Science of the Total Environment 542 (2016) 620–628

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Science of the Total Environment

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Pesticides in persimmons, jujubes and soil from China: Residue levels,

risk assessment and relationship between fruits and soils
Yihua Liu, Shiliang Li, Zhanglin Ni, Minghua Qu, Donglian Zhong, Caifen Ye, Fubin Tang ⁎
Research Institute of Subtropical Forestry, Chinese Academy of Forestry, Fuyang 311400, China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• 36.4% of persimmon and 70.8% of jujube

samples contain pesticide residues;
• 4.5% (persimmon) and 25.0% (jujube)
samples exceeded the MRLs set by
China;
• consumption risk from cyhalothrin, al-
drin and dieldrin give cause for concern.

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

Article history: Extreme and uncontrolled usage of pesticides produces a number of problems for vegetation and human health. In
Received 27 August 2015 this study, the existence of organophosphates (OPs), organochlorines (OCs), pyrethroids (PYs) and fungicides (FUs)
Received in revised form 27 October 2015 were investigated in persimmons/jujubes and their planted soils, which were collected from China. One OP (dimeth-
Accepted 28 October 2015
oate), three OCs (DDT, quintozene and aldrin), six PYs (bifenthrin, fenpropathrin, cyhalothrin, cypermethrin,
Available online 3 November 2015
fenvalerate and deltamethrin) and two FUs (triadimefon and buprofezin) were found in 36.4% of persimmons
Editor: A Covaci and 70.8% of jujubes, with concentrations from 1.0 μg/kg to 2945.0 μg/kg. The most frequently detected pesticides
in the two fruits were fenpropathrin in persimmons and cypermethrin in jujubes, with the detection frequencies
Keywords: of 30.0% and 22.7%, respectively. The residues of 4.5% (persimmon) and 25.0% (jujube) of samples were higher
Persimmon than the maximum residue limits (MRLs) of China. Compared with the fruits, more types of pesticides and higher
Jujube residues were observed in their planted soils. The most frequently detected pesticides were HCH in persimmon
Soil soil and DDT in jujube soil, with the detection frequencies of 10.9% and 12.7%, respectively. For the tested samples,
Pesticide 39.1% of fruit samples and 63.0% of soil samples with multiple residues (containing more than two pesticides) were
Residue
noted, even up to 8 residues in fruits and 14 residues in soils. Except for cyhalothrin, the other short-term risks for
Risk assessment
the tested pesticides in the fruits were below 10%, and the highest long-term risk was 14.13% for aldrin and dieldrin.
There was no significant health risk for consumers via consumption of the two fruits.
© 2015 Elsevier B.V. All rights reserved.

Abbreviations: OPs, organophosphates; OCs, organochlorines; PYs, pyrethroids; FUs, fungicides; GC, gas chromatography; LOD, limit of detection; LOQ, limit of quantification; MRL,
maximum residue limit; aHI, acute/short-term consumer health risk; ESTI, estimated short-term intake; ARfD, acute reference dose; HQ, chronic/long-term consumer health risk; EDI, es-
timated daily intake; ADI, acceptable daily intake; cHI, cumulative risk.
⁎ Corresponding author.
E-mail address: yalin_zj@163.com (F. Tang).

http://dx.doi.org/10.1016/j.scitotenv.2015.10.148
0048-9697/© 2015 Elsevier B.V. All rights reserved.
 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628
1. Introduction
The use of pesticides for crop protection is expected to increase
based on a growing world population and the need for more food sup-
plies. While pesticides increase agricultural production, bioaccumula-
tion through the food chain can eventually become a risk to mammals
because the pesticides induce certain negative effects. Public health con-
cerns regarding the improper use of pesticides and poison have in-
creased in recent years. To date, certain countries, regions and
international organizations have established maximum residue limits
(MRLs) for foodstuffs. Additionally, national food monitoring programs
for pesticides have been enacted worldwide (Jardim and Caldas, 2012;
Lozowicka et al., 2014; Skretteberg et al., 2015) to ensure consumer
health, improve management of agricultural resources and prevent eco-
nomic losses.
There have been numerous reports regarding pesticide residues de-
tected in grains (Lozowicka et al., 2014), vegetables (Shoiful et al.,
2013), milk (Tsakiris et al., 2015) and fish (Wu et al., 2013). Fruits are
one of the most important foodstuffs in people's diets, and several re-
ports also focused on their pesticide levels. In a Nordic project on pesti-
cide residues in fruit and vegetables imported from Southeast Asia, 12%
of the samples exceeded the EU MRLs (Skretteberg et al., 2015). Pesti-
cides were found in over 60% of apple samples in Poland, and the
most frequently detected pesticides were fungicides (Lozowicka,
2015). At least one pesticide was detected in 70.5% of the tomato sam-
ples from Bogota, Colombia, and the most detected pesticides were
pyrimethanil, carbendazim, dimethomorph and acephate (Arias et al.,
2014). However, information regarding pesticide residue levels in per-
simmons (Diospyros spp.) and jujubes (Ziziphus spp.) are scarce. Persim-
mons and jujubes are important fruit commodities, and they could be
made into various dry fruits and jams. There are several reports regard-
ing pesticide residue in persimmons and jujubes. The determination of
pesticide residues in persimmons using gas chromatography/negative
chemical ionization-mass spectrometry (GC/NCI-MS) (Barreda et al.,
2006) and liquid chromatography–tandem mass spectrometry (LC–
MS) (Min et al., 2011) and in jujubes using gas chromatography and
mass spectrometry (GC–MS) (Zhao et al., 2014) has been developed.
After two, three or four applications, pyrimethanil residues on the col-
lected persimmons averaged 0.44, 0.48 or 0.53 mg/kg, respectively
(Shim et al., 2007). The pesticide residues of persimmons were only re-
ported on samples collected from Konya (Ucan et al., 2009), Brazil
(Ciscato et al., 2009) and Pakistan (Parveen et al., 2011). The presence
of pesticide residues in jujubes has not been determined in any coun-
tries. China ranks 1st in the world for persimmon and jujube production,
and many products are exported to other countries every year. One of
the aims of the present study was to determine the concentrations of
pesticides (organophosphate, organochlorine, pyrethroid and 2 fungi-
cides) in persimmons and jujubes collected from different main produc-
ing regions of China between 2013 and 2014, as well as to evaluate the
health effects of detected residues.
Soil plays an important role in the pesticide residue in plants. There
are two pathways for pesticide transfer between the plants and their
planted soils. Firstly, most of the pesticides could shift or fall onto the
soil when the pesticide is applied onto plants. Next, most of the depos-
ited pesticide on the plant could be washed off by rainfall to the soil. Sec-
ondly, the residues of adsorbed pesticides in soil, especially for
organochlorine pollutants, remain as contaminants in the environment
because of their long-term persistence and mobility, and they could
enter into food again via the plant uptake effect (Fantke and Jolliet,
2015; Fantke et al., 2013). The uptake of contaminants by vegetables
has been shown to vary with vegetable types. There were significant
positive correlations between the polychlorinated biphenyls (PCBs)
and organochlorine pesticide (OC) concentrations (p b 0.05) in soils
and organic-farmed carrots but no significant correlation was found be-
tween the concentrations of any contaminants in soils and organic-
farmed potatoes (Zohair et al., 2006). Root vegetables accumulate
621
weathered organochlorine pollutants to a greater extent than other veg-
etables (Florence et al., 2015). In addition, the uptake of contaminants
by vegetables has also been shown to vary with soil type, contaminant
concentration and contaminant source (Gaw et al., 2008). Some scien-
tists even developed various mathematical models to predict uptake
of organic chemicals from soil into plants (Ding et al., 2014; Trapp,
2007), which were validated by field data from apple (Trapp, 2007),
radish (Trapp, 2015) and urban afforestation tree species (Ding et al.,
2014). However, more information regarding the uptake effect for
fruits, especially for tree-planted fruits, should be given. Another aim
of this study was to elucidate the relationship of pesticide residues be-
tween fruits and their planted soils, especially to determine if the con-
taminants in the planted soils were available for uptake by
persimmons/jujubes and, if so, to establish the relationship between
the fruits and soil contaminant concentrations. Among the tested pesti-
cides (Table 1), most OPs and OCs have long been banned for use; how-
ever, their long persistence in the environment and/or high toxicity to
humans/animals lead to the demand for monitoring their residues in
food and the environment. Moreover, the tested pyrethroids and fungi-
cides are the primary pesticides used in persimmon/jujube farming in
China.
2. Materials and methods
2.1. Chemicals
Pesticide analytical standards were purchased from the National In-
formation Center for Certified Reference Materials (Beijing, China) with
certified quality. Individual pesticide stock solutions (100 mg/L) were
prepared in acetone and stored at −20 °C. A series of dilutions contain-
ing the mixture of standards was prepared (10 mg/L) in acetone or hex-
ane. GC-grade acetone and hexane were obtained from Merck
(Darmstadt, Germany). A Milli-Q-Plus ultrapure water system from
Millipore (Milford, MA, USA) was used throughout the study to obtain
the HPLC-grade water for the analyses. Other solvents were from
Shanghai GuoYao Chemical Reagents (Shanghai, China), with pesticide
residue analysis quality.
2.2. Sample extraction and cleanup
2.2.1. Persimmon/jujube sample preparation
A representative portion of the sample (without the kernel) was
prepared using a knife and mixed thoroughly using a food chopper.
Next, 25.0 g of the homogenized sample mixed with 50 mL of acetoni-
trile was blended in a homogenizer for 2 min at high speed. The extrac-
tion solvent was filtered into a 100 mL graduated measuring cylinder
containing 7 g of sodium chloride and then was shaken vigorously
with a cap on for at least 1 min; the extraction was allowed to be sepa-
rated for approximately 10 min, then 25 mL of acetonitrile phase was
measured into a 100 mL flask and evaporated to near dryness with a ro-
tary vacuum evaporator at 40 °C. Finally, the extract was reconstituted
to 2 mL with acetone for the analysis of organophosphate (OP) residues.
For the analysis of organochlorines (OCs), pyrethroids (PYs) and
fungicides (FUs), a purification step was needed as the follows: 10 mL
of acetonitrile phase was measured in a 50 mL flask and evaporated to
near dryness with a rotary vacuum evaporator at 40 °C. The extract
was reconstituted to 2 mL with hexane, loaded into a florisil SPE car-
tridge (1.0 g, preconditioned with 5 mL of 10% acetone/hexane followed
by 5 mL of hexane). The cartridge was eluted using 5 mL of 10% acetone/
hexane. The eluant was collected and then evaporated to near dryness
with a rotary vacuum evaporator at 40 °C. Finally, the eluant was
reconstituted to the final volume of 2.0 mL with hexane.
2.2.2. Soil sample preparation
5.0 g of soil sample (sieved through a 2 mm mesh) was mixed with
2 mL of distilled water for 5 min. The sample was added with 20 mL of
622 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628

Table 1
The properties of the tested pesticides.

Pesticide CAS RN Mw Vapor pressurea (mPa) LogPa Half lifeb (d) Use situationc Dosaged Use levele
(g/mol) (g/ha)

Dichlorvos 62–73-7 221.0 2100 1.90 7.8 N 600–800 L

Methamidophos 10,265–92-6 141.1 2.3 −0.79 11.5 B / /
Acephate 30,560–19-1 183.2 0.226 −0.85 11.0 N 200–300 L
Phorate 298–02-2 260.4 112 3.86 12.5 B / /
Omethoate 1113–02-6 213.2 3.3 −0.74 10.8 N 10–20 L
Dimethoate 60–51-5 229.3 0.247 0.70 11.3 N 150–200 M
Chlorpyrifos 2921–88-2 350.9 1.43 4.70 12.2 N 150–200 M
Parathion-methyl 298–00-0 263.2 0.2 3.00 12.2 B / /
Fenthion 55–38-9 278.3 0.37 4.84 13.1 N 180–250 L
Fenitrothion 204–524-2 277.2 0.676 3.32 12.3 N 120–200 L
Parathion 56–38-2 291.3 0.89 3.83 12.4 B / /
Isocarbophos 24,353–61-5 289.3 0.52 2.70 11.8 N 120–180 L
Phosmet 732–11-6 317.3 0.065 2.96 11.6 N 150–180 L
Monocrotophos 6923–22-4 223.2 0.29 −0.22 10.9 B / /
Triazophos 24,017–47-8 313.3 1.33 3.55 12.0 N 60–90 L
DDT 50–29-3 354.5 / 6.91 Not calculated B / /
HCH 608–73-1 290.8 / 2.50 Not calculated B / /
Endosulfan 204–079-4 406.9 0.83 4.75 12.5 N 150–200 L
Quintozene 82–68-8 295.3 12.7 4.46 13.6 N 2–3 (per tree) L
Aldrin 309–00-2 364.9 3.0 6.50 14.0 B / /
Dieldrin 60–57-1 380.9 0.024 3.70 12.2 B / /
Bifenthrin 82,657–04-3 422.9 0.0178 6.60 12.5 N 4–6 M
Fenpropathrin 39,515–41-8 349.4 0.76 6.04 13.0 N 13–20 H
Cyhalothrin 68,085–85-8 449.9 1.00E−09 6.80 12.3 N 3–4 H
Cypermethrin 52,315–07-8 416.3 0.00023 5.30 11.9 N 3–4 H
Fenvalerate 51,630–58-1 419.9 0.0192 5.01 11.7 N 10–20 H
Deltamethrin 52,918–63-5 505.2 0.0000124 4.60 10.6 N 1–2 M
Triadimefon 43,121–43-3 293.8 0.02 3.18 25.7 N 20–25 M
Buprofezin 69,327–76-0 305.4 0.042 4.93 19.0 N 40–60 M

Notation.
a
The properties of the pesticides were taken from PPDB (Pesticide Properties Database, http://sitem.herts.ac.uk/aeru/ppdb/en/index.htm).
b
The half-lives of pesticides in persimmons/jujubes were estimated based on Fantke's model (Fantke et al., 2014).
c
B: banned from use in environment or fruit trees in China; N: normally used in China.
d
The dosage of pesticide was based on the usage of active ingredient.
e
H: high; M: medium; L: low.

methanol and acetone (1:1, v/v) and vortexed for 30 min; then, the
sample was centrifuged for 5 min (4000 rpm). The extracts were sol-
vent exchanged to acetone (1 mL) under a gentle stream of N2 before
OPs analysis. The purified step for OC, PY and FUanalyses in the soil sam-
ple was the same as that for the food sample described above.
(holding for 2 min) and was increased to 250 °C at a rate of 20 °C/min
(holding for 33 min). Nitrogen was used as the carrier gas, with a flow
rate of 30 mL/min. The detector temperature was 280 °C.
2.4. Quality control

2.3. Instrumental analysis
2.3.1. GC–FPD
OPs were determined using FPD in phosphorus mode. Pesticide res-
idue analysis was conducted with an Agilent 6890N gas chromatograph
equipped with a programmed temperature vaporization injector, an
Agilent AOC-20i autosampler, and an Agilent flame photometric detec-
tor. The injector temperature was 220 °C, with an injection volume of
1 μL. The detector temperature was 250 °C. Nitrogen was used as the
carrier gas at a constant flow rate of 1.5 mL/min. The flow rates of air
and hydrogen were 100 mL/min and 75 mL/min, respectively. The
makeup flow was 25 mL/min. The injection volume was 1.0 μL. OP pes-
ticides were determined with a DB-1701 capillary column
(30 m × 0.32 mm × 0.32 μm). The temperature of the column oven
was programmed from an initial value of 100 °C (held for 2 min) to
210 °C at 15 °C/min (held for 7 min), and then to 250 °C at 25 °C/min
(held for 15 min).
The residues were quantified by the external standard calibration
curve method. To avoid any interference or contamination, a procedural
blank (except with no sample added, the other experimental proce-
dures were exactly the same as that for the samples from the extraction
until the instrumental analysis) was analyzed for every batch of five
samples. No analytes of interest were detected. Relative standard devi-
ations of the method (n = 5) were below 10%, indicating acceptable re-
peatability of the method. For residue quantification, standard solutions
were prepared daily for calibration of the instrument. Multi-level cali-
bration curves in the linear response interval of the detector were creat-
ed for the quantification and good correlation (r2 N 0.995) was achieved.
The limit of detection (LOD) was the lowest addition level for the recov-
ery analysis. The LODs for the target compounds ranged from 1 μg/kg to
5 μg/kg (Table 1), with the recoveries ranging from 75.3% to 108.7% and
the relative standard deviations below 16%.
2.5. Sample collection

2.3.2. GC–ECD
OCs, PYs and FUs were determined using Agilent 6890N gas chroma-
tography with an electron capture detector (GC–ECD) and DB-1701
capillary column (30 m × 0.32 mm × 0.32 μm). The injector tempera-
ture was 240 °C, with an injection volume of 1 μL. The oven temperature
was programmed as follows: the initial temperature was 150 °C
All of the samples (22 persimmons and 24 jujubes) were collected
from 3 primary producing areas of China (Hebei, Shaanxi, Shangdong).
All samples were collected from local farmers and harvested at the ma-
turity stage between 2013 and 2014. Every sampling area was located in
the main producing areas of the corresponding persimmon/jujube pro-
duction and had a long history for persimmon/jujube production.
 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628
Representative samples were collected via random sampling: 7–10
fruits were collected from the same fruit tree, and then the collection
was repeated in the same sampling site 10 to 15 times (from different
trees with diagonal-line sampling method); the fruit samples were
then mixed to obtain one representative sample for every sampling
site (N1 kg). A corresponding soil sample (depth of 20 cm) was taken
at each sampling point by a soil auger. In one site, a final sample of
soil (N1 kg) was drawn from well-mixed samples of soils collected at
different points. All samples were wrapped in black plastic bags and
transported to the laboratory where they were prepared and stored at
−20 °C until analysis.
2.6. Health risk assessment
The acute/short-term consumer health risk (aHI) was calculated
based on the estimated short-term intake (ESTI) and the acute reference
dose (ARfD). The chronic/long-term consumer health risk (hazard quo-
tient, HQ) was calculated based on the estimated daily intake (EDI) and
the acceptable daily intake (ADI). The relevant formulas are as follows.
For precise evaluation, ARfD and ADI are expressed as a percentage of
daily intake for a 60 kg person. The hazard quotient (HQ) indicates an
unacceptable risk when it is higher than 100%, and a higher aHI/HQ
value represents higher risk.
ESTI ¼ the highest residue level  food consumption=body weight ð1Þ
aHI ¼ ESTI=ARfD  100%
EDI ¼ mean residue level  food consumption=body weight
Q ¼ EDI=ADI  100%:
The cumulative risk index (cHI) will be used for the sum of HQs from
the multiple pesticide residues that the consumer is exposed to: it is cal-
culated by summing the hazard quotients (HQs) for each pesticide in
the sample:
cHI ¼ ΣHQ:
2.7. Statistical analysis
Data were log-transformed as required for statistical analyses using
SPSS base 17.0 software. To avoid overestimating fruit and soil concen-
trations of pesticides, zero was used for results less than the detection
limits for both fruit and soil analyses (Gaw et al., 2008). The normality
of the variables was checked prior performing the test. Data were statis-
tically evaluated by one-way ANOVA analysis. When significant differ-
ences were found at a 95% confidence level (p b 0.05), the least
significant difference (LSD) test was used to determine the differences
among means. The relationship between fruit and soil was performed
independently for each pesticide and fruit.
3. Results and discussion
3.1. Pesticide residue levels in persimmons and jujubes
The concentrations of pesticide residues in the two fruits are shown
in Table 2. For OPs, only 1 jujube sample was detected with dimethoate
residue (78.0 μg/kg). Among all the metabolites of DDTs detected in this
work, p,p-DDT was the only metabolite that was detected in 1 jujube
sample, with the concentration at 32.0 μg/kg. The other DDTs, HCHs
and endosulfan were not found in the tested samples. The residues for
OPs and OCs in the two fruits did not exceed the MRLs set by China/
EU/EPA/CAC. Quintozene was also found in 2 persimmon and 2 jujube
samples, with detected residue levels of 1.0 μg/kg–31.5 μg/kg. The
623
residue of quintozene in 1 persimmon sample (31.5 μg/kg) exceeded
the MRLs. Among the OCs, the detection frequency for aldrin, which
was found in 1 persimmon and 4 jujubes, was the highest, with concen-
trations of 1.4 μg/kg–42.2 μg/kg. The detected concentration of aldrin at
42.2 μg/kg exceeded the MRL set by EU/EPA (but did not exceed the
MRL of China and CAC). Moreover, the detection frequency for PYs
was the highest among all the tested pesticide types. The concentrations
of 6 PYs had ranges of 15.4 μg/kg–222.4 μg/kg (persimmon) and 59.4
μg/kg–2945.0 μg/kg (jujube). The detection frequencies for residues ex-
ceeding the MRLs of China were 4.3% (bifenthrin), 4.3% (cyhalothrin),
2.2% (fenvalerate), and 2.2% (deltamethrin). However, due to the strict
MRLs of the EU, the detection frequencies were improved to 26.1%
(fenpropathrin), 6.5% (cyhalothrin), 30.4% (cypermethrin), and 21.7%
(fenvalerate). It is worth noting that fenvalerate residue in 1 positive ju-
jube sample was even up to 2945.0 μg/kg, which was much higher than
the MRLs. Moreover, triadimefon and buprofezin were only found in 1
jujube (10.2 μg/kg) and 1 persimmon (69.5 μg/kg), respectively.
Among all the tested pesticide types, the order for detection of dif-
ferent pesticides was PYs (54.3%) N OCs (13.0%) N FUs (4.3%) N OPs
(2.2%). The results were not similar with those in Brazil, in which OPs
and carbamates were the main pesticides found in persimmons
(Ciscato et al., 2009). The highest detection frequency for PYs resulted
from the current wide use of these pesticides in China. Many types of
PYs were also found in various vegetables (Wang et al., 2013; Yuan
et al., 2014) and fruits (Chen et al., 2011). Although most of the OCs
have been banned, they were still detected in the atmosphere, river,
ð2Þ soil and most types of organisms, owing to their highly lipophilic and
persistent properties (Xu et al., 2015). However, the detection frequen-
ð3Þ cies and residue levels for OCs in persimmons in this work were lower
than those in Konya (Ucan et al., 2009), Brazil (Ciscato et al., 2009)
ð4Þ and Pakistan (Parveen et al., 2011). Among OPs, the banned OPs were
not found, and the only detection of dimethoate resulted from the
many preparation products in use (especially mixtures with PYs). Di-
methoate was one of the most detectable OPs in vegetables (Li et al.,
2014), drinking water and raw milk (Zhao et al., 2012) from China.
Moreover, the application of fungicide control and the relatively long
half-lives (seen in Table 1) of triadimefon (25.7 d) and buprofezin
ð5Þ (19.0 d) led to the detection in the fruits.
3.2. Pesticide residue levels in the planted soils
Soil is an important indicator of the residue levels in foods. The pes-
ticide residues in the soils for persimmon and jujube cultivation are
shown in Table 3. Compared with persimmons and jujubes, the detec-
tion frequencies of pesticides in soils were obviously higher than the
former. There were 2 OPs, 13 OCs, 6 PYs and 2 FUs found in the tested
soils. Dimethoate was detected in 1 persimmon soil, with the residue
at 6.3 μg/kg. Chlorpyrifos was the most often found OP in the soils,
with concentrations that ranged from 8.3 μg/kg to 25.5 μg/kg. China
was a large producer and consumer of DDT and HCH in the last cen-
tury, and they were banned in 1992. However, due to their persis-
tence in the environment, they are still detected in food (Xu et al.,
2015) and agricultural soil (Lu and Liu, 2015). The sum of DDTs
and HCHs in the persimmon soils were 7.0 μg/kg–71.8 μg/kg and
4.5 μg/kg–14.2 μg/kg, respectively. The corresponding values in the
jujube soils were 11.9 μg/kg–238.1 μg/kg and 7.9 μg/kg–41.0 μg/kg.
In 5 of the 46 samples, the concentrations exceeded China's Soil En-
vironment Quality Standard for DDTs (Class I—50 μg/kg) (GAQ,
1995). The patterns of DDTs and HCHs in the soils were analyzed in
Fig. 1. Obviously, o, p-DDT and δ-HCH were the main isomers for
DDTs and HCHs in the soils, with average rates of 62.9% and 81.9%, re-
spectively. The ratio of α −/γ-HCH may be used to monitor the
source (technical HCH or lindane), while the ratio of α-/β-HCH
may be used to determine the usage history of technical HCH (fresh
or historical) (Lu and Liu, 2015). In this study, the two ratios were
less than 0.1, which indicated that no fresh lindane inputs occurred
624 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628

Table 2
The concentration ranges of pesticide residues in persimmon and jujube (μg/kg).

Group Pesticide Persimmon Jujube LOD MRL (China/EU/EPA/CAC)

Dichlorvos n.d. n.d. 5 200/10/500*/200

Methamidophos n.d. n.d. 5 50/10/100*/50
Acephate n.d. n.d. 5 500/10/2000*/500
Phorate n.d. n.d. 5 10/10/50*/10
Omethoate n.d. n.d. 5 20/20/none/20
Dimethoate n.d. n.d.–78.0 5 2000/20/2000*/2000
Chlorpyrifos n.d. n.d. 5 1000/50/50/1000*
Parathion-methyl n.d. n.d. 5 20/10/none/20
Fenthion n.d. n.d. 5 50/10/none/50
Fenitrothion n.d. n.d. 5 500/10/none/500
Parathion n.d. n.d. 5 10/10/none/10
Isocarbophos n.d. n.d. 5 20/none/none/20
Phosmet n.d. n.d. 5 5000/50/5000/5000*
Monocrotophos n.d. n.d. 5 30/10/none/30
G1 Triazophos n.d. n.d. 5 200/10/none/200*
G2 p,p-DDE n.d. n.d. 2 ΣDDT
p,p-DDD n.d. n.d. 2 50/50/100/50
p,p-DDT n.d. n.d.–32.0 2
o, p-DDT n.d. n.d. 2
α-HCH n.d. n.d. 2 ΣHCH
β-HCH n.d. n.d. 2 50/20/none/50
γ-HCH n.d. n.d. 2
δ-HCH n.d. n.d. 2
α-Endosulfan n.d. n.d. 2 Σendosulfan
β-Endosulfan n.d. n.d. 2 1000/50/1000/50*
Quintozene n.d.–31.5 n.d.–2.6 1 20*/20/none/20*
Aldrin n.d.–4.1 n.d.–42.2 1 50/10/20/50
Dieldrin n.d. n.d. 1 20/10/20/20
G3 Bifenthrin n.d. n.d.–59.4 2 50/50/50/50*
Fenpropathrin n.d.–222.4 n.d.–322.0 2 5000/10/2000/5000
Cyhalothrin n.d.–15.4 n.d.–583.0 2 200/20/500/200*
Cypermethrin n.d.–226.0 n.d.–249.5 2 1000/50/1000/1000*
Fenvalerate n.d.–80.1 n.d.–2945.0 2 200/20/1000/200
Deltamethrin n.d. n.d.–150.0 2 50/50/200/50*
G4 Triadimefon n.d. n.d.–10.2 5 1000/100/none/1000*
Buprofezin n.d.–69.5 n.d. 5 500/50/2500/500*

n.d. = not detected, which means that the pesticide residues were below LOD. The MRL values were set by China, EU, EPA and CAC for the corresponding pesticides in fruits (including
persimmons and jujubes) or other similar foods. Data with * mark indicate the MRL values from other similar foods when there is no MRL for the pesticide in persimmons or jujubes.
G1: organophosphates (OPs); G2: organochlorines (OCs); G3: pyrethroids (PYs); G4: fungicides (FUs).

and the technical HCHs in this area were mainly from historical usage. The
two ratios were considerably lower than those from agricultural soils of
China (Lu and Liu, 2015; Zhu et al., 2014) and other locations in the
world (Ge et al., 2013), which reflected that the historical usage and du-
ration of HCH in the forestry area (producing the two fruits) were less. En-
dosulfan, quintozene, aldrin and dieldrin were detected in less than 13% of
the samples, indicating the small use of these pesticides in the region.
Similar to DDT and HCH, it was not surprising to find the residues of aldrin
and dieldrin (banned) in the soil samples, which confirmed the long per-
sistence of these pesticides in the environment. These banned OCs were
also found in different agricultural soils from China (Zhu et al., 2014)
and other countries (Chaiyarat et al., 2015). The concentrations of OCs
in the two soils (values above the LODs) ranged from 7.4 μg/kg to 88.6
μg/kg (persimmon soil) and 2.1 μg/kg to 285.1 μg/kg (jujube soil), respec-
tively. The OC levels were within the concentration range in soils recently
reported from south (Lu and Liu, 2015) and north China (Zhu et al., 2014).
Among the PYs, the most often found pesticide was fenpropathrin, with
detected concentrations of 33.3 μg/kg–400.1 μg/kg. In addition, the detec-
tion frequency for triadimefon was notably higher than that for
buprofezin, with the corresponding values being 28.3% (triadimefon)
and 15.2% (buprofezin). Among all the tested pesticide types, the order
for different pesticides detection in the soils was OCs (71.7%) N PYs
(60.9%) N FUs (45.7%) N OPs (8.7%).
3.3. The multiple residues in the fruits and their planted soils
The occurrence of multiple residues resulted from the mixtures of
different pesticides: residues resulting from soil uptake in cases in
which pesticides have high persistence in the soil and residues resulting
from spray drift from neighboring plots or cross-contamination during
the processing of the crops (Lozowicka, 2015). The samples containing
one, two and multiple residues are shown in Fig. 2. The occurrence of
multiple residues in persimmons (4 residues) was notably lower than
that in jujubes (8 residues). The ratios for no pesticides detected in
the two fruits were 63.6% (persimmon) and 29.2% (jujube), respective-
ly. The multiple residues in the other persimmon samples were not
above 4 residues, including 13.6% (1 residue), 13.6% (3 residues) and
9.1% (4 residues). The most often found pesticide in persimmon samples
was fenpropathrin, with a detection frequency of 30.0%. The total con-
centrations of the multiple residues in the persimmon samples fell
within the range of 15.4 μg/kg–528.5 μg/kg. However, 8 residues were
found in 4.2% jujube samples, and the other multiple residues in jujubes
ranged from 8.3% to 25.0%. The detection frequency for the most often
found pesticide was 22.7% (cypermethrin in jujubes). The total concen-
trations of the multiple residues in the jujube samples fell within the
range of 9.1 μg/kg–2945.0 μg/kg. The reason for the highest detection
of fenpropathrin and cypermethrin in the two fruits was the wide appli-
cation of the two PYs in the sampling sites, which coincided with our in-
vestigation of the pesticide usage situation (details seen in Table 1).
Interestingly, the two PYs were not the main pesticides whose residues
exceeded the MRLs. In the tested fruits, the residues exceeding the MRLs
in China were 4.5% (persimmon) and 25.0% (jujube). In the positive
samples, although there was only one pesticide exceeding the MRLs,
the pesticide type was various. Four PYs, including bifenthrin,
cyhalothrin, fenvalerate and deltamethrin were found in the positive ju-
jube samples. Quintozine was the only pesticide found in the positive
 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628 625

Table 3 the excessive use of some chemicals, especially to diminish the use of
The concentration ranges of pesticide residues in the planted soils (μg/kg). PYs.
Group Pesticide Persimmon soil Jujube soil LOD Conversely, the multiple residues in the tested soils were notably
Dichlorvos n.d. n.d. 5
higher than those in the fruits. The multiple residues in the soils were
Methamidophos n.d. n.d. 5 even up to 14 residues for persimmon soils and 13 residues for jujube
Acephate n.d. n.d. 5 soils, respectively. The ratios for no pesticide detected in the soil were
Phorate n.d. n.d. 5 31.8% (persimmon soil) and 20.8% (jujube soil). The highest detection
Omethoate n.d. n.d. 5
frequency for multiple residues was 18.2% for both of 10 and 11 residues
Dimethoate n.d.–6.3 n.d. 5
Chlorpyrifos n.d.–25.5 n.d.–8.8 5 in the persimmon soils, in which the most often found pesticide type
Parathion-methyl n.d. n.d. 5 was OCs and HCH was the most often found pesticide (10.9%). More-
Fenthion n.d. n.d. 5 over, 11 and 10 residues ranked as the top two highest detection fre-
Fenitrothion n.d. n.d. 5 quencies in the jujube soils, with corresponding values of 15.2% and
Parathion n.d. n.d. 5
Isocarbophos n.d. n.d. 5
13.0%. DDT was the most often found pesticide in the jujube soils,
Phosmet n.d. n.d. 5 with a detection frequency of 12.4%.
Monocrotophos n.d. n.d. 5
G1 Triazophos n.d. n.d. 5 3.4. The relationship between fruits and their planted soils
p,p-DDE n.d.–22.2 n.d.–74.1 1
p,p-DDD n.d.–5.9 n.d.–3.8 1
p,p-DDT n.d.–12.3 n.d.–75.8 1 Environmental pollution and food safety are two of the most impor-
o, p-DDT n.d.–38.5 n.d.–152.6 1 tant issues of our time. Soil pollution, in particular, has historically im-
α-HCH n.d.–1.0 n.d.–1.0 1 pacted food safety, representing an important threat to human health.
β-HCH n.d.–8.9 n.d.–6.6 1 Some works have demonstrated that plants could uptake pesticides
γ-HCH n.d.–7.4 n.d.–1.0 1
from their planted soils (Fantke et al., 2013), especially OCs (Florence
δ-HCH n.d.–12.4 n.d.–40.1 1
α-Endosulfan n.d.–3.5 n.d.–5.1 1 et al., 2015). Concentrations of DDT, DDE and Cu in lettuce and radishes
β-Endosulfan n.d.–5.6 n.d.–14.8 1 increased with increasing soil concentrations, and there was a signifi-
Quintozene n.d.–1.1 n.d.–3.6 1 cant linear correlation (p b 0.001) between the mean soil and mean
Aldrin n.d.–1.0 n.d.–2.5 1
plant tissue concentrations for the contaminants (Gaw et al., 2008).
G2 Dieldrin n.d.–19.4 n.d.–2.7 1
G3 Bifenthrin n.d.–7.1 n.d.–18.3 2 The uptake for OCs differed among the three matrices (soil, moss and
Fenpropathrin n.d.–400.1 n.d.–353.9 2 tree-bark), and significant correlations were found between bark and
Cyhalothrin n.d.–7.3 n.d.–16.0 2 moss concentrations for most α-HCH and p, p-DDD (p b 0.01) (Tarcau
Cypermethrin n.d.–44.7 n.d.–35.5 2 et al., 2013). However, in this work, no significant correlation
Fenvalerate n.d.–15.9 n.d.–2.5 2
(p N 0.01) between the concentrations of soil/fruit for the tested pesti-
Deltamethrin n.d.–42.8 n.d.–46.9 2
G4 Triadimefon n.d.–15.7 n.d.–94.5 1 cides was found (even for OCs). The previous linear correlations be-
Buprofezin n.d.–18.6 n.d.–8.8 1 tween plant and soil were based on various specific data from plant/
n.d. = not detected, which means that the pesticide residues were below LOD. soil samples, in which the soil had a relatively high level of contami-
G1: organophosphates (OPs); G2: organochlorines (OCs); G3: pyrethroids (PYs); G4: fun- nants. However, in this work, the pesticide levels in soil were relatively
gicides (FUs). low (even below the LODs) and most of the pesticides could not be de-
tected in fruits (below the LODs), which made it difficult to establish
any model (linear or non-linear model) even parameters like environ-
persimmon sample. For better production and esthetic value, farmers mental conditions and soil type (Florence et al., 2015) were taken into
use a large amount of pesticide during the entire period of growth of ag- account. In the present study, in one hand, for banned pesticides, even
ricultural foods, and sometimes farmers ignore the recommended inter- if the uptake effect happened, the detected levels were relatively low
val period between harvest and last spray (Wang et al., 2013), which which made the corresponding pesticide concentrations in fruits were
might explain the differences between pesticide types regarding high below the LODs; in the other hand, for other pesticides, the residues de-
detection and exceeding MRLs. It is important to note that 31.8% tected in the fruits were mainly from the pesticide application, which
(persimmon) and 62.5% (jujube) of the samples exceeded the strict had little relationship to the uptake effect from soil.
EU MRLs, which might influence the export of the two fruits to the EU Although there were no significant correlations between the con-
market. The results pointed to the need for urgent action to control centrations, the detected pesticide types and frequencies in persim-
mon/jujube samples and soils had certain correlations (Fig. 3). There
were 7 and 11 pesticides detected in persimmon and jujube samples,
and the corresponding detected pesticides in their soils were 16 and
15, respectively. Although more pesticide types were found in the
soils than those in the fruits, all the detected pesticides in persim-
mons/jujubes (except for dimethoate, which was only detected in one
jujube sample) were also found in their planted soils. For PYs, when
more pesticide residues were found in the fruits, the probability for res-
idues found in their planted soils was high. For example, when
fenpropathrin was found in a persimmon sample at 19.9 μg/kg, the cor-
responding residue in the soil sample was below the LOD, but when the
residues in persimmon samples increased to 32.3 μg/kg and 222.4 μg/kg,
the residues in soils were 77.0 μg/kg and 91.2 μg/kg, respectively. The
concentrations of PYs in the soils were increased with increasing
concentrations of the fruits, but no linear correlation was found (p N
0.01). Moreover, the detection frequencies for the tested pesticides
were higher in soils than those in fruits (p b 0.05). The detection fre-
quencies for the six pesticides found in fruits, including quintozine, al-
Fig. 1. Patterns of DDTs and HCHs in the soils from the sampling sites. drin, fenpropathrin, cyhalothrin, cypermethrin and cypermethrin,
626 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628

Fig. 2. The multiple residues of tested pesticides in the fruits and their planted soils.

ranged from 4.2% to 41.7%. The corresponding values found in their been banned, but the high persistence of OCs in soils led to the highest
planted soils ranged from 9.1% to 58.3%. Moreover, the frequency distri- detection frequencies (12.5%–75.0%) among the tested pesticides. Most
bution of the various pesticide types presented the different historical of the tested OPs have also been banned; however, the relatively lowest
usages and current situation of pesticide application. OCs have long detection frequencies (b9.1%) for OPs occurred due to the non-

Fig. 3. The detection frequencies of different pesticides in the fruits and their planted soils.
 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628 627

persistence ability. Obviously, the relatively high detection frequencies
(18.2%–54.5%) of PYs and FUs in soils further confirmed that these pes-
ticides are currently the ones mainly applied (seen in Table 1), which
could also explain why these pesticides were detected in the fruits
with high detection frequencies (4.2%–41.7%).
3.5. Health risk assessment for the detected residues in persimmons and
jujubes
The human body is often the final accumulator of pollutants, which
can lead to health problems. As food consumption is the primary pathway
for human exposure to environmental contaminants, public demand for
food safety has increased. For risk assessment of a consumer's exposure
to pesticide residues in persimmon and jujube samples, the estimated
daily intakes, expressed as percentages of the ARfD and ADI values for
the tested pesticides, were derived from JMPR (Joint FAO/WHO Meeting
on Pesticide Residues) evaluations (http://apps.who.int/pesticide-
residues-jmpr-database). The dietary exposure to pesticides
(mg/kg/bw/day) was calculated based on consumption data and individ-
ual body weights, as well as residue monitoring data (the highest residue
and mean residue). The results are shown in Table 4. For short-term risk
assessment, most of the ESTI values were much less than the ARfD values
submitted by JMPR. Except for cyhalothrin, the other aHIs were below
10%, which meant that there was a negligible short-term or acute risk cor-
responding to exposure to the tested pesticides via consumption of the
two fruits. Interestingly, the aHI from fenvalerate (with the highest resi-
due of 2945 μg/kg) was 9.82%, which resulted from the relatively low tox-
icity (ARfD) of the pesticide. It was not surprising to find the high aHI of
cyhalothrin (19.43%), which had a relatively high detection frequency in
the fruits (10.9%), with the detected residues of 18.0 μg/kg–583.0 μg/kg.
Moreover, in the long-term risk assessment, most of the risk indexes
(HQs) were notably lower than the aHIs, which indicated that the chronic
risk from pesticide exposure via persimmon/jujube consumption should
be ignored. However, for aldrin and dieldrin, the HQ value for the two
pesticides was 14.13%, which meant that the risk should be considered.
In an investigation of pesticide residues in fruits and vegetables from
Pakistan, higher hazard risk index values were calculated for dieldrin,
methamidophos, o, p-DDT, diazinon and p, p-DDT in apples, mangos, ba-
nanas, melons, potatos and onions (Syed et al., 2014). In general, com-
pared with other reports focused on vegetables (Arias et al., 2014; Shen
et al., 2013) and fruits (Syed et al., 2014), most of the health risks from
pesticide residues in persimmons/jujubes of this work were relatively
small. The consumption quantity (for risk assessment) from this work
was equal or greater than others from the above literature, which showed
that the risk difference was due to a lesser contamination from this work.
The cumulative risks (cHI) for the tested pesticides were 10.90% (OPs),
16.09% (OCs), 5.95% (PYs) and 0.70% (FUs). The total cHI was 33.64%. Ob-
viously, the cumulative risk could be significantly reduced if the use of
OCs and OPs could be gradually diminished (even banned). Nevertheless,
for the already banned pesticides, the usage history and residue back-
ground in the soil should be considered during the site selection process
for fruit plantations. Moreover, it is important to note that the short-
term risks of fenpropathrin, fenvalerate and cyhalothrin ranged between
7%–20%, which indicated the probability of acute risk from these PYs.
Their residues exceeding the China/EU MRLs were 4.7%/6.5% for
cyhalothrin, 2.2%/21.7% for fenvalerate and 0%/26.1% for fenpropathrin,
respectively. A conclusion could be made that the use frequency of the
three PYs should be reduced or that they should be used in rotation

Table 4
The short-term and long-term risks due to average daily intake of pesticides through persimmon/jujube consumption in China.

Pesticide Short-term risk Long-term risk Use suggestion

ESTI ARfD aHI EDI ADI HQ

(%) (%)

Dichlorvos 1.87E−-04 0.1 0.19 1.67E−05 0.004 0.42 D

Methamidophos 7.92E−05 0.01 0.79 1.67E−05 0.004 0.42 B
Acephate 1.15E−04 0.1 0.11 1.67E−05 0.03 0.06 D
Phorate 6.37E−05 0.003 2.12 1.67E−05 0.0007 2.38 B
Omethoate 5.51E−04 / / 1.67E−05 / / D
Dimethoate 5.20E−04 0.02 2.60 2.73E−05 0.002 1.37 B
Chlorpyrifos 1.40E−04 0.1 0.14 1.67E−05 0.01 0.17 D
Parathion-methyl 1.74E−04 0.03 0.58 1.67E−05 0.003 0.56 B
Fenthion 1.24E−04 0.01 1.24 1.67E−05 0.007 0.24 D
Fenitrothion 1.17E−04 0.04 0.29 1.67E−05 0.006 0.28 D
Parathion 7.77E−05 0.01 0.78 1.67E−05 0.004 0.42 B
Isocarbophos 9.72E−05 / / 1.67E−05 / / D
Phosmet 1.15E−04 0.2 0.06 1.67E−05 0.01 0.17 D
Monocrotophos 1.30E−04 0.002 6.49 1.67E−05 0.0006 2.78 B
Triazophos 5.86E−05 0.001 5.86 1.67E−05 0.001 1.67 D
DDT 2.40E−04 0.01 2.40 5.26E−05 / / B
HCH(for lindane) 1.03E−04 0.06 0.17 6.67E−06 0.005 0.13 B
Endosulfan 1.09E−04 0.02 0.55 1.09E−04 0.006 1.82 D
Quintozene 2.10E−04 / / 7.60E−06 / / D
Aldrin and Dieldrin 2.81E−04 / / 1.41E−05 0.0001 14.13 B
Bifenthrin 3.96E−04 0.01 3.96 2.06E−05 0.01 0.21 U
Fenpropathrin 2.15E−03 0.03 7.16 1.98E−04 0.03 0.66 R
Cyhalothrin 3.89E−03 0.02 19.43 1.41E−04 0.02 0.71 R
Cypermethrin 1.66E−03 0.04 4.16 2.99E−04 0.02 1.50 U
Fenvalerate 1.96E−02 0.2 9.82 5.28E−04 0.02 2.64 R
Deltamethrin 1.00E−03 0.05 2.00 2.39E−05 0.01 0.24 U
Triadimefon 6.80E−05 0.08 0.09 1.93E−05 0.03 0.06 U
Buprofezin 4.63E−04 0.5 0.09 5.70E−05 0.009 0.63 U

Note: ARfD (mg/kg/bw/day) and ADI (mg/kg/bw/day) were adopted from the JMPR database. The symbol of “/” represents that there was no authorized value for ARfD/ADI and the cor-
responding risk index could not be computed. The persimmon/jujube consumption value is based on the recommended dietary intake per day for fruits of 400 g/day (data from Chinese
Dietary Guide (Nutrition, 2011)).
When the detected residues in the samples were below the LOD, data were treated with LOD/2.
Use suggestion. B: already banned use; D: gradually diminish use until banned; U: use and consider the pre-harvest interval; R: reduce the use frequency or rotate use with different
pesticides.
628 Y. Liu et al. / Science of the Total Environment 542 (2016) 620–628
with different pesticides to lower the acute risk. Regardless, the other PYs
and the two FUs could be normally used, but the pre-harvest interval
should be considered.
4. Conclusions
This study indicated that the two fruits (persimmon and jujube)
contained pesticide residues in 36.4% of persimmons and 70.8% of jujubes
collected. There were 7 pesticides (2 OCs, 4 PYs, 1 FU) found in persim-
mon samples and 11 pesticides (1 OP, 3 OCs, 6 PYs, 1 FU) in jujube sam-
ples. The most frequently detected pesticides were fenpropathrin in
persimmons and cypermethrin in jujubes. In the tested fruits, the residues
exceeding the MRLs in China were 4.5% (persimmon) and 25.0% (jujube),
and the pesticides included bifenthrin, cyhalothrin, fenvalerate, delta-
methrin and quintozine. Moreover, the residues in the tested soils were
notably higher than those in the fruits. The ratios for pesticides detected
in the two soils were 68.2% (persimmon soil) and 79.2% (jujube soil).
The most frequently detected pesticides were HCH in persimmon soil
and DDT in jujube soil. Although there was no significant correlation
(p N 0.01) between the concentrations of soil/fruit for the tested pesti-
cides, the detected pesticide types and frequencies in persimmon/jujube
samples and soils had a certain correlation. OCs and PYs had the highest
detection frequencies in the soils and fruits, respectively, due to long per-
sistence (OCs) and wide used (PYs). There was a negligible short-term or
acute risk with the exposure to the monitored pesticides via persimmon/
jujube consumption. However, the chronic risk for aldrin and dieldrin
should be considered. From the public health point of view, the observed
levels of pesticide residues in persimmons and jujubes do not pose a seri-
ous health risk to the consumers, but the pesticide contamination in ju-
jubes might give cause for concern. Above all, the consumption of OPs
and OCs should be gradually reduced until completely banned, and PYs
and FUs should be applied in rotation or reduced in usage frequency. Fur-
thermore, the importance of pre-harvest interval should be considered.
Acknowledgments
We gratefully acknowledge the financial support from the Special
Fund for Forestry Scientific Research in the Public Interest
(201304705). The authors state that there are no conflicts of interest.
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