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Organohalogen contaminants in wildlife from the Yangtze River Delta: Development of methods and assessments of legacy and emerging persistent organic pollutants
Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Stockholm University.
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Rapid economic development has occurred during the past few decades in China with the Yangtze River Delta (YRD) area as one of the most progressive areas. The urbanization, industrialization, agricultural and aquaculture activities result in extensive production and application of chemicals. Organohalogen contaminants (OHCs) have been widely used as i.e. pesticides, flame retardants and plasticizers. They are persistent, bioaccumulative and pose a potential threat to ecosystem and human health. However, limited research has been conducted in the YRD with respect to chemicals environmental exposure.

The main objective of this thesis is to investigate the contamination level, distribution pattern and sources of OHCs in the YRD. Wildlife from different habitats are used to indicate the environmental pollution situation, and evaluate selected matrices for use in long term biomonitoring to determine the environmental stress the contamination may cause. In addition, a method is developed for dicofol analysis. Moreover, a specific effort is made to introduce statistic power analysis to assist in optimal sampling design.

The thesis results show extensive contamination of OHCs in wildlife in the YRD. The occurrences of high concentrations of chlorinated paraffins (CPs) are reported in wildlife, in particular in terrestrial species, (i.e. short-tailed mamushi snake and peregrine falcon). Impurities and byproducts of pentachlorophenol products, i.e. polychlorinated diphenyl ethers (PCDEs) and hydroxylated polychlorinated diphenyl ethers (OH-PCDEs) are identified and reported for the first time in eggs from black-crowned night heron and whiskered tern. High concentrations of octachlorodibenzo-p-dioxin (OCDD) are determined in these samples. The toxic equivalents (TEQs) of polychlorinated dibenzo-p-dioxin (PCDDs) and polychlorinated dibenzofurans (PCDFs) are at mean levels of 300 and 520 pg TEQ g-1lw (WHO2005 TEQ) in eggs from the two bird species, respectively. This is two orders of magnitude higher than European Union (EU) regulation limit in chicken eggs. Also, a novel pattern of polychlorinated biphenyls (PCBs) with octa- to decaCBs, contributing to as much as 20% of total PCBs therein, are reported in birds. The legacy POPs shows a common characteristic with relatively high level of organochlorine pesticides (i.e. DDT, hexacyclohexanes (HCHs) and Mirex), indicating historic applications. In contrast, rather low concentrations are shown of industrial chemicals such as PCBs and polybrominated diphenyl ethers (PBDEs).

A refined and improved analytical method is developed to separate dicofol from its major decomposition compound, 4,4’-dichlorobenzophenone. Hence dicofol is possible to assess as such. Statistic power analysis demonstrates that sampling of sedentary species should be consistently spread over a larger area to monitor temporal trends of contaminants in a robust manner.

The results presented in this thesis show high CPs and OCDD concentrations in wildlife. The levels and patterns of OHCs in YRD differ from other well studied areas of the world. This is likely due to the extensive production and use of chemicals in the YRD. The results strongly signal the need of research biomonitoring programs that meet the current situation of the YRD. Such programs will contribute to the management of chemicals and environment in YRD, with the potential to grow into the human health sector, and to expand to China as a whole.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2016. , 83 p.
Keyword [en]
Organochlorine pesticides, flame retardants, chlorinated paraffins, PCBs, PCDEs, PBDEs, PCDD/Fs, dicofol, environmental monitoring, bioindicator, shellfish, snail, bird eggs
National Category
Environmental Sciences Analytical Chemistry Other Chemistry Topics
Research subject
Environmental Chemistry
Identifiers
URN: urn:nbn:se:su:diva-131986ISBN: 978-91-7649-477-6OAI: oai:DiVA.org:su-131986DiVA: diva2:946394
Public defence
2016-09-02, William-Olssonsalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 2: Manuscript. Paper 5: Submitted. Paper 6: Manuscript.

 

Available from: 2016-08-09 Created: 2016-07-05 Last updated: 2016-09-06Bibliographically approved
List of papers
1. Chlorinated and brominated organic pollutants in shellfish from the Yellow Sea and East China Sea
Open this publication in new window or tab >>Chlorinated and brominated organic pollutants in shellfish from the Yellow Sea and East China Sea
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2015 (English)In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 22, no 3, 1713-1722 p.Article in journal (Refereed) Published
Abstract [en]

The global contamination with persistent organic pollutants (POPs), or compounds with similar characteristics, is well known. Still there are data gaps for POP concentrations from many areas in the world. The aim of the present study is to assess several legacies POPs and also hexabromocyclododecane (HBCDD) and methoxylated polybrominated diphenyl ethers (MeO-PBDEs) in shellfish from three locations in the Yellow Sea and East China Sea. The sources of the contaminants are discussed. Pooled samples were treated by liquid-liquid extraction and acid and column cleanup prior to analysis by gas chromatogram equipped with electron capture detector (GC-ECD) and gas chromatography-mass spectrometry (GC-MS). The by far most abundant environmental contaminant originates from dichlorodiphenyltrichloroethane (DDT), independent of species analyzed or sampling site. The results indicate ongoing or at least recent discharges of DDT. The second highest concentrations were reported for HBCDD (21–40 ng/g fat) in the shellfish, independent of sampling sites. The two natural products, 6-MeO-BDE-47 and 2′-MeO-BDE-68, were also present in the shellfish (1.3–22 and 1–14 ng/g fat, respectively). The polychlorinated biphenyl (PCB) congener CB-153 (0.8–6.5 ng/g fat), hexachlorobenzene (HCB) (1.1–3.6 ng/g fat), and β-hexachlorocyclohexane (β-HCH) (2.3–4.9 ng/g fat) were all higher than the concentrations of other HCH isomers, β-endosulfan, PBDE congeners, and mirex. Apart from the DDTs and HBCDDs, it is evident that the pollution of shellfish was similar to, or lower than, the contamination of shellfish in other parts of the world.

Keyword
Shellfish, Pesticides, HBCDD, DDT, MeO-PBDE, China
National Category
Chemical Sciences Earth and Related Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-112141 (URN)10.1007/s11356-014-3198-8 (DOI)000348917400021 ()
Available from: 2015-01-09 Created: 2015-01-09 Last updated: 2016-07-05Bibliographically approved
2. A refined method for analysis of 4,4’-dicofol and 4,4’-dichlorobenzophenone
Open this publication in new window or tab >>A refined method for analysis of 4,4’-dicofol and 4,4’-dichlorobenzophenone
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(English)Manuscript (preprint) (Other academic)
Keyword
dicofol, on-column injection, dichlorobenzophenone, cod, recovery study
National Category
Analytical Chemistry
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-131982 (URN)
Available from: 2016-07-05 Created: 2016-07-05 Last updated: 2016-07-06Bibliographically approved
3. Extensive organohalogen contamination in wildlife from a site in the Yangtze River Delta
Open this publication in new window or tab >>Extensive organohalogen contamination in wildlife from a site in the Yangtze River Delta
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2016 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 554, 320-328 p.Article in journal (Refereed) Published
Abstract [en]

The environmental and human health concerns for organohalogen contaminants (OHCs) extend beyond the 23 persistent organic pollutants (POPs) regulated by the Stockholm Convention. The current, intense industrial production and use of chemicals in China and their bioaccumulation makes Chinese wildlife highly suitable for the assessment of legacy, novel and emerging environmental pollutants. In the present study, six species of amphibians, fish and birds were sampled from paddy fields in the Yangtze River Delta (YRD) were screened for OHCs. Some extensive contamination was found, both regarding number and concentrations of the analytes, among the species assessed. High concentrations of chlorinated paraffins were found in the snake, Short-tailed mamushi (range of 200-340 mu g g(-1) lw), Peregrine falcon (8-59 mu g g(-1) lw) and Asiatic toad (97 mu g g(-1) lw). Novel contaminants and patterns were observed; octaCBs to decaCB made up 20% of the total polychlorinated biphenyls (PCBs) content in the samples and new OHCs, substituted with 5-8 chlorines, were found but are not yet structurally confirmed. In addition, Dechlorane 602 (DDC-DBF) and numerous other OHCs (DDTs, hexachlorocyclohexanes (HCHs), polybrominated diphenyl ethers (PBDEs), hexbromocyclododecane (HBCDD), chlordane, heptachlor, endosulfan and Mirex) were found in all species analyzed. These data show extensive chemical contamination of wildlife in the YRD with a suite of OHCs with both known and unknown toxicities, calling for further indepth studies.

Keyword
Wildlife, Chlorinated paraffins (CPs), Persistent organic pollutants (POPs), Emerging contaminants, Yangtze River Delta
National Category
Earth and Related Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-129886 (URN)10.1016/j.scitotenv.2016.02.176 (DOI)000373274700035 ()26956179 (PubMedID)
Available from: 2016-05-06 Created: 2016-05-03 Last updated: 2016-07-05Bibliographically approved
4. A novel pollution pattern: Highly chlorinated biphenyls retained in Black-crowned night heron (Nycticorax nycticorax) and Whiskered tern (Chlidonias hybrida) from the Yangtze River Delta
Open this publication in new window or tab >>A novel pollution pattern: Highly chlorinated biphenyls retained in Black-crowned night heron (Nycticorax nycticorax) and Whiskered tern (Chlidonias hybrida) from the Yangtze River Delta
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2016 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 150, 491-498 p.Article in journal (Refereed) Published
Abstract [en]

Contamination of organochlorine pesticides (OCPs), polychlorinated diphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), hydroxylated polybrominated diphenyl ethers (OH-PBDEs) and their methylated counterparts (MeO-PBDEs) were determined in Black-crowned night heron (Nycticorax nycticorax) and Whiskered tern (Chlidonias hybrida) from two drinking water sources, e.g. Tianmu lake and East Tai lake in Yangtze River Delta, China. A novel PCBs contamination pattern was detected, including 11% and 6.9% highly chlorinated biphenyls (PCBs with eight to ten chlorines) in relation to total PCB concentrations in the Black-crowned night heron and Whiskered tern eggs, respectively. The predominating OCPs detected in the present study were 4,4'-DDE, with concentration range 280-650 ng g(-1) lw in Black crowned night heron and 240-480 ng g(-1) lw in Whiskered tern, followed by beta-HCH and Mirex. 6MeO-BDE-90 and 6-MeO-BDE-99 are the two predominant congeners of MeO-PBDEs whereas 6-OH-BDE-47 contributes mostly to the OH-PBDEs in both species. Contamination level was considered as median or low level compared global data.

Keyword
Organochlorine pesticides (OCPs), Polychlorinated diphenyls (PCBs), Polybrominated diphenyl ethers (PBDEs), Water bird, Yangtze river delta (YRD)
National Category
Earth and Related Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-129889 (URN)10.1016/j.chemosphere.2015.11.112 (DOI)000372765100060 ()26705146 (PubMedID)
Available from: 2016-05-06 Created: 2016-05-03 Last updated: 2016-07-05Bibliographically approved
5. High concentrations of OCDD and related chemicals in heron and tern eggs from Yangtze River Delta indicating PCP origin
Open this publication in new window or tab >>High concentrations of OCDD and related chemicals in heron and tern eggs from Yangtze River Delta indicating PCP origin
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(English)Article in journal (Other academic) Submitted
Place, publisher, year, edition, pages
Stockholm:
Keyword
PCDD/Fs, PCDEs, OH-PCDEs, Yangtze River Delta, bird egg
National Category
Analytical Chemistry Organic Chemistry
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-131984 (URN)
Available from: 2016-07-05 Created: 2016-07-05 Last updated: 2016-07-06Bibliographically approved
6. Sampling designs for contaminant temporal trend analyses using sedentary species exemplified by the snails (Bellamya aeruginosa) and (Viviparus viviparus)
Open this publication in new window or tab >>Sampling designs for contaminant temporal trend analyses using sedentary species exemplified by the snails (Bellamya aeruginosa) and (Viviparus viviparus)
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(English)Manuscript (preprint) (Other academic)
Keyword
Sampling design, convenience sampling, clustered sampling, statistical power; temporal trend assessment, organic contaminants, benthic organisms
National Category
Computational Mathematics Other Chemistry Topics
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-131983 (URN)
Available from: 2016-07-05 Created: 2016-07-05 Last updated: 2016-07-06Bibliographically approved

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