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Occurrence, Distribution and Source Apportionment of Polychlorinated Naphthalenes (Pcns) in Sediments and Soils from the Liaohe River Basin, China*

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Occurrence, Distribution and Source Apportionment of Polychlorinated Naphthalenes (Pcns) in Sediments and Soils from the Liaohe River Basin, China* Environmental Pollution 211 (2016) 226e232 Contents lists available at ScienceDirect Environmental Pollution journal homepage: www.elsevier.com/locate/envpol Occurrence, distribution and source apportionment of polychlorinated naphthalenes (PCNs) in sediments and soils from the Liaohe River Basin, China* Fang Li a, b, Jing Jin a, Yuan Gao a, Ningbo Geng a, b, Dongqin Tan a, b, Haijun Zhang a, * Yuwen Ni a, Jiping Chen a, a Key Laboratory of Separation Science for Analytical Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, No. 457 Zhongshan Road, Dalian 116023, China b University of Chinese Academy of Sciences, Beijing 100049, China article info abstract Article history: The occurrence and spatial distribution of polychlorinated naphthalenes (PCNs) were investigated in Received 23 July 2015 sediments, upland and paddy soils from the Liaohe River Basin. Concentrations of SPCNs were in the À À Received in revised form range of 0.33e12.49 ng g 1 dry weight (dw) in sediments and 0.61e6.60 ng g 1 dw in soils, respectively. 28 September 2015 Tri-CNs and tetra-CNs were the dominating homologues. An increasing trend of PCNs contamination was Accepted 29 September 2015 found in sediments with the rivers flowing through industrial areas and cities. Soils collected near cities Available online 14 January 2016 exhibited higher abundance of PCNs than that of rural areas. The distribution of PCNs was related to the local industrial activities, rather than total organic carbon. Positive matrix factorization (PMF) was used Keywords: Polychlorinated naphthalenes for the source apportionment of PCNs in sediments and paddy soils. The result of PMF indicated that Occurrence PCNs in sediments and paddy soils were mainly from the industrial processes, with additional contri- Distributions butions from the historical use of Halowax 1014 and atmospheric deposition. Source apportionment © 2015 Elsevier Ltd. All rights reserved. 1. Introduction been ubiquitously detected in numerous environmental and bio- logical samples (Bidleman et al., 2010a). The occurrence of PCNs in Polychlorinated naphthalenes (PCNs), a family of chlorinated sediments and soils was in the low to sub-ppb concentrations polycyclic aromatic hydrocarbons, consist of 75 possible congeners. (Castells et al., 2008; Helm et al., 2008a; Ishaq et al., 2009; Meijer They were commercially produced and mainly used in the electrical et al., 2001b; Schuhmacher et al., 2004). Currently, only limited industry with ideal chemical properties and thermal stability in the studies have focused on PCNs contaminant in China (Pan et al., 20th century (Falandysz, 1998). It has been identified that some 2011; Wang et al., 2012; Xu et al., 2015). The Liaohe River is one congeners can induce dioxin-like toxicity via binding to the aryl of the most heavily polluted rivers in China, and runs through many hydrocarbon receptor in vivo (Domingo, 2004). Due to their po- large industrial areas of Liaoning Province. It consists of the Hun tential properties of persistent organic pollutants (POPs) and River, Taizi River and Daliao River. The Hun River converges with adverse effects on living organisms including humans, PCNs have the Taizi River and flows into the Daliao River before entering into been listed in Annexes A and C of the Stockholm Convention on the Bo Sea. The Liaohe River serves as an important resource for POPs in May 2015 (Stockholm Convention). drinking water, aquaculture and industrial use. Moreover, the Sediments and soils hold the bulk of contemporary POPs car- Liaohe River Basin is also an important agricultural area, and rice is rying aquatic and terrestrial environmental burden. Thus, it is the major agricultural crop. There are more than one million acres essential to monitor POPs in sediments and soils which were of paddy fields irrigated with river water. In 2011, our research approved as secondary pollution sources. As reported, PCNs have group investigated the levels of PCNs in sediments from the Daliao À River Estuary with the range of 0.033e0.284 ng g 1 dw, and it was found that organic matter and molecular properties could influence * This paper has been recommended for acceptance by Jay Gan. the partition behavior between sediment and water phase (Zhao * Corresponding author. et al., 2011). However, further detailed studies are needed to E-mail address: [email protected] (J. Chen). http://dx.doi.org/10.1016/j.envpol.2015.09.055 0269-7491/© 2015 Elsevier Ltd. All rights reserved. F. Li et al. / Environmental Pollution 211 (2016) 226e232 227 13 investigate the PCNs pollution in this basin for environmental solutions (2.0 ng, C10eCN 27, 42, 52, 67, 73 and 75) were added to assessment. subsamples as the surrogate standard to monitor the analytical Although their production was prohibited in most countries in recovery efficiency. Ten gram subsamples were soxhlet-extracted 1980s, PCNs can also be released into the environments via unin- with n-hexane/acetone (1:1, v/v) for 16 h with copper granules tentionally emissions from the industrial thermal processes and (2.0 g) to remove the sulfur, and the extract was concentrated to other chlorination processes (Liu et al., 2014). Several approaches approximately 1 mL with rotary evaporator. Then gel permeation have been used to identify sources of PCNs in the environmental chromatography (GPC) with SX-3 Bio-Beads column was used to matrices. Ratios or fractions of several indicator congeners of PCNs remove lipid and other high molecular weight interferences using À such as CN 36/45, 42, 54, 53/55, 66/67, 71/72 have been widely used dichloromethane as a mobile phase at the flow rate of 5 mL min 1. to assess the contribution of industrial thermal processes (Liu et al., The extracts were passed through an open silica column packed 2014, Liu et al., 2012). However, overlaps of different industrial with 5.0 g 5% deactivated silica gels (activated at 650 C for 5 h and thermal sources limit its use in source identification of PCNs. Prin- then deactivated with 5% (w/w) Milli-Q water). PCNs were eluted cipal component analysis (PCA) has also been used to examine the with 80 mL of n-hexane, then the fraction was reduced in volume indicator congeners of PCNs based on the relationship between the and further cleaned up on an alumina column (from bottom to top: individual congener profiles of various possible sources (Bidleman 2.0 g anhydrous sodium sulfate, 10.25 g alumina, 2.0 g anhydrous et al., 2010b; Liu et al., 2014). Nevertheless, it is difficult to assess sodium sulfate). The eluent was discarded with 40 mL of n-hexane, the relative importance of individual sources. Currently, the chemical then PCNs were eluted with 120 mL of 5% dichloromethane in n- mass balance (CMB) and positive matrix factorization (PMF) are two hexane. Finally, the final eluent was concentrated and exchanged of the widely-used multivariate receptor modeling approaches for into 200 mL of nonane containing d7-CN 2 (2.0 ng) for instrumental the source apportionment of pollutants in the environments (Seike analysis. PCNs were analyzed by a gas chromatography-triple et al., 2007; Watson et al., 2001). The main shortcoming of the quadrupole mass spectrometer (GCeMS/MS, ThermoFisher Scien- CMB model is that it requires information of all sources and their tific) with electron impact source (Li et al., 2014). Details on the profiles before beginning the analysis. Whereas PMF model can operation parameters of chromatography and MS are presented in reconstruct the profile of potential sources through decomposing the Table S2 of the SI. sample data matrix consisting of sample concentration and uncer- tainty into factor profiles and factor contributions. Then the potential 2.3. Quality assurance and quality control emission sources would be identified based on fingerprints or composition of sources. Hitherto, few studies have applied the PMF An internal standard isotope-dilution method was employed for model for the source apportionment of polychlorinated dibenzo-p- the quantification of PCNs in the current study. It was assumed that dioxins, polychlorinated dibenzofurans (PCDD/Fs) (Sundqvist et al., the response of individual congeners of each homologue group was 2010), polychlorinated biphenyls (PCBs) (Praipipat et al., 2013)in equal to that of the 13C-labled congeners with the same degree of sediments. However, the PMF model has not been mentioned for the chlorination except for congeners of tri-CNs. For tri-CNs congeners, 13 source apportionment of PCNs in environmental matrices. the response of C10eCN 42 was used. The quantification of PCNs The objective of the present study was to investigate the total was performed by using a relative response factor (native to concentrations (SPCNs, tri-to octa-CNs) and spatial distribution of labeled) of the labeled congener at the same level of chlorination PCNs in sediments and ambient upland and paddy soils from the and the similar retention time. The concentration of each homo- Liaohe River Basin. Then the PMF model was used to generate logue is equal to the sum of the concentration of all congeners in candidate source profiles and estimate their relative contribution to this homologue. The limits of detection (LODs) and limits of PCNs in sediments and paddy soils. It is hoped that the work will be quantification (LOQs) of PCNs congeners were governed by the S/N helpful for creating the inventories, understanding sources and ratio. LODs were defined as the minimum amount of PCNs conge- environmental fate and further developing treatment strategies for ners with three times S/N in a chromatogram, and LOQs were controlling PCNs contamination in China. determined as ten times of S/N in blank samples. The LOQs ranged À from 0.10 to 1.75 pg g 1 dw (dry weight) for individual congeners of 2. Material and methods PCNs (Table S2).
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