Dioxin-like compounds in Australian sewage sludge--review and national survey

An Australian survey of dioxin-like compounds in sewage sludge was conducted in two parts (a) a national survey, and (b) a time-study. All sewage sludge samples analysed as part of these studies had low overall concentrations of dioxin-like compounds. Out of 37 samples, all except one, were within the reported concentration range of soil within the Australian environment. The mean concentration of dioxin-like compounds in the Australian sewage sludge survey of 2006 was found to be 5.6 (s.d. 4.5) ng WHO(05) TEQkg(-1) (n=14) and were within the range of 1.2-15.3 ng WHO(05) TEQ kg(-1). All the Australian sewage sludge samples cited in these studies were below the Victorian EPA "investigation limit" of 50 ng WHO(98) TEQ kg(-1), and well below the European proposed guidelines of 100 ng I-TEQ kg(-1). The burden of dioxin-like compounds in Australian sewage sludge is low and its land application as biosolids is not likely to pose a problem. A general positive relationship was found between population of the town producing the waste and both dioxin-like PCDD/Fs and dioxin-like PCBs. The one exception to this trend was sludge from a town that had a history of smelting and had a relatively high burden of dioxin-like compounds. Sludge from one rural WWTP also had a higher burden of dioxin-like compounds. The treatment plant services a geographically isolated town with a low population and no known emitters of dioxin-like compounds. However, this sample also had a relatively high burden of dioxin-like PCBs, which could be the source of the dioxin-like PCDD/Fs found in this sludge. The time study analyzing sludges from three WWTP from the same city between the years 2002 and 2006 found no apparent difference between WWTPs, but a statistically significant decline of 1.49 ng WHO(05) TEQ kg(-1) per year. Also, a comprehensive review of the scientific literature, presents typical levels and sources of dioxin-like compounds in international sewage sludges.     

Occurrence of organic contaminants in sewage sludges from eleven wastewater treatment plants, China

This study presents the occurrence of 43 semi-volatile organic compounds (SVOCs) listed as priority pollutants by both China and the United States Environmental Protection Agency, in sewage sludges collected from eleven wastewater treatment plants (WWTPs) of mainland and Hong Kong, China. Thirty-six SVOCs were detected by gas chromatography coupled with mass spectrometer (GC-MS) and at least 14 in each sample. The most abundant compounds were phthalic acid esters (PAEs) and polycyclic aromatic hydrocarbons (PAHs) with total concentrations ranging from 10 to 114mgkg(-1) dry weight (d.w.) (with a mean of 30mgkg(-1) d.w.) and from 1.4 to 33mgkg(-1)d.w. (with a mean of 16mgkg(-1) d.w.), respectively, followed by chlorobenzenes, nitroaromatics, haloethers and halogenated hydrocarbons which occurred generally at concentrations lower than 10mgkg(-1) d.w. Large variations were observed between the concentrations of individual compounds as well as their total concentrations in sludge samples from different WWTPs. The highest values of sum concentration of 16 PAHs and of 6 PAEs were found in sewage sludge from Beijing. The mean total concentration of each class of SVOCs in sewage sludge from mainland was remarkably higher than that from Hong Kong. The concentrations of di(2-ethylhexyl) phthalate in 91% sludge samples met the limit (100mgkg(-1)d.w.) proposed by the Europe Union for land application, whereas the PAH concentrations of 64% sludge samples exceeded the maximum permissible concentration (6.0mgkg(-1)d.w.). The occurrence of SVOCs in this study are compared with other studies and their sources are discussed.     

Hydroxylated polybrominated diphenyl ethers (OH-PBDEs) in biosolids from municipal wastewater treatment plants in China

Hydroxylated polybrominated diphenyl ethers (OH-PBDEs) along with methoxylated polybrominated diphenyl ethers (MeO-PBDEs) have been frequently identified as natural compounds in marine environment and also assumed as metabolites of PBDEs. In the present study, nine OH-PBDE, nine MeO-PBDE and 10 PBDE congeners were studied in the sewage sludge collected from 36 municipal wastewater treatment plants (WWTPs) in 27 cities of China. The results suggest that OH-PBDEs and PBDEs are ubiquitous in sewage sludge in China, however, methoxylated PBDEs were not detectable. Composition profiles of detected OH-PBDE congeners were different depending on the sampling location. ΣOH-PBDEs in WWTPs sludge ranged from 0.04 to 2.24 ng g^?1 dry weight (mean: 0.35 ng g^?1 dry weight). The total amount of the two most prominent congeners (6-OH-BDE-47 + 2′-OH-BDE-68) accounted for about 53.3–100% of the sum of all six identified congeners. A significant linear relationship was found between 6-OH-BDE-47 and 2′-OH-BDE-68. A distinct geographical distribution of ΣOH-PBDEs was observed with greater concentrations of OH-PBDEs at coastal areas than inland regions in China.     

A comparison of TEQ contributions from PCDDs,PCDFs and dioxin-like PCBs in sewage sludges from Catalonia,Spain

Eight sewage sludges from rural, urban and industrial wastewater treatment plants (WWTPs) in Catalonia (Spain) were analysed for polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and biphenyls (PCBs) to determine the present levels of contamination. A method based on an automated cleanup system followed by an isotope-dilution high-resolution mass spectrometric analysis was employed. Total toxicity equivalent (WHO-TEQ) values were calculated using the toxicity equivalent factors (WHO-TEFs) proposed by WHO for dioxin-like PCBs, PCDDs and PCDFs. The WHO-TEQ(PCDD/F) values for these samples ranged from 4.9 to 20.8 pg/g dry weight (d.w.), with a mean value of 9.3 pg/g d.w., whereas WHO-TEQ(PCB) levels ranged between 1.9 and 6.6 pg/g d.w., with a mean value of 4.2 pg/g d.w. The WHO-TEQ(PCB) contribution varied from 13% to 50%, suggesting that PCB contribution on the toxicity of the samples must be taken into account. Moreover, these contemporary PCDD, PCDF and PCB concentrations were compared with previous data obtained from sewage sludge samples collected during the 80s. Our findings show that contemporary PCDD, PCDF and PCB levels have declined since the 80s.     

Polybrominated diphenyl ethers and organochlorine pesticides in sewage sludge of wastewater treatment plants in China

The concentrations of chemicals in sewage sludge from wastewater treatment plants (WWTPs) may relate to their levels of use and environmental pollution in the region. In this work, sludge samples were collected from 31 WWTPs in 26 cities in China and analyzed for polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs). The concentrations of SigmaPBDE (sum of congeners 17, 28, 47, 66, 71, 85, 99, 100, 138, 153, 154, and 183) ranged from 6.2 to 57ng/g (dw). The concentration of decabromodiphenyl ether (BDE-209) ranged from below limit of detection (LOD) to 1109ng/g (dw) (with a median of 27ng/g (dw)), and averaged 55% (median 69%) of the total PBDEs. These levels are about 10-100 times lower than those found in Europe and North America. PBDE levels in sludge were not found to depend on the location and capacity of the WWTPs. Concentrations of hexachlorocyclohexanes (HCHs), dichlorodiphenyltrichloroethane (DDTs) and its major degradation products, and hexachlorobenzene (HCB) ranged from below detection limit to 167ng/g (dw), 11 to 1065ng/g (dw), and 7.5 to 319ng/g (dw), respectively. The major DDT degradation products were p,p'-DDE and p,p'-DDD. The major hexachlorocyclohexane (HCH) isomer in sludge is beta-HCH, reflecting its higher affinity to solids and resistance to degradation than other isomers.     

Effect of sewage sludges contaminated with polybrominated diphenylethers on agricultural soils

The fate of polybrominated diphenyl ethers (PBDEs) in sewage sludge after agricultural application was analysed. This study was based on the analysis of sewage sludge and sludge amended soil samples collected during 2005. PBDE concentrations in sewage sludge ranged from 197 to 1185ng/g dry weight (dw), being deca-BDE-209 the predominant congener. PBDE levels in soils ranged between 21 and 690ng/g dw, being BDE-209 also the predominant congener in all soil samples. Sewage-sludge amendment at the research stations increased concentrations of all BDE congeners 1.2- to 45-fold, with the highest increases for BDE-209. Results obtained evidenced the cumulative effect of the sludge application rates. Moreover, high levels found at soils four years after the last sludge application indicate persistence of PBDEs in soils, including deca-BDE-209.     

Distribution and levels of brominated flame retardants in sewage sludge

One hundred and sixteen sewage sludge samples from 22 municipal wastewater treatment plants in Sweden were analysed for brominated flame retardants. Polybrominated diphenyl ethers (PBDEs) were in the range n.d.-450 ng/g wet weight, tetrabromobisphenol A (TBBPA) varied between n.d. and 220 ng/g wet weight, 2,4,6-tribromophenol was in the range n.d.-0.9 ng/g wet weight and polybrominated biphenyls were not detected (except for a possible analytical interference). There was a significant variation in the samples among plants. Influence from industries and other local sources can therefore be assumed. The correlation pattern indicated contribution from three different types of technical products; composed of either low-brominated PBDEs, decaBDE or TBBPA.     

PCDDs and PCDFs in sewage sludges from two wastewater treatment plants in Beijing, China

The levels of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) were analyzed by an isotope-dilution high-resolution mass spectrometric in 16 sewage sludges, sampled from 2004 to 2009, from two municipal wastewater treatment plants (WWTPs) in Beijing. Total toxicity equivalent (TEQ) values were evaluated using the toxicity equivalent factors proposed by International for PCDD/Fs. The I-TEQs for these sewage sludges were from 0.97 to 15.0 pg g⁻¹ dry weight (dw) with a mean value 4.43 pg g⁻¹ dw, indicating that all I-TEQs were below Chinese legislation limit value regulated for agricultural use in soils.The results from limited samples (16 samples) showed that the levels of PCDD/Fs might be correlated with the sludge age. Meanwhile, the temporal trends of PCD/Fs suggested that the I-TEQs may correlate with rainfall in the present study.     

Congener-specific accumulation and environmental risk assessment of polybrominated diphenyl ethers in diverse Korean sewage sludge types

Industrial, domestic wastewater, and livestock sludge samples were collected from 23 wastewater treatment plants in Korea and analyzed for polybrominated diphenyl ethers (PBDEs). The concentrations of Σ₁₉PBDE ranged from 4.01 to 10,400 ng/g dry weight. The average Σ₁₉PBDE concentrations in industrial, domestic wastewater, and livestock sludge were 1,560?±?3,610, 402?±?148, and 27.6?±?50.4 ng/g dry weight, respectively. The composition of PBDEs differed according to the type of sludge. Among the PBDE congeners, BDE 209 was dominant in all sludge samples. After BDE 209, relatively high levels were found for BDE 28 and 47 from industrial sludge, BDE 47 and 99 from domestic wastewater sludge, and BDE 206, 207, and 208 from livestock sludge. Using hierarchical cluster analysis, sludges were divided into three groups according to PBDE congener composition. A risk assessment of PBDEs in sludge used for soil amendment was carried out. Preliminary results indicated that the potential risk of soil exposed to PBDEs in sludge was relatively low.     

PCBs, PCNs and PBDEs in sediments and mussels from Qingdao coastal sea in the frame of current circulations and influence of sewage sludge

Influence of current circulation and sewage sludge on spatial distributions of polychlorinated biphenyls (PCBs), polychlorinated naphthalenes (PCNs), and polybrominated diphenyl ethers (PBDEs) in sediments and mussels from the Qingdao coastal sea were investigated. Total concentrations of PCBs, PCNs and PBDEs in sediments ranged 6.5-32.9, 0.2-1.2, and 0.1-5.5 ngg(-1) dry wt, respectively. The maximum concentrations were all found near the Haibo River mouth, affected by sewage sludge input from the river. Under the current system in Jiaozhou Bay the organic pollutants were subject to deposit on the east side of the bay and trapped inside the bay. Sewage sludge was an important source of PCBs, PCNs and PBDEs in the bay and exponentially magnified the enrichment of PCBs. On the other hand, the congener profiles of PCBs in sediments outside the bay may signify an atmospheric source of PCBs. Total Concentrations of PCBs, PCNs and PBDEs in mussels were 61.4-88.6, 9.0, and 13.8 ngg(-1)lipid, respectively. Mussels enriched significantly PCBs, PCNs and PBDEs relative to the sediments. The total toxicity equivalent quantities (TEQs) of PCNs in mussels were generally lower than that of PCBs. The fluxes of the total PCBs and their TEQs have been decreased steadily since 1950s. The lower chlorinated/brominated congeners of PCNs and PBDEs may exhibit a greater tendency due to less lipophilic and thus a greater probability of being affected by the current circulation in the bay.     

Changes of polycyclic aromatic hydrocarbons during composting of sewage sludges with chosen physico-chemical properties and PAHs content

The aim of the experiment was to determine changes in the PAH content during sewage sludge composting. The extent was evaluated to which sewage sludge properties influences on PAHs losses during composting. Five municipal sewage sludges were studied from sewage treatment plants located in the south-east of Poland, i.e. in Stalowa Wola, Kra?nik, Lublin, Zamo?? and Bi?goraj. The treatment plants selected were characterised by their differentiation with catchments area as well as the industrial character of the areas. Sludge composting was carried out in aerobic conditions in plastic containers for a period of 76 days. The content of 14 polycyclic aromatic hydrocarbons (PAHs) and some physical-chemical (TOC, Nt, TOC/Nt, CEC, BS, TEB, pH, available potassium and phosphorus, total forms of cations) sewage sludge properties were monitored. In the present study correlations between PAHs losses (during various phases of composting) and physical-chemical properties of sewage sludges and composts were also evaluated. The sewage sludges were characterised both by differentiated properties and by PAH content. The total PAH content (the sum of 14 PAHs from the EPA List with exception of naphthalene and acenaphthene) in the sludges ranged from 3674 to 11236 microg kg(-1). Four- and three-ring compounds were predominant in the sewage sludges. Almost all of the sludges were characterised by differentiated content levels of both individual PAHs groups and PAHs sum. After 76 days of composting, a significant lowering of the PAH content was observed in all sludges as compared to the beginning of the experiment. The range of total observed PAH losses was from 15.8% to 48.6%, depending on the sewage sludge. The largest lowering of the PAH content was observed in the sludge with the lowest concentration of the xenobiotics studied. The largest losses in individual PAHs were observed in the case of five- and six-rings compounds, and were probably related to strong pollutant binding by other components of the sewage sludge. The few significant relationships showed that PAH losses during composting were only slightly determined by the analysed physical-chemical properties.     

Comparison of sewage sludge toxicity to plants and invertebrates in three different soils

Understanding the effect of soil type on the overall toxicity of sewage sludge is one of the most important issues concerning environmental risks associated with the sewage sludge land application. The aim of the study was to determine the influence of different soils (sandy, loamy and OECD soil) on sewage sludges toxicity in relation to plants (Lepidium sativum, Sorghum saccharatum, Sinapis alba) and an invertebrate species (Heterocypris incongruens). The most evident negative influence of sewage sludges on root growth was observed in the case of OECD soil. The EC(50) values determined on the basis of the root growth inhibition of all tested plants were in the range 0.1-6.4%, 0.03-9.4% and 6.6-22.1% (% of sewage sludgekg(-1) soil) for OECD, sandy and loamy soil, respectively. Soil type also affects the sewage sludge toxicity in relation to H. incongruens. The LC(50) (mortality) values ranged from 0.26% to 11.5% depending on the sludge tested. For EC(50) (growth inhibition) values ranged from 10.7% to 36.2%.     

Analysis and evaluation of chlorinated persistent organic compounds and PAHs in sludge in Korea

The concentrations of 12 POPs listed in the Stockholm convention, chlorophenols (CPs) and PAHs were investigated in sludge samples from wastewater and sewage treatment plants (WWTPs and STPs). The concentrations of PCDD/Fs in the wastewater sludge ranged from 0.189 to 1092 ng-TEQkg(-1) dry wt., and most of the sludge samples had levels below the EU guideline for the land application of PCDD/Fs (<100 ng-TEQkg(-1) dry wt.) except one sample. Co-PCB congeners were analyzed from four WWTPs, with total concentrations ranging from 0.265 to 26.6 ng-TEQkg(-1) dry wt., which were similar to the results obtained from previous studies. The levels of PCDD/Fs and Co-PCBs varied according to the main source of the influent to each WWTP and the paper industry was the main source of these compounds in the sludge due to the chlorine bleaching process. In case of OCPs, HCB and p,p'-DDE were detected at relatively high levels in the sludge samples compared to other target compounds, ranging from 1.30 to 21.5 microg kg(-1) dry wt. and 0.758 to 14.8 microg kg(-1) dry wt., respectively. Different OCP distribution patterns were observed according to sludge types, with HCB and DDTs being dominant in the sludge from WWTPs and STPs, respectively. The total levels of PAHs and CPs ranged from 1.24 to 44.9 mg kg(-1) dry wt. and 0.340 to 3.85 mg kg(-1) dry wt., respectively. The PAHs and CPs were also shown to have various distribution patterns, possibly due to the different wastewater sources to the WWTPs.     

Short- and long-chain perfluorinated acids in sewage sludge from Shanghai, China

Perfluorinated acids (PFAs) are the subject of increasingly intense environmental research. In this study, sewage sludge samples were collected from 25 wastewater treatment plants (WWTPs) in Shanghai, China to evaluate the levels and profile of C3-C14 PFAs. The results showed a ubiquitous PFAs contamination of sewage sludge in Shanghai with the total PFAs (∑PFAs) range of 126-809 ng g(-1)dw. Perfluorooctanoic acid (PFOA) was found to be the dominant PFA pollutant and its concentration ranged from 23.2 to 298 ng g(-1)dw, much higher than the levels in other countries. Moreover, concentrations of short-chain PFAs (相似文献   

Brominated flame retardants in the Australian population: 1993-2009

Brominated flame retardants, including hexabromocyclododecane (HBCD) and polybrominated diphenyl ethers (PBDEs) are used to reduce the flammability of a multitude of electrical and electronic products, textiles and foams. The use of selected PBDEs has ceased, however, use of decaBDE and HBCD continues. While elevated concentrations of PBDEs in humans have been observed in Australia, no data is available on other BFRs such as HBCD. This study aimed to provide background HBCD concentrations from a representative sample of the Australian population and to assess temporal trends of HBCD and compare with PBDE concentrations over a 16 year period. Samples of human milk collected in Australia from 1993 to 2009, primarily from primiparae mothers were combined into 12 pools from 1993 (2 pools); 2001; 2002/2003 (4 pools); 2003/2004; 2006; 2007/2008 (2 pools); and 2009. Concentrations of ∑HBCD ranged from not quantified (nq) to 19 ng g(-1)lipid while α-HBCD and γ-HBCD ranged from nq to 10 ng g(-1)lipid and nq to 9.2 ng g(-1)lipid. β-HBCD was detected in only one sample at 3.6 ng g(-1)lipid while ∑(4)PBDE ranged from 2.5 to 15.8 ng g(-1)lipid. No temporal trend was apparent in HBCD concentrations in human milk collected in Australia from 1993 to 2009. In comparison, PBDE concentrations in human milk show a peak around 2002/03 (mean ∑(4)PBDEs=9.6 ng g(-1)lipid) and 2003/04 (12.4 ng g(-1)lipid) followed by a decrease in 2007/08 (2.7 ng g(-1)lipid) and 2009 (2.6 ng g(-1)lipid). In human blood serum samples collected from the Australian population, PBDE concentrations did not vary greatly (p=0.441) from 2002/03 to 2008/09. Continued monitoring including both human milk and serum for HBCD and PBDEs is required to observe trends in human body burden of HBCD and PBDEs body burden following changes to usage.     

The air-water exchange of polychlorinated biphenyls and polybrominated diphenyl ethers at an urban lake, a receipt water body for the effluent from a municipal sewage treatment plant

The effluents and sludge from municipal sewage treatment plants (MSTPs) are considered as potential sources of many contaminants to the ambient environments. In the present work, the air-water exchange of polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) was studied using passive air samplers at an urban lake, which receives the effluents from a MSTP in Beijing, China. The concentrations of PCBs and PBDEs in atmosphere were in the range 15.5-108 ng sample⁻¹ and 2.37-27.8 ng sample⁻¹, respectively, during the sampling period (August, 2007-July, 2008). The predominant PCBs and PBDEs were lowly halogenated congeners. The calculation for the exchange fluxes of PCBs and PBDEs using fugacity model showed that, the net exchange fluxes in different seasons were closely related to the halogen number of different congeners. Except for CBs-28 and 52, the net exchange fluxes was mainly directed from air to water for most of predominant congeners, which implied that the lower chlorinated CBs were dominated by volatilization process rather than the dry/wet depositions and diffusion between air-water interface, additionally, for heavy congeners, the dry/wet deposition process was an important source of PCBs and PBDEs in this lake.     

Occurrence and concentrations of polybrominated diphenyl ethers in sewage sludge from three wastewater treatment plants in Kuwait

Polybrominated diphenyl ether (PBDE) concentrations were measured in sewage sludge samples collected from three wastewater treatment plants in Kuwait over a six month period. PBDEs were detected in all samples analyzed and there were significant differences between the three wastewater treatment plants. The mean (and range) of summation PBDEs concentrations measured are as follows: Jahra 52.5 ng g(-1) (5.7-169.5 ng g(-1)); Reqqa, 144 ng g(-1) (32-296 ng g(-1)); Umm Haylaman, 377 ng g(-1) (23-1599 ng g(-1)). The differences in concentrations of the sum of penta congeners were consistently different at the three treatment plants with values increasing in the order: Jahra相似文献   

Waste water treatment plants as sources of polyfluorinated compounds, polybrominated diphenyl ethers and musk fragrances to ambient air

To investigate waste water treatment plants (WWTPs) as sources of polyfluorinated compounds (PFCs), polybrominated diphenyl ethers (PBDEs) and synthetic musk fragrances to the atmosphere, air samples were simultaneously taken at two WWTPs and two reference sites using high volume samplers. Contaminants were accumulated on glass fiber filters and PUF/XAD-2/PUF cartridges, extracted compound-dependent by MTBE/acetone, methanol, or hexane/acetone and detected by GC-MS or HPLC-MS/MS. Total (gas + particle phase) concentrations ranged from 97 to 1004 pg m⁻³ (neutral PFCs), <MQL to 13 pg m⁻³ (ionic PFCs), 5781 to 482,163 pg m⁻³ (musk fragrances) and <1 to 27 pg m⁻³ (PBDEs) and were usually higher at WWTPs than at corresponding reference sites, revealing that WWTPs can be regarded as sources of musk fragrances, PFCs and probably PBDEs to the atmosphere. Different concentrations at the two WWTPs indicated an influence of WWTP size or waste water origin on emitted contaminant amounts.     

Long-chain perfluorinated chemicals in digested sewage sludges in Switzerland

This study focused on the occurrence of long-chain perfluorinated chemicals (PFCs) in anaerobically stabilized sewage sludges from 20 municipal WWTPs using current and historic samples to evaluate the levels of PFCs and to identify the relative importance of commercial and industrial sources. A quantitative analytical method was developed based on solvent extraction of the analytes and a LC-MS/MS system. For total perfluoralkyl carboxylates (PFCAs), the concentrations ranged from 14 to 50 μg/kg dry matter. Concentrations of perfluorooctane sulfonic acid (PFOS) ranged from 15 to 600 μg/kg dry matter. In three WWTPs, the PFOS levels were six to nine times higher than the average values measured in the other plants. These elevated PFOS concentrations did not correlate with higher levels of PFCAs, indicating specific additional local sources for PFOS at these WWTPs. Average concentrations in selected samples from the years 1993, 2002, and 2008 did not change significantly.     

Analysis of some polyhalogenated organic pollutants in sediment and sewage sludge

A laminated sediment core collected in the southern part of the Baltic Proper was analysed for DDT compounds, polychlorinated biphenyls (PCB) including the coplanar congeners, polybrominated diphenyl ethers (PBDE) and polychlorinated naphthalenes (PCN). Two sewage sludge samples were also analysed for the same compounds.

The results of the sediment analyses indicate the presence of PCB, DDT and PBDE compounds in sediment layers dating from the 1950s and later. Neither coplanar PCB nor PCN were detected at any level of the sediment core. The PCB concentrations indicate a slight increase in levels during the last decades, while there were no changes in the levels of DDT compounds. In contrast, TeBDE levels increase 4- to 8-fold and one PeBDE congeners levels increase 10- to 20-fold. The results of sewage sludge analyses showed the concentration of the individual PBDE to be at about the same level as for the individual PCB congeners. The congener pattern in sludge samples indicates low-chlorinated products to be the main PCN source.