ORIGINAL ARTICLE

Polycyclic aromatic hydrocarbons in the sediments of XiangjiangRiver in south-central China: occurrence and sources

Lei Zhang • Yanwen Qin • Binghui Zheng •

Tian Lin • Yuanyuan Li

Received: 10 October 2011 / Accepted: 21 August 2012 / Published online: 6 February 2013

� Springer-Verlag 2013

Abstract The Xiangjiang River (XR), located in Hunan

province in south-central China, is the second largest tribu-

tary of the Yangtze River. The occurrence, and sources of the

polycyclic aromatic hydrocarbons (PAHs) in the 20 surface

sediment samples from XR were analyzed, and the biological

risks of the PAHs on the benthic organisms were assessed

using sediment quality guidelines. The results showed that

the occurrence level of the 16 USEPA priority PAHs in the

surface sediments ranged from 190 to 983 ng/g (dry weight)

with a mean concentration of 452 ± 215 ng/g. The concen-

tration of phenanthrene was the highest with a mean con-

centration of 104 ± 44 ng/g. The compositions and principal

components analysis indicated that the PAHs in the sediments

in XR were mainly from pyrogenic sources which could be

attributed to the open burning of rice straws and coal com-

bustion of the local industries in the XR basin. The PAH

contamination in the sediments was considered to be mod-

erate, and has posed a small adverse biological effect on the

benthic organisms.

Keywords PAHs � Source � Surface sediments �Xiangjiang River � China

Introduction

Polycyclic aromatic hydrocarbons (PAHs) are a large

group of persistent organic pollutants. They are highly

stable in the environment and are known to be carcinogens.

PAHs are the products of the incomplete combustion of

organic materials, or from the spillage of crude oils and

refined oil products (Lima et al. 2005). High emission of

PAHs is usually associated with highly industrialized and

urbanized activities which are mostly concentrated in the

coastal areas and inland cities along major rivers (Mai et al.

2003; Boonyatumanond et al. 2006; Yim et al. 2007).

China is facing serious PAH pollution problem due to the

drastic increased use of fossil fuels in the past 30 years (Xu

et al. 2005; Guo et al. 2006).

PAHs partitioning in aquatic conditions strongly favors

the particulate phase (e.g., sediments) (Mitra et al. 1999;

Mai et al. 2003) due to the low solubility and high octanol/

water partition coefficient (Kow) (Lipiatou and Albaiges

1994; Mai et al. 2003). Thus, the sediments are the long-

term reservoir for the PAHs.

The Xiangjiang River (XR) in Hunan province of south-

central China is the second largest tributary of the Yangtze

River (the largest river in Asia) in discharge. Its length is

856 km and the watershed is 94,600 km2. In the past

30 years, XR has been contaminated by local mining and

smelting industries (Zhou and Li 2003; Cai et al. 2010; Liu

et al. 2010). Moreover, Hunan province is a major center of

agriculture, and the open burning of rice straws in there is

regarded as a significant source of atmospheric pollution

(Streets et al. 2001; Zhang et al. 2007).

There were several papers on heavy metal pollution in

XR (Zhou and Li 2003; Cai et al. 2010; Liu et al. 2010;

Wang et al. 2011), but few on the occurrence and com-

positions of PAHs, and the assessment of biological risk of

L. Zhang � Y. Qin (&) � B. Zheng

State Environmental Protection Key Laboratory of Estuarine

and Coastal Environment, Chinese Research Academy

of Environmental Sciences, Beijing 100012, China

e-mail: qinyw@craes.org.cn

T. Lin

State Key Laboratory of Environmental Geochemistry,

Institute of Geochemistry, Chinese Academy of Sciences,

Guiyang 550002, China

Y. Li

Department of Environmental Science and Engineering,

Fudan University, Shanghai 200433, China

123

Environ Earth Sci (2013) 69:119–125

DOI 10.1007/s12665-012-1939-x

PAHs has been still untouched. The objectives of this study

are to examine these issues.

Materials and methods

Sampling

Sampling sites were evenly distributed in the middle and

lower reaches of the river with high population density and

intensive industrial activity. Twenty surface sediment

samples were collected using a grab sampler in April,

2010. The locations of sampling sites are shown in Fig. 1.

Each sampling site was chosen at position 3 m away from

the river bank and was restricted to depths of less than 1 m.

The top 3-cm sediment was carefully wrapped in aluminum

foil and stored at -20 �C until analysis.

Organic analysis

The PAH analysis procedure followed that described by Mai

et al. (2003) and Qin et al. (2011). Briefly, homogenized

samples were freeze-dried, ground and sifted through 80 mesh

sieves. About 5 g of the sample was spiked with a mixture of

recovery standards of five deuterated PAHs (naphthalene-d8,

acenaphthene-d10, phenanthrene-d10, chrysene-d12, and per-

ylene-d12). The samples were extracted with dichloromethane

in a Soxhlet extractor for 48 h, with activated copper added to

remove the sulfur in the samples. The extract was concentrated

and fractionated using a silica–alumina (1:1) column. PAHs

were eluted using 35 ml of hexane/dichloromethane (1:1). The

PAHs fraction was concentrated to 0.5 ml, and hexamethyl-

benzene was added as internal standard. The mixture was

further reduced to 0.2 ml and subjected to GC–MS analysis.

An Agilent 5975C mass spectrometer interfaced to Agilent

7890 gas chromatography was used to analyze the samples.

The GC was equipped with a DB-5MS capillary column

(30 m 9 0.25 mm i.d. 90.25 lm film thickness), with He as

carrier gas. The chromatographic conditions were as follows:

injector temperature, 290 �C; detector temperature, 300 �C;

temperature program: 60 �C (3 min), 60–290 �C at 3 �C/min,

held at 290 �C for 20 min. The PAHs quantified were as fol-

lows: naphthalene (Nap), acenaphthylene (Ac), acenaphthene

(Ace), fluorene (Fl), phenanthrene (Phe), methylphenanthrene

(MP, 5 isomers), anthracene (Ant), fluoranthene (Flu), pyrene

(Pyr), benz[a]anthracene (BaA), chrysene (Chr), benzo[b]flu-

oranthene (BbF), benzo[k]fluoranthene (BkF), benzo[a]pyrene

(BaP), indeno[1,2,3-cd]pyrene (IP), dibenz[a,h]anthracene

(DBA), and benzo[ghi]perylene (BghiP). Standard-spiked

matrix, duplicate samples and procedural blank were analyzed

for quality assurance and control. Recoveries of the PAHs in

the standard reference material (NIST 1941) ranged from 80 to

120 % of the certified values. Nominal detection limits for

individual PAH ranged from 0.2 to 2 ng/g (dry weight) for

10 g of sediment. PAH recoveries of standard-spiked matrix

ranged from 85 to 95 %, the relative precision of paired

duplicated samples was below 15 % (n = 4), and the targeted

compounds were not detected in procedural blank (n = 4).

Recovery was 76 ± 8 % for naphthalene-d8, 84 ± 11 % for

acenaphthene-d10, 92 ± 8 % for phenanthrene-d10, 93 ± 6 %

for chrysene-d12, and 97 ± 11 % for perylene-d12. PAH

concentrations were recovery corrected.

Fig. 1 Map of the sampling sites

120 Environ Earth Sci (2013) 69:119–125

123

Results and discussion

Occurrence of PAHs

The concentrations of the PAHs in the surface sediments

are given in Table 1. All concentrations were on dry basis.

The total concentrations of the 16 PAHs in the surface

sediments ranged from 190 to 983 ng/g with a mean of

452 ± 215 ng/g. As shown in Fig. 2, the Phe concentration

was the highest in the PAHs (mean 104 ± 44 ng/g), fol-

lowed by Flu and Pyr. These top three compounds com-

prised 50.8 % of the 16 PAHs measured. The PAHs can be

Table 1 Concentrations (ng/g) of 16 PAHs in the sediment samples from the Xiangjiang River

Sites Nap Ac Ace Fl Phe MP Ant Flu

HY2 6.4 1.9 7.4 33.3 59.1 38.8 8.3 43.0

HY5 9.9 3.6 8.4 39.5 59.1 28.3 10.5 35.1

HY6 7.7 2.4 9.9 53.3 90.3 39.1 9.6 36.4

HY8 8.0 4.1 8.4 39.9 75.7 44.0 11.1 54.9

HY9 6.8 1.7 6.6 31.0 52.9 28.2 5.1 24.4

HY19 36.4 6.2 76.1 107.9 197.7 161.2 28.2 134.0

HY24 4.3 1.4 4.5 25.4 49.1 22.2 6.5 23.1

HY25 5.2 2.2 6.4 38.0 84.6 39.9 11.2 54.8

HY29 10.2 4.2 9.1 50.0 106.9 86.0 13.7 65.6

HY30 7.3 1.5 7.1 37.4 75.9 42.9 9.6 37.2

HY33 20.6 2.3 8.0 45.0 83.0 85.0 10.7 49.7

HY34 8.7 3.7 9.9 57.1 113.0 73.9 14.9 66.5

HY36 8.3 3.0 8.7 44.0 91.5 66.0 12.8 46.1

HY37 6.6 2.3 6.4 40.5 83.3 56.3 11.3 46.6

HY41 7.3 4.9 9.0 46.4 111.8 45.9 18.3 85.2

XY1 13.6 7.0 16.9 85.1 138.1 113.3 28.3 115.8

QY1 12.2 5.3 23.4 81.9 158.5 155.3 31.1 127.7

QY2 12.9 5.0 18.2 63.5 155.1 123.4 28.5 126.2

QY3 10.4 3.7 15.1 61.0 128.2 88.4 18.8 86.9

QY4 9.1 3.1 11.9 45.1 108.7 60.2 16.6 102.2

Sites Pyr BaA Chr BbF BkF BaP IP DBA BghiP PAHs

HY2 36.5 21.6 13.0 15.9 4.2 8.5 4.9 1.2 4.8 270

HY5 29.6 16.4 11.9 14.0 4.0 7.3 4.6 1.1 4.0 258

HY6 29.9 13.0 13.1 15.1 3.4 6.0 4.7 1.1 4.3 300

HY8 47.3 34.0 24.3 32.7 8.7 17.8 11.0 2.5 9.6 390

HY9 20.1 9.4 9.0 11.3 2.7 3.7 3.6 0.7 3.1 192

HY19 109.1 70.6 64.9 68.0 15.1 27.3 18.8 5.2 17.9 983

HY24 18.3 16.6 11.0 13.0 3.2 5.3 3.9 1.3 3.1 190

HY25 44.9 28.4 17.0 21.5 5.7 11.0 7.2 1.8 6.2 346

HY29 62.4 28.1 25.6 28.1 6.6 13.5 9.1 2.4 12.8 448

HY30 30.6 15.0 12.3 11.2 2.5 3.6 1.8 0.7 1.9 255

HY33 41.7 26.5 22.4 25.9 5.8 11.5 7.5 2.0 7.6 370

HY34 58.2 30.5 28.0 33.5 8.0 15.7 11.4 2.6 10.5 472

HY36 44.0 24.1 21.2 26.0 6.2 11.4 8.3 1.9 8.1 365

HY37 41.3 22.9 20.3 24.0 5.6 10.9 7.7 1.9 7.4 339

HY41 69.4 35.8 23.3 28.3 7.2 13.9 9.3 2.1 8.3 480

XY1 96.4 43.9 43.5 40.6 14.6 21.0 19.7 2.9 18.8 706

QY1 103.3 63.3 45.5 55.6 14.0 28.8 16.9 4.3 15.6 787

QY2 104.1 70.7 4.9 60.4 16.0 31.5 19.7 4.9 17.4 739

QY3 71.3 47.6 34.9 42.1 10.6 20.9 13.4 3.5 11.7 580

QY4 76.1 53.9 36.4 48.0 12.4 21.6 14.5 3.7 12.4 575

Environ Earth Sci (2013) 69:119–125 121

123

divided into three groups based on the number of aromatic

rings: 2 ? 3 rings (91–452 ng/g, mean 195 ± 85 ng/g), 4

rings (62–378 ng/g, mean 182 ± 94 ng/g) and 5 ? 6 rings

(21–152 ng/g, mean 74 ± 41 ng/g) with the 2 ? 3 ring

(45.0 ± 6.0 %) and 4 ring (39.2 ± 3.8 %) members being

the dominant PAHs (Fig. 3).

The highest concentration of PAHs was found at site HY

19 (983 ng/g), which was significantly higher than other

sites in the upper reach of XR (190–480 ng/g, n = 15). The

PAHs at this site was from sewage outfall where the high

levels of heavy metals were also detected (Qin et al. 2011).

The upper reach of the river showed a mean PAHs con-

centration of 334 ± 94 ng/g.

The average PAH concentration in the lower reach of

XR was 677 ± 85 g/g (n = 5) which was much higher

than the upper reach except for HY19. XR discharges

directly into Dongtinghu Lake (the second largest fresh-

water lake in China) with many tributaries in the estuary.

This could make more PAHs be co-deposited with fine-

grained sediments due to the weak dynamic environment in

this area.

Compared to the other rivers in China and other coun-

tries (Table 2), the PAHs concentrations in the sediments

from XR were relatively lower than the other rivers such as

the Lower Pearl River, South China (Mai et al. 2002),

Lower Haihe River, North China (Jiang et al. 2007), the

upper reach of Yellow River, Northwest China (Xu et al.

2007), Gomti River, India (Tripathi et al. 2009), and the

urban stretch of Tiber River, Italy (Patrolecco et al. 2010),

while it was similar to those of the Qiantang River, East

China (Chen et al. 2007), the lower Yangtze River, China

(Hui et al. 2009) and Daliao River, North China (Guo et al.

2007), and it was higher than that in the lower Yellow

River (Huanghe) (Hui et al. 2009).

Composition and sources of PAHs

The composition distribution of the PAHs in the surface

sediment is shown in Figs. 2 and 3. The compositions and

the relative abundance of PAHs did not present a signifi-

cant variation. As shown in Fig. 3, the composition pattern

of PAHs was characterized by abundant 2 ? 3 rings PAHs,

followed by the 4 rings PAHs and 5 ? 6 rings PAHs. It

was found that PAHs in the sediments from urban river

system had a unique distribution dominated by 5 ? 6 rings

and 4 rings PAHs (Luo et al. 2006; Shen et al. 2009). In

general, the low molecular weight (LMW, with two or

three rings) parent PAHs originate mainly from petrogenic

sources and low-temperature pyrogenic sources, while

high-temperature pyrogenic procedures produce mainly

high molecular weight parent (HMW, with four or more

rings) PAHs (Mai et al. 2003). In this study, most of LMW/

HMW ratios were lower than 1, indicating that high-tem-

perature pyrogenic contribution should be significant in the

region.

The diagnostic ratios of the individual PAH can also be

used to identify the sources of the PAHs. MP/Phe measured

in combustion mixtures are generally \1, whereas

unburned fossil fuel PAH mixtures typically display a

range of 2–6 (Yunker et al. 2002; Mai et al. 2003). The

Phe/Ant ratio is high when petrogenic sources are

Fig. 2 Proportion of the individual PAHs in the total concentrations

of the 16 PAHs

Fig. 3 Compositions of 2 and 3, 4, 5 and 6 rings PAHs in the

sediment samples

122 Environ Earth Sci (2013) 69:119–125

123

dominant since Phe is more abundant than Ant in crude

oils, while the ratio is lower when pyrogenic sources are

dominant because Ant is more stable than Phe (Soclo et al.

2000). Phe/Ant [15 indicates petrogenic sources and Phe/

Ant\10 signals pyrogenic sources (Yunker et al. 2002). In

the present study, MP/Phe ratios in the sediments were in

range of 0.41–1.0 and Phe/Ant ratios were 4.8–10.6

(Fig. 4a). This suggests that the PAHs, especially Phe, in

the sediments in XR were derived from pyrogenic sources.

It is indicated that PAHs from pyrogenic source has a

Flu/(Flu ? Pyr) ratio of 0.4–0.5 for liquid fossil fuel

(automotive and crude oil) combustion while [0.5 is

characteristics of coal, grass or wood combustion (Yunker

et al. 2002). IP/(IP ? BghiP) ratio of 0.2–0.5 is possibly

liquid fossil fuel (automotive and crude oil) combustion,

while coal, grass and wood combustion would yield a ratio

[0.5 (Yunker et al. 2002; Mai et al. 2003). In this study,

Flu/(Flu ? Pyr) ratios were [0.5, implying that coal and

wood combustion could be the major contributors of the

pyrogenic PAHs in the sediments which is also supported

by [0.5 IP/(IP ? BghiP) ratios (Fig. 4b). Thus, it can be

concluded that pyrogenic sources from coal and wood

combustion would be the major sources of PAHs in XR.

Principal components analysis of PAHs

Principal components analysis (PCA), a multivariate ana-

lytical tool, was used to determine the distribution of the

samples and to study the relationship of the measured

parameters. Prior to analysis, the non-detectable values

were first replaced with concentration values of one half

the method detection limits (Zaghden et al. 2007; Hu et al.

2009). Overall, all PAH compounds in the sediments in XR

clustered mostly on the positive scale of the PC1 axis

which explains 84 % of the total variance (Fig. 5a). It was

further found that PC1 had significant correlations with

HMW PAHs including BkF, BaP, IP, DBA and BghiP

compared to LMW PAHs (Nap, AC and ACE). Thus, PC1

was mostly related to pyrogenic PAHs. Similarly, the score

plots in Fig. 5b indicate that the samples can be grouped

near the positive PC1 which explains 93 % of the total

variance, indicating a small variability of PAH composi-

tional patterns among the samples. Consequently, the PCA

Table 2 Concentration ranges and mean values of PAHs in sedi-

ments from different rivers in China and other countries

Location PAHs (ng/g) n References

Mean Range

Lower Pearl

River

2,047 ± 2,970 408–10,881 10 Mai et al.

(2002)

Lanzhou, upper

reach of Yellow

River

1414 464–2,621 14 Xu et al.

(2007)

Lower Yellow

River

90.7 10.8–252 15 Hui et al.

(2009)

Lower Yangtze

River

259 84.6–620 6 Hui et al.

(2009)

Lower Haihe

River

27,074 775–255,372 13 Jiang et al.

(2007)

Qiantang River 315 91–614 45 Chen et al.

(2007)

Daliaohe River 287 61–840 12 Guo et al.

(2007)

Xiangjiang River 452 ± 215 190–983 20 This study

Gomti River,

India

1,182 68–3153 16 Tripathi

et al.

(2009)

The urban stretch

of Tiber River,

Italya

215 ± 44 157–271 5 Patrolecco

et al.

(2010)

a the mean and range of the 6 PAHs(fluoranthene, benzo(b)fluo-

ranthene, benzo(k)fluoranthene, benzo(a)pyrene, benzo(g,h,i)per-

ylene, indeno(1,2,3-cd)pyrene)

Fig. 4 Cross plots for the

ratios of MP/Phe and Phe/Ant

(a) and Flu/(Flu ? Pyr) and IP/

(IP ? BghiP) (b) in the

sediment samples

Environ Earth Sci (2013) 69:119–125 123

123

results further suggest that the PAH contamination in XR is

essentially from the similar sources.

Potential biological risks

The potential ecological risks of the PAHs in the sediments

were assessed using sediment quality guidelines according

to Long et al. (1995), and the results are summarized in

Table 3. The effect range low (ERL) and effect range

median (ERM) have been used to assess aquatic sediment

quality with a ranking of low to high impact values (Long

et al. 1995). ERL represents the concentration below which

an adverse effect would rarely be observed. ERM repre-

sents the concentration above which adverse effects would

frequently occur. Table 3 shows that the maximum con-

centrations do not exceed their respective ERL values of

individual PAHs except Ace and Fl. The ERL for Ace was

exceeded at 20 % (n = 4) of the sites in the study area, and

for Fl, measured concentrations were higher than the ERL

value but lower than the ERM (Tables 1, 2). This indicates

that the PAHs in XR probably have posed a small adverse

biological effect on the benthic organisms.

Conclusions

The PAH compositions and diagnostic ratios indicate that

the PAHs in the sediments in XR were dominantly derived

from pyrogenic sources attributable to the open burning of

rice straws and coal combustion from local industries

within the XR basin. The PCA results show that there is no

obvious spatial variation of PAH sources along the river.

The assessment of the corresponding quality guidelines for

sediments indicates that the PAHs in the sediments in the

river probably have posed an adverse biological effect on

the benthic organisms although it is small.

Acknowledgments This work was supported by the major program

of the national water pollution control and management in China (No.

2009ZX07528-002). We wish to thank Dr. Zhao Y.M., Dr. Liao Y.H.,

Mr. Liu X., Mr. Jia N., Mr. Wang M.Y., and Miss Jia J. for the sample

collection.

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