were also detected in Katyna in Brazil and Xiamen in
China, with fenpropathrin having the highest concentration of all
pyrethroids detected. Pyrethroid levels were particularly high in
Egypt. There are few data for land-based organisms in Table 7, but
there are data regarding the secretions of specific land-based or-
ganisms, such as honey and milk, probably because they are easier
to collect and analyze. The levels of pesticide residues differ in
different organs, which makes measurements difficult. Pesticides
are used widely and frequently in developed countries, which have
resulted in a large number of residues entering the environment.
3.8. Pyrethroids and their metabolite residues in the human body
Because food, the residential environment, and various envi-
ronmental media contain pyrethroid pesticides, these pesticides
can enter the human body in various ways. The most frequently
(67%) detected pyrethroid biomarker was 3-PBA (Morgan, 2012),
which is a urinary metabolite of several pyrethroids. The other
metabolites were 4-fluoro-3-phenoxybenzoic acid (from cyflu-
thrin), cis-DCCA (from permethrin, cypermethrin, and cyfluthrin),
trans-DCCA (from permethrin, cypermethrin, and cyfluthrin), and
cis-3-(2,2-dibromovinyl)-2,2-dimethylcyclopropane carboxylic
acid (from deltamethrin). Table 8 shows the reported concentra-
tions of pyrethroid metabolites in human urine or other secretions.
In China, the frequency of detection of urinary 3-PBA was between
36.0% and 98.8%, and the geometric mean concentrations ranged
from 0.08 to 0.97 mg L 1. During the monitoring of children in China,
urinary 3-PBA had both the highest frequency of detection and
1
Religion Pesticide Type and Concentration (ng g )
Fujian 1.00e15.40
Heilongjiang NDe2.40
Beijing NDe3.90
Hebei NDe2.60
Guizhou 2.10e114.50
The United States 19600.00
Brazil 2000.00e55000.00
India (Kerala) 26.91e42.15
France (Vende
e) 0.20e70.00
Egypt 1.30e19.00
Brazil (Caatinga) 5.00
Egypt 1.30e2.70
India (Punjab) 0.50e0.90
France 0.34  10 6
1000 W. Tang et al. / Chemosphere 191 (2018) 990e1007

Table 8
Concentrations of pyrethroids and their metabolite residues in the human body worldwide.

Metabolities Study Country n (samples size) Percent (%) Geometric mean

3-PBA Jiangsu, 2009e2010 (Qi et al., 2012) China 1149 98.8 0.97 mg L 1

Jiangsu, 2010e2011 (Wu et al., 2013) 481 83.8 0.44 mg L 1

Nanjing, 2014 (Wang et al., 2016a) 406 36.0 0.08 mg g 1

Shanghai, 2010e2011 (Ding et al., 2012) cases:176 88.1 0.54 mg L 1

controls:180 81.7 0.39 mg L 1

5 provinces of east China, 2012e2015 (Chen et al., 2016) cases:161 91.3 0.88 mg L 1

controls:170 82.9 0.44 mg L 1

Shanxi, 2013e2014 (Han et al., 2017) cases:72 94.4 e

controls:136 89.0
Mexico, 1997e2001 (Watkins et al., 2016) USA 21 46.0 0.26 mg L 1
NHANES, 2001e2002 (Wagner-Schuman et al., 2015) 687 78.9 1.14 mg L 1 A
NHANES, 2001e2002; 3032 e 0.32 mg g 1
2009e2010 (Jain, 2016) 2810 0.44 mg g 1
Mendota, 2009 (Trunnelle et al., 2014a) 208 79.8 1.14 mg L 1
California, 2007e2009 (Trunnelle et al., 2014b) 173 62.4 0.79 mg L 1 A
Gdansk, 2010e2011 (Wielgomas et al., 2013) Poland 132 79.7 0.26 mg L 1
northern Poland, 2012 (Wielgomas and Piskunowicz, 2013) 374 82.4 0.26 mg L 1
Lodz, 2008e2011 (Radwan et al., 2015) 195 e 0.17 mg L 1
Tokyo, 2002e2003 (Imai et al., 2014) Japan 322 91.3 0.68 mg L 1
Tokyo, 2009e2011 (Zhang et al., 2013) 213 e 0.33 mg L 1
Aichi, 2012e2013 (Osaka et al., 2016) 223 100.0 1.16 mg L 1
GerES IV, 2006 (Becker et al., 2006) Germany 395 90.0 0.31 mg L 1
CHMS, 2007e2009 (Ye et al., 2015) Canada 5604 99.4 1.17 nmol L 1
Featured Caribbean countries, 2008e2011 (Dewailly et al., 2014) e 295 100.0 0.54 mg L 1
KNEHS, 2009e2010 (Yoo et al., 2016) Korea 3671 e 1.83 mg g 1
Pichincha, 2010e2012 (Handal et al., 2016) Ecuador 26 27.0 0.12 mg L 1
Bangkok, 2014 (Fiedler et al., 2015) Thailand 53 e 1.74e2.26 mg g 1

Brittany, 2002e2006; France Prenatal:205 30.2 e

2008e2014 (Viel et al., 2015) Childhood:284 63.7
DCCA Pichincha, 2010e2012 (Handal et al., 2016) Ecuador 26 4.0 0.09 mg L 1
Aichi, 2012e2013 (Osaka et al., 2016) Japan 223 99.6 0.76 mg L 1
Bangkok, 2014 (Fiedler et al., 2015) Thailand 53 e 1.11e1.73 mg g 1

cis-DCCA Jiangsu, 2009e2010 (Qi et al., 2012) China 1149 95.3 0.47 mg L 1
Shanghai, 2010e2011 (Ding et al., 2012) cases:176 80.1 0.39 mg L 1
controls:180 69.4 0.27 mg L 1
Jiangsu, 2010e2011 (Wu et al., 2013) 481 68.8 0.20 mg L 1
5 provinces of east China, 2012e2015 (Chen et al., 2016) cases:161 73.9 0.22 mg L 1
controls:170 68.2 0.21 mg L 1
GerES IV, 2006 (Becker et al., 2006) Germany 395 56.0 0.12 mg L 1
CHMS, 2007e2009 (Ye et al., 2015) Canada 5604 98.5 0.38 nmol L 1
Lodz, 2008e2011 (Radwan et al., 2015) Poland 195 e 0.12 mg L 1
Featured Caribbean countries, 2008e2011 (Dewailly et al., 2014) e 295 99.0 0.17 mg L 1
Brittany, 2002e2006; France Prenatal:205 64.9 e
2008e2014 (Viel et al., 2015) Childhood:283 64.7
trans-DCCA Jiangsu, 2009e2010 (Qi et al., 2012) China 1149 98.3 1.22 mg L 1

Shanghai, 2010e2011 (Ding et al., 2012) cases:176 83.5 0.47 mg L 1

controls:180 74.4 0.32 mg L 1

Jiangsu, 2010e2011 (Wu et al., 2013) 481 97.1 1.00 mg L 1

5 provinces of east China, 2012e2015 (Chen et al., 2016) cases:161 85.7 0.56 mg L 1

controls:170 75.9 0.29 mg L 1

GerES IV, 2006 (Becker et al., 2006) Germany 395 74.0 0.20 mg L 1
1
CHMS, 2007e2009 (Ye et al., 2015) Canada 5604 99.6 0.96 nmol L
Lodz, 2008e2011 (Radwan et al., 2015) Poland 195 e 0.16 mg L 1
Featured Caribbean countries, 2008e2011 (Dewailly et al., 2014) e 295 99.0 0.40 mg L 1
Brittany, 2002e2006; France Prenatal:205 98.0 e
2008e2014 (Viel et al., 2015) Childhood:283 96.5
4-F-3-PBA California, 2007e2009 (Trunnelle et al., 2014b) USA 173 6.3 e
CHMS, 2007e2009 (Ye et al., 2015) Canada 5604 42.4 e
Featured Caribbean countries, 2008e2011 (Dewailly et al., 2014) e 295 71.0 0.02 mg L 1

Brittany, 2002e2006; France Prenatal:205 8.8 e

2008e2014 (Viel et al., 2015) Childhood:284 15.8
Nanjing, 2014 (Wang et al., 2016a) China 406 17.7 0.04 mg g 1

cis-DBCA California, 2007e2009 (Trunnelle et al., 2014b) USA 173 1.7 e

CHMS, 2007e2009 (Ye et al., 2015) Canada 5604 47.5 e
Lodz, 2008e2011 (Radwan et al., 2015) Poland 195 e 0.05 mg L 1

Featured Caribbean countries, 2008e2011 (Dewailly et al., 2014) e 295 77.0 0.03 mg L 1

Brittany, 2002e2006; France Prenatal:205 68.3 e

2008e2014 (Viel et al., 2015) Childhood:283 85.2
Nanjing, 2014 (Wang et al., 2016a) China 406 0.7 NC
tCDCA Aichi, 2012e2013 (Osaka et al., 2016) Japan 223 91.9 0.15 mg L 1

cis-CDDA Shanxi, 2013e2014 (Han et al., 2017) China cases:72 98.6 e

controls:136 98.5
tCDDA cases:72 90.3
controls:136 79.4
 W. Tang et al. / Chemosphere 191 (2018) 990e1007
Table 8 (continued )
Metabolities Study
cis-Cl2CA Gdansk, 2010e2011 (Wielgomas et al., 2013)
tCl2CA
Br2CA
cis–Cl2CA northern Poland, 2012 (Wielgomas and Piskunowicz, 2013)
tCl2CA
Br2CA
pyrethroids in human breast milk Brazil, Colombia, Spain, 2009e2010 (Corcellas et al., 2012)
Note: NC: not calculated; A: arithmetic mean; NHANES: national health and nutrition examination surveys; CHMS, Canadian Health Measures Survey; KNEHS, Korean National
Environmental Health Survey.
concentration in Shanxi Province, followed by eastern China. In
America, the detection rates of urinary 3-PBA were between 46.0%
and 79.8%, and the geometric mean concentrations ranged from
0.26 to 1.14 mg L 1. Concentrations of urinary 3-PBA were higher
among participants from 2007 to 2010 than among those from
2001 to 2002, perhaps because of the well-documented increase in
the use of pyrethroids for indoor and outdoor residential applica-
tions since the 2001 federally mandated phase-out of residential
use of the OP insecticides, chlorpyrifos, and diazinon (Williams
et al., 2008; Horton et al., 2011; US EPA, 2012; US EPA, 2013). In
northern Poland, exposure to pyrethroids was highest among rural
populations and children. Furthermore, diet was the main source of
exposure to pyrethroids in urban areas, with the use of pet-care
products increasing exposure (Wielgomas and Piskunowicz,
2013). In Japan, the frequency of detection of urinary 3-PBA was
between 91.3% and 100.0%, and the geometric mean concentrations
ranged from 0.33 to 1.16 mg L 1. Corcellas et al. (2012) analyzed 13
pyrethroids in human breast milk samples from areas where py-
rethroids were not used for malaria control, such as Brazil,
Colombia, and Spain, and found that cypermethrin, l-cyhalothrin,
permethrin, and fenvalerate were present in all samples.
When comparing all of the data, it was apparent that the levels
of 3-PBA were higher in Korea than in all other studies conducted
on the general population from the United States or European
Union countries, probably because most Koreans are widely
exposed to various forms of pyrethroid insecticides such as sprays
and fumigants (Yoo et al., 2016). The highest frequency of detection
of urinary 3-PBA reported was in Canada, followed by Poland, with
the United States having the fewest reports among the countries
where it was detected. The geometric mean concentration rankings
of urinary 3-PBA among pregnant women from different countries
were China, followed by Caribbean countries, Japan, America,
Ecuador, and France. Among children, the concentrations were
ranked as Thailand, followed by Japan, America, China, and Ger-
many. Because 3-PBA, cis-DCCA, and trans-DCCA are the main
metabolites of permethrin and cypermethrin, it is apparent that
permethrin and cypermethrin have been used extensively both in
China and other countries. Cyfluthrin was widely used in China,
America, Canada, France, and the Caribbean. The data revealed a
greater use of deltamethrin in Antigua and Barbuda in the Carib-
bean than in America, Canada, Poland, and France.
4. Pathways of pyrethroid transportation
The transport of pyrethroid pesticides in soil-plant systems can
occur in both directions, and depends on several factors. For
example, the degradation rate of pyrethroids in soils is related to
the pH, phosphorus content, and microbial activity of the soils.
Some reports have indicated that plants can absorb pesticides from
soils (Fantke et al., 2013), and pesticide residues in crops are always
1001
Country n (samples size) Percent (%) Geometric mean
Poland 132 8.3 e
6.8
11.3
Poland 374 46.0 e
46.8
17.1
1
e 50 8.0e100.0 1.45e24.20 ng g lw
positively correlated with those in soils. Liu et al. (2016) found that
as pyrethroid concentrations in soils increased, the concentrations
in fruits also increased, but there was no linear correlation. Re-
ported cypermethrin concentrations were generally higher in crops
than in soils. In the main tea-producing areas of Chongqing, China,
Li (2007) found that alpha-cypermethrin concentrations followed
the order: soil samples > fresh leaf samples > finished tea samples.
The infrequent detection in finished tea samples may be due to the
decomposition of insecticides during high-temperature
treatments.
Pesticides enter streams and rivers by rain scouring and trans-
port through soils, and can finally reach the groundwater or marine
environment. Given the hydrophobicity of pyrethroids, their sorp-
tion to soils, suspended particles, and sediments is an important
process in the aquatic environment. Gong (2013) modeled
permethrin behavior in the environment, and found that concen-
trations in soil samples were almost the same as the high levels in
sediment samples, while concentrations in air and water samples
were lower. When discharged into a water body, a high percentage
(96.0%) of permethrin is transported to sediments. It has also been
reported that pyrethroid levels were two orders of magnitude
lower in water than in both soils and sediments, and that cyper-
methrin and deltamethrin concentrations were higher in sedi-
ments than in both soils and water.
There is an underlying trend for pesticide residues to transfer
from water bodies to sediments. However, this trend may be
reversible when the use of pesticides is reduced and no pesticides
are discharged into water bodies. This behavior can be used to
determine whether the presence of a pesticide residue has resulted
from recent use. In the Chaohu Lake Basin, Anhui, China (Wu, 2015),
Wu found that urban and agricultural pyrethroids were predomi-
nant in water and sediment samples, respectively. The urban py-
rethroid concentration increased from the bottom to the surface of
the sediment profile, while the agricultural pyrethroid concentra-
tion decreased. Furthermore, the fugacity model evaluation of py-
rethroids indicated that urban pyrethroids were mainly transferred
from water to sediments, whereas transfer of agricultural pyre-
throids was the opposite. This indicates that usage is changing from
agricultural to urban pyrethroids. Delgado-Moreno et al. (2011)
suggested that pesticides applied during the dry season may
accumulate on the surface of soils and then be mobilized by the
overland flow caused by winter rain events.
Pyrethroids can enter the human body in different ways.
Exposure to pyrethroids is influenced by age, sampling location
(i.e., agricultural or non-agricultural areas), consumption of vege-
tables, beans, and nuts (Ye et al., 2015), and the application of py-
rethroid pesticides to textiles and in residential environments
(Ding et al., 2012). High levels of pyrethroid exposure are largely
due to the widespread use of household pesticides. Pyrethroid
residues in the human body are generally higher in locations where
1002 W. Tang et al. / Chemosphere 191 (2018) 990e1007
they are used as a mosquito repellent. For example, pyrethroid
concentrations and their frequency of detection were higher in
pregnant women living in rural areas of Jiangsu in China than in
children, and their median levels of urinary metabolites were about
4e10 times higher than those reported in the general population
from developing countries. Moreover, about half (45.5%) of the
women reported that they or their family members had used
commercially available indoor insecticides during pregnancy (Qi
et al., 2012). In addition to the use of indoor pesticides, some
agricultural pesticides can enter homes following adherence to
clothes or shoes, which may explain the high pyrethroid residues
reported in farmworker households. Permethrin is used in skin
lotions and shampoos and can therefore enter the human body by
direct exposure. Moreover, pesticide residues are also enriched in
food chains, through which they can finally reach the human body.
In general, the transport of pyrethroid pesticides in environ-
mental media can be two-directional or multi-directional and de-
pends on several factors. One-way movement usually does not exist
among two or more media. For example, water and sediments are
not only sites where pollutants are accumulated but are also
sources from which they can be released again. Due to global
transport, pyrethroid residues have also been detected in some
regions where they have never been used. We are unable to
determine the trends in pyrethroid residue movement over these
transport pathways. This may be because, although they produced
considerable amounts of data, all of the experiments reviewed here
were conducted separately; thus, the background parameters were
not consistent. In addition, the sampling methods and testing
procedures differed, which also made it difficult to draw accurate
conclusions.
5. Conclusions
Cypermethrin was the most frequently reported pyrethroid (102
times) and was detected in both environmental media and organ-
isms, with the exception of human bodies. Fenvalerate (including
fenvalerate and cis-fenvalerate) was reported 59 times. Both
cypermethrin and fenvalerate are agricultural pyrethroids. Cyper-
methrin and fenvalerate concentrations decreased in the order:
crops > sediments > soils > water, and the frequency of detection of
cypermethrin was 52.5%, 44.4%, 57.9%, and 44.0% in these media,
respectively, while the frequency of detection of fenvalerate in the
same media was 27.5%, 33.3%, 33.3%, and 26.0%, respectively.
Agricultural pesticides are usually sprayed directly onto the surface
of crops and then accumulate in soils or enter rivers and sediments
by rain scouring or other transport mechanisms. Cypermethrin and
fenvalerate concentrations generally decreased along their trans-
port pathways; however, concentrations were sometimes higher in
sediments than in soils and water, perhaps because of their hy-
drophobic properties. Pyrethroids move rapidly in streams and
rivers, but in the long-term they are likely to accumulate once they
reach sediments. Cypermethrin and fenvalerate were also detected
in residential environments, aquatic organisms, and land organ-
isms; however, the available data in these areas were limited.
Like cypermethrin, deltamethrin is also an agricultural pyre-
throid, and was reported 66 times in environmental media and
organisms. However, unlike cypermethrin and fenvalerate, delta-
methrin had a more balanced distribution between environmental
media and organisms (between 21.4% and 42.9%). The maximum
concentrations (59.74 mg g 1) were detected in river sediments in
Hanoi and Ho Chi Minh City, Vietnam, but there were also some
reports of low concentrations in sediments. High concentrations
were also detected in adipose tissue adjacent to mammary tumors
in female dogs from Brazil (55.00 mg g 1) and in dust samples from
residential environments in Berlin (54.50 mg kg 1).
Permethrin was the second-most frequently detected pyre-
throid. It is not only used as an insecticide and acaricide in home
products but is also present in skin lotions and shampoos for the
medical treatment of lice and scabies. A study in Nigeria revealed
the presence of permethrin not only in agrochemical products but
also in personal care products arising from the disposal of domestic
wastes into a stream (Olutona et al., 2016). Permethrin in envi-
ronmental media was reported 73 times, with the highest con-
centration (800.00 mg kg 1) and frequency of detection (65.0%)
reported in residential environments, followed by sediments, with
a concentration of 6410.00 ng g 1 and frequency of detection of
46.3%. Permethrin levels were much lower in other media.
As with permethrin, bifenthrin does not have a-cyano within its
structure, and its toxicity is lower than that of cypermethrin and
deltamethrin. However, unlike permethrin, it was reported only
once in a residential environment, which may indicate that it is
rarely used as a household insecticide. The highest frequency of
detection (44.5%) for bifenthrin was in sediments, and it was the
most commonly detected pyrethroid in California. Bifenthrin was
also frequently detected in the water of the Pearl River Basin and
the seawater of Fujian in southern China. Permethrin had fre-
quencies of detection of 22.0% and 17.5% in water and crops,
respectively, while concentrations were higher in crops than in
water.
The main metabolites of permethrin and cypermethrin, 3-PBA,
cis-DCCA, and trans-DCCA were commonly detected in the human
body. It is apparent that permethrin and cypermethrin have been
extensively used both in China and other countries.
There were more reports of pyrethroids in sediments, water, and
crops than in residential environments and the human body. This
may be because it is easier to collect and analyze sediment, water,
and crop samples. It may also be due to the different frequencies
and scope of pesticide use. Despite the difficulties in monitoring,
pesticide residues in residential environments and the human body
should be given more attention.
Acknowledgments
This project is supported by National Natural Science Founda-
tion of China (No. 31400371, 41571214, 41705098, 51279075), and
Major Research Projuct of Shandong Province (Public Welfare
Special) (No. 2017GNC11116).
Appendix A. Supplementary data
Supplementary data related to this article can be found at
https://doi.org/10.1016/j.chemosphere.2017.10.115.
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