1

Environment and human exposure to persistent organic pollutants (POPs) in India: A systematic review of recent and historical data

Brij Mohan Sharmaa,*, Girija K. Bharatb, Shresth Tayala,b, Luca Nizzettoc,d, Pavel Čuprd, Thorjørn Larssenc

aTERI University, 10 Institutional Area, Vasant Kunj, NewDelhi- 110070, Delhi, India.

bThe Energy and Resources Institute, Darbari Seth Block, India Habitat Center, Lodhi Road New Delhi, DL 110003 (India).

cNorwegian Institute for water Research, Gaustadalleen 21, Oslo 0349, Norway.

dResearch Centre for Toxic Compounds in the Environment, Masaryk University, Brno 62500, Czech Republic.

*Corresponding author at: Department of Natural Resources, TERI University, 10 Institutional Area, Vasant Kunj, New Delhi-110070, India. Email: brijmsharma05@gmail.com

Electronic Supplementary Information

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S1. Approach for the Systematic study

S1.1 data collection

Search of all studies on India, published between November 2012 and 1980 that analyzed the distribution of concentrations of persistent organic pollutants in representative samples from various possible sources of surface water (rivers, small streams, ponds, lakes, coastal water, rain water, etc.), ground water, soil, sediments, aquatic biota, and human compartments (blood and breast milk), was carried out through electronic search of the databases Medline/PubMed and in other abstracting, indexing and citation databases like ScienceDirect, Scopus, ISI/Thomson’s and Blackwell’s Synergy. “Persistent organic pollutants”, “POPs”, “persistent toxic substances”, “PTS”, “PTSs”, “persistent toxic pollutants”, “persistent toxic residues”, “environmental pollutants/toxicants”, “environmental exposure/adverse effects”, “human population”, “chlorinated pesticides”, “insecticides”, “human blood”, “human biomonitoring”, “environmental monitoring”, “human samples”, “human milk”, “Stockholm Convention”, “serum”, “breast milk”, terms and their combinations were used while searching the data. Specific chemical names (e.g. DDT (dichlorodiphenyltrichloroethane), HCH (hexachlorocyclohexane), aldrin, dieldrin, endrin, chlordane, heptachlor, mirex, HCB, endosulfan, PCBs, polychlorinated biphenyls, and PFOS, fluorinated compounds) were also used in combinations with precious terms. Printed media was also searched for reports of Ministry of Environment and Forests (MoEF), Central/State Pollution Control Boards, Ministry of Agriculture; Ministry of Health and Family Welfare and other related ministries and agencies. Similar methods for data collection were adopted for searching data on POPs contamination in surface water, human and aquatic organisms in China.

S1.2 Conditions for inclusion and exclusion

Included literature was broadly of two types: studies published in peer reviewed journals generally lead by scientific research groups and reports of national and international government agencies. Studies/reports, which were not approved by relevant authorities, were not included in this study.

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Fig. S1. Consumption of pesticides in metric tons (MoSPI, GOI, 2009-10), sewage generation in MLD (CPCB, GOI, 2009-10) and gross domestic product in million US$ (Directorate of Economics & Statistics of respective State Governments and All India Central Statistics office, 2010) in India. (Logarithmic Scale)

Fig. S2. Annual production of DDTs and HCHs in India (Ministry of Agriculture, Govt. of India)

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Table S1. Average concentrations (ng/L) of POPs in surface water resources in various regions of India

Indian StateSource and sampling year

Aldrin Dieldrin Endrin Chlordane Heptachlor Mirex HCBendosulfaΣ

nReferences

Uttar Pradesh Gomti River (NA) 13.2 5.72 0.17 7.14 11.55 - 6.4 16.48 (Malik et al. 2009)

Lucknow, Uttar Pradesh

Rain Water (NA) 0.28 2.41 BDL 3.14 2.2 - 0.94 2.99 (Malik et al., 2007)

Unnao, Uttar Pradesh

Streams, Ponds and canals (2003)

0.5 < 0.05 < 0.05 < 0.1 4 - 0.2 7 (Singh et al., 2007)

Tamil NaduTamiraparani river basin (2008-2009)

<0.02–1.5

<0.03–7.5 <0.02–58.0 <0.01-0.49 <0.06-2.1<0.01-

0.7- -

(Kumarasamy et al., 2012)

Aldrin Dieldrin Heptachlor endosulfaΣn

References

Devprayag, Uttarakhand

Ganges River (2010)

2.3 - 0.07 ND

(Mutiyar and Mittal, 2013)

Rishikesh, Uttarakhand

1.89 - 0.32 0.92

Haridwar, Uttarakhand

0.12 - 0.06 0.16

Kannauj, Uttar Pradesh

Ganges River (2011)

1.2–1.3 - 0.14–0.2 0.8–31.6

(Mutiyar and Mittal, 2013)

Kanpur, Uttar Pradesh

ND–1.1 - ND–0.08 9.7–11.6

Allahabad, Uttar Pradesh

ND–0.4 - ND ND–0.15

Varanasi, Uttar Pradesh

0.5–2.2 - ND–0.1 ND–85.4

Lucknow, Uttar Pradesh

Gomti River (2011) 0.6 - ND 1.16(Mutiyar and Mittal, 2013)

Patna, Bihar Ganges River (2011) ND–1.17 - ND ND–5.03(Mutiyar and Mittal, 2013)

Bhagalpur, Bihar Ganges River (2011) 8.8–16.4 - 3.2–11.8 13.8–17.9(Mutiyar and Mittal, 2013)

5

Table S1. Continued

Indian State Source and sampling year

Aldrin Dieldrin Heptachlor endosulfaΣn

References

Hisar, Haryana Rain Water (2002) - - 3.33 786.83 (Kumari et al., 2007)

West BengalWater bodies near Tea Gardens (2006)

- - 4300 2100 (Bishnu et al., 2009)

HaryanaGhaggar River (1999-2000)

< 0.04 < 0.14 - < 0.3 (Kaushik et al., 2010)

Delhi Yamuna (1995-01) 0 – 0.237 0 – 0.129 - (CPCB 2000)

Kanpur, Uttar Pradesh

Ganges River (NA) ND 278.5 - ND(Sankararamakrishnan et al., 2005)

Andhra Pradesh

Kolleru lake,Prawn Ponds (NA)

- 11.2 - 98.6 (Amaraneni, 2006)

Andhra Pradesh

Kolleru Lake (NA) 46 86 - 2396(Amaraneni and Pillai 2000)

Jaipur, Rajasthan

Ramgarh water reservoir (NA)

- - 1352000 (Bakore et al., 2004)

Bhagalpur, Bihar

Ganges River (2007-08) - - - 241.7 (Singh et al., 2012)

Kumaon Himalayan Region, Uttrakhand

Sharda (kali river) (1999)

- - - ND

(Sarkar et al., 2003)

Saryu (1999) - - - ND

Gori (1999 - - - ND

Ram Ganga (1999) - - - ND

Dhuali (1999) - - - ND

Kosi (1999) - - - ND

Gomti River (1999) - - - 2

Ladhiya (1999) - - - ND

Lohawati (1999) - - - ND

PCBsΣ Chlordane References

Delhi Yamuna (NA) 0.041 0.000008(Anbu et al., 2002)

Kolkata, West Bengal

Hooghly river (NA) 0.00045 0.00018(Anbu et al., 2002)

GoaMandori Suburban river (NA)

0.0026 0.000035(Anbu et al., 2002)

Bangalore, Andhra Pradesh

Ulsoor Lake (NA) 0.048 0.00054(Anbu et al., 2002)

Chennai, Tamil Nadu

Cooum River (NA) 0.0015 0.001(Anbu et al., 2002)

Delhi Yamuna (1999)0.190 –

1.92-

(Parivesh, 2001)

Chennai, Tamil Nadu Bay of Bengal (Sea

Water), (1998)

4.458 -(Rajendran et al., 2005)Cuddalore,

Tamil Nadu1.934 -

PFOS References

Allahabad, Uttar Pradesh

Yamuna River (2008) 1.81(Yeung et al., 2009)

Patna, Bihar Ganga River (2008) 0.363(Yeung et al., 2009)

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Table S2. Average concentrations (ng/L) of POPs in ground water in various regions of India

Indian State Source and sampling year AldrinDieldri

nHeptachlo

rendosulfaΣ

nReferences

Hisar, Haryana Tubewell (2002-2003) - - - 183.66 (Kumari et al., 2008)

Delhisamples of ground water used for agricultural purposes (NA)

4.3 - < 1 53(Mukherjee and Gopal, 2002)

Jaipur, Rajasthan Tubewell (NA) - - 789000 - (Bakore et al., 2003)

Kanpur, Uttar Pradesh

samples from the Agricultural area (NA)

ND ND - ND(Sankararamakrishnan et al., 2005)samples from the industrial

area (NA)ND 2486.3 - ND

Agra, Uttar Pradesh

Groundwater (NA) 53.27 254.47 29.4 12.27 (Singh, 2001)

Hyderabad, Andhra Pradesh

Domestc well supply (NA) - - - 2610.67 (Shukla et al., 2006)

Table S3. Average concentrations (ng/g) of POPs in soil in various regions of India

Indian StateSource and sampling year Aldrin Dieldrin Endrin Chlordane

Heptachlor

endosulfaΣn HCB References

Hisar, HaryanaSoil from Farmers fields (2002-2003)

- - - 8.8 - 18.916 - (Kumari et al., 2008)

Unnao District, Uttar Pradesh

Agricultural soils (NA)

0.16 < 0.05 < 0.05 0.04 0.25 0.23 0.06 (Singh et al., 2007)

Agra, Uttar Pradesh

349 843 - - 232 30 - (Singh, 2001)

West Bengalsamples collected from nearby area to Tea Garden (2006)

- - - - 238 4701 - (Bishnu et al., 2009)

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Table S4. Average concentrations (ng/g) of POPs in sediments in various regions of India

Indian State Source and sampling year Aldrin Dieldrin Endrin Chlordane Heptachlor Mirex ΣPCBs HCB Σendosulfan PBDEs References

Delhi Yamuna River (NA) 11.65 21.8 26.81 - 8.9 - - - - - (Pandey et al., 2011)

Delhi Yamuna River (2010) - - - - - -0.16-30.05

- - - (Kumar et al. 2011)

Keoladeo National Park, Bharatpur, Rajasthan

Inside National Park (NA) 478.4 117.32965.

9- 4617.1 - - - 4529.5 -

(Bhadouria et al. 2012)Outside National Park (NA) 687.3 439.5

2198.4

- 3854.3 - - - 4542.5 -

Uttar Pradesh Gomti River (NA) 0.98 0.19 0.54 0.62 5.12 - - 0.12 0.14 - (Malik et al. 2009)

Bhagalpur, Bihar Ganga River (2007-08) - - - - - - - - 178.77 - (Singh et al., (2012)

West BengalLower stretch of Hugli estuary (2003)

- < 0.05 < 0.05 - - < 0.10 0.75 0.144 - - (Guzzella et al., 2005)

sunderban wetlands

Bay of Bengal (2005) - - - - - - 6.637 0.274 - 4.893(Sarkar et al., Binelli et al., Binelli et al., 2007)

East coast of IndiaMouth of Hugli estuary, (1998, 1999, 2000)

- - - - - - - - 105 -(Bhattacharya et al., 2003)

- - - - - - - - 203.81 -- - - - - - - - 107.25 -

Mumbai, Maharashtra

surface sediment of A. marina (NA)

0.049 - - - - - - - 0.183 - (Shete et al., 2009)

Mumbai, Maharashtra

Thane creeks (NA) - - - - - - 6.467 - - - (Sahu et al., 2009)

Andhra PradeshKolleru lake ,Prawn Ponds (NA)

-1-

19600- - - - - -

89600-238000

- (Amaraneni, 2006)

Tamil Nadu, South India

Tamiraparani river basin (2008-09)

<0.02–562

<0.03–1693

<0.02<0.01-

93.6<0.06-103

<0.01-88.5

- - - -(Kumarasamy et al. 2012)

Chennai, Tamil Nadu

Bay of Bengal (1998)

- - - - - -1.801

95- - -

(Rajendran et al., 2005)

Mahapalipuram, Tamil Nadu

- - - - - -0.041

7- - -

Pondicherry - - - - - -0.026

3- - -

Cuddalore, Tamil Nadu

- - - - - -0.489

4- - -

Nagapattinum, Tamil Nadu

- - - - - -0.055

2- - -

Mandapam, Tamil Nadu

- - - - - -0.090

8- - -

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Table S5. Average concentrations (ng/g) of POPs in biota samples from various regions of India

Indian State Species Name PCBsΣ Dieldrin Chlordane HCB Heptachlor References

Gomti River, Uttar Pradesh

fish(Channa punctatus) muscles (2004-2005)

- 1.12 0.553 < 0.1 0.803 (Malik et al., 2007)

Chilika Lake, Orrisa

Rawaddy dolphins (Year 2000-2001)

112.5 - 8.6 6.8 -(Kannan et al., 2005)

Subarnarekkha and Konarak, Orissa

green mussel (Perna viridis) (1995)

5.6 - 0.49 < 0.01 -(Tanabe et al., 2000)

Digha, West Bengal green mussel (Perna

viridis) (1995)

3.3 - 0.29 < 0.01 -(Tanabe et al., 2000)

Mahim, Maharashtra

2.1 - 0.23 0.03 -

Goa, Goagreen mussel (Perna viridis) (1995)

5.1 - 0.17 0.02 -(Tanabe et al., 2000)

Inland Wetlands, Karnataka

Anguilla bicolor bicolor (2002-03)

- <1.0 - - 10.8

( Dhananjayan and Muralidharan, 2010)

Catla catla (2002-03) - <1.0 - - 2.6

Channa striatus (2002-03) - <1.0 - - 2.8

Cirrhinus mrigala (2002-03)

- 1.6 - - <1.0

Clarias batrachus (2002-03)

- 4.4 - - 6.4

Cyprinus carpio (2002-03) - <1.0 - - 2.2

Heteropneustes fossilis (2002-03)

- <1.0 - - <1.0

Labeo rohita (2002-03) - 2.7 - - 6.7

Tilapia mossambica (2002-03)

- 2.7 - - 4.6

Mangalore, Karnataka

green mussel (Perna viridis) (1995)

3.9 - 0.68 0.01 -

(Tanabe et al., 2000)

Vishakhapatnam, Kakinada, Machilipatnam, Andhra Pradesh

1.86 - 0.883 < 0.01 -

Kolleru lake, Andhra Pradesh

Prawn - 3100 - - - (Amaraneni, 2006)

Coatal area, Tamil Nadu

green mussel (Perna viridis (1995)

1.07 - 0.396 0.15 -

(Tanabe et al., 2000)

Pondicherry, Pondicherry

10.55 - 0.235 0.06 -

Cochin and Calicut, Kerala

3.85 - 0.55 0.015 -

Bay of Bengal, India

Bottle-nose dolphin (Tursiops truncatus)(1997-99)

580 - - - -

(Karuppiah et al., 2005)

Spinner dolphin (Stenella longirostris)

141 - - - -

Hump-backed dolphin (Sousa chinensis)

1220 - - - -

9

Bay of BengalCat fish (Tachysurus thalassinus) 1997

- - - - 201.65 (Das et al., 2002)

Bay of Bengal, India (1990-91)

Bottle-nose dolphin (Tursiops truncatus)

515 - - - -

(Tanabe et al. 1993)

Spinner dolphin (Stenella longirostris)

530 - - - -

Hump-backed dolphin (Sousa chinensis)

1227 - - - -

Indian State Species NameendosulfaΣ

nAldrin Endrin PBDEΣ References

Kumaon Himalayan Region

Tor Putitora (1999) ND - - -(Sarkar, 2003)Schizothorax Richardsonii

(1999) ND - - -

Ganga River Basin,India

Fish Tissues 0.462 - - -(Akthar et al, 2009)

Gomti River, Uttar Pradesh

fish(Channa punctatus) muscles (2004-2005)

1.84 2.18 0.14 -(Malik et al., 2007)

Chilika Lake, Orrisa

Rawaddy dolphins (Year 2000-2001)

- - - 4.08(Kannan et al., 2005)

Inland Wetlands, Karnataka

Anguilla bicolor bicolor (2002-03)

3.1 - - -

(Dhananjayan and Muralidharan, 2010)

Catla catla (2002-03) <1.0 - - -

Channa striatus (2002-03) 4.3 - - -

Cirrhinus mrigala (2002-03)

2.3 - - -

Clarias batrachus (2002-03)

4.1 - - -

Cyprinus carpio (2002-03) 1.8 - - -

Heteropneustes fossilis (2002-03)

<1.0 - - -

Labeo rohita (2002-03) 3.7 - - -

Tilapia mossambica (2002-03)

<1.0 - - -

Kolleru lake, Andhra Pradesh

Prawn 27800 - - -(Amaraneni, 2006)

Bay of BengalCat fish (Tachysurus thalassinus) (1997)

- 54.046 - -(Das, et al., 2002)

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Table S6. Average concentrations (µg/l) of POPs in human blood samples from various regions of India

Indian State Source and sampling year Aldrin Dieldrin Chlordane Heptachlor endosulfanΣ PCBsΣ PBDEs References

Bhatinda, Roper District of Punjab

4 Villages (NA) 6.2 0 9.0 0.60 4.6 - - (Mathur, 2005)

Jaipur, Rajasthan

Normal Female (NA) 127.7 - - 76.3 - - -

(Mathur et al., 2002)Female suffering from Breast Cancer (NA)

2192.7 - - 523.7 - - -

Bangalore (Rural), Karnataka

Samples of Agriculture and sheep wool workers (NA)

- - - - 7.12 - -(Dhananjayan et al., 2012)

Bangalore, KarnatakaE-waste recycling workers (2007)

- - - - - 0.210 0.340 (Eguchi et al., 2012)

Chidambaram, Tamil Nadu

Residents from coastal area (2007)

- - - - - 0.140 0.330 (Eguchi et al., 2012)

Table S7. Average concentrations (ng/g lipid wt.) of POPs in human milk samples from various regions of India

Indian State Source, Age and sampling year Chlordane HCB PCBsΣ PBDEs References

New Delhi Human milk (2005-06) 2.60 3.20 23.0 - (Devanathan et al., 2009)

Ahmedabad, Gujarat Human (18-30), (1981-82) - - ND - (Jani et al., 1988)

Kolkata, Urban, West Bengal

Human milk (2009) - - 60.0 1.90(Devanathan et al., 2012)

Kolkata (Dumping site), West Bengal

Municipal dumping (2009) - - 1700.0 3.60

Kolkata, West BengalDumping site (2004-05) 5.70 2.85 265.0 - (Someya et al., 2010)

Reference site (2004-05) 2.85 4.50 39.50 - (Devanathan et al., 2009)

Banglore, Andhra Pradesh Human Milk from Urban slum (2009) - - 35.0 0.83 (Devanathan et al., 2012)

Chennai, Tamil nadu Human milk from Urban (2009) - - 36.0 2.40 (Devanathan et al., 2012)

Chennai, Tamil nadu Human milk (2002-03) 7.30 4.20 34.0 - (Subramanian et al., 2007)

Chidambaram, Tamil Nadu Human milk from Sub-urban (2009) - - 15.0 0.80 (Devanathan et al., 2012)

Parangipettai, Tamil Nadu Human milk from Fishing village (2009)  - -  32.0 1.30 (Devanathan et al., 2012)

“ND” Not detected; “– “Not analyzed

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Table S8. Analytical procedures for determination of POPs contamination in human breast milk and human blood in India

Matrices Analytes Extraction (method, condition, extraction solvents, sample size)

Clean-up Detection (method, column, mobile phase)

Recovery Detection limits Reference

Human milk 4 HCHs, 5 DDTs

n.s.; methanol, sodium oxalate and ethyl ether:petroleum ether (1:1, v/v)

Glass column packed with 5 % deactivated alumina and anhydrous sodium sulfate

GC-ECD, HP- 5 capillary column (35m x 0.32mm x 0.25 m)μ

88-97% DDTs: 0.01-0.2 ng/g lipid wt; HCHs: 0.02-0.3 ng/g lipid wt

(Mishra and Sharma, 2011b)

Human milk 12 PCBs, 13 PBDEs

High speed solvent extraction; acetone:hexane (1:1, v/v)

Gel Permeation chromatography (GPC); mobile phase- 50:50 dichloromethane and hexane

GS-MS, isotope dilution method; silica column- (30m x 0.25mm x 0.25 m) forμ PCBs and mono- to hepta-BDEs, (15m x 0.25mm x 0.1 m) for μocta- to deca-BDEs

PCBs- 69-112%, PBDEs- 82-109%

0.01 ng/g lipid wt.

(Devanathan et al., 2012)

Human milk 3 HCHs, 3 DDTs, chlordane, PCBs, HCB

Diatomaceous earth packed in glass column; diethylether; 10g

GPC, Activated florisil packed in glass column

GC-ECD PCBs: 97±4.2%; DDTs: 105±5.7%; HCHs: 98.9±6.3%; Chlordane: 103.9±4.3%; HCB: 104.1±7.9%

n.s. (Subramanian et al., 2007)

Breast milk 12 PCBs, DDTs, HCHs, chlordane, HCB

(Kunisue et al., 2004b); diatomaceous earth packed in a glass column, diethyl ether; 40g

(Kunisue et al., 2004b), gel permeation chromatography (GLP), activated florisil

GC-ECD with automatic injector

DDTs: 99.5±3.5%, PCBs: 98±1.1%, HCHs: 92±3.1%, HCB: 98±2.1%, chlordane: 101±2.2%

n.s. (Someya et al., 2010)

Human milk 3 HCHs, 4 DDTs and PCBs

n.s.; n.s., acetone/hexane (1:1 v/v), 25g

Conc. sulphuric acid GC-ECD; glass column of 8% QF1 and 5% SF 96on supelcoport (100/200). Confirmation of all compounds was done on a 5% OV-17 column

n.s. n.s. (Jani et al., 1988)

Blood samples 4 HCHs,3 DDTs, endosulfan, heptachlor

Mechanical shaking; 2 hours in a slow speed; formic acid, hexane; 4-5 ml

n.s. GC-ECD, fused silica capillary column (30m x 0.32mm x 0.5 m) μDB-608 (5% diphenyl and 95% dimethyl polysiloxane) stationary phase

94-103 % 1000 ng/l (Dhananjayan et al., 2012)

12

Human venous blood

3 DDTs, 4 HCHs, Heptachlor, aldrin, dieldrin, , - α βendosulfan and endosulfate, chlordane

US-EPA method 8081A; n.s.; Hexane/acetone (1:1); 5ml

USEPA method 3620B- Florisil cleanup by column chromatography

Trace GC-ECD; Capillary column: DB-1701 (14%-Cyanopropyl-phenyl-methylpolysiloxane), DB-5 (5% Phenyl and 95% dimethylpolysiloxane); 30m x 0.25mm, 0.25µm

> 80 % for all pesticides

n.s. (Mathur et al., 2005)

Human blood 3 HCHs, 3 DDTs, dieldrin, heptachlor

Method as suggested by (Bush et al. 1984); hexane (HPLC), methanol (5ml) and 1:1 diethylether/hexane (8ml)

Glass column packed with glass wool, activated silica gel (5g) and anhydrous sodium sulfate (5g)

GC-ECD coupled with an integrator HP 3396A. A coiled capillary column HP-1 (methyl silicon gum) 10m x 0.54mm x 2.65 µm

n.s. n.s. (Rathore et al., 2002)

Serum 22 PCBs, 13 OH-PCBs, 9 PBDEs, 5 OH-PBDEs, 2 MeO-PBDEs

(Nomiyama et al., 2010); 50% methyl t-butyl ether/hexane; 2g

GPC, column containing activated silica gel

GC-MS analysis (HRGC/HRMS)

PCBs: 85-105%, OH-PCBs: 57-117%, PBDEs: 62-109%, OH-PBDEs: 53-111%

n.s. (Eguchi et al., 2012)

Human blood 4DDTs, 3 HCHs

Sample vials were placed in Styrofoam container with wet ice. In the laboratory blood samples were routinely spun down at 2,000 rpm and the serum was collected in separate tubes kept in freezer. Two ml of blood sample was taken and vortexed for about 20 min till RBCs were separated

Hexane and Sodium sulphate

Chemito series 2865; microprocessor controlled GC equipped with ECD having Nickel (63 Ni) foil as electron source.; Glass column (2m x 6.25 mm (1/4'') diameter

DDTs: 98.93%, HCHs: 87.69%

n.s. (Kaushik et al., 2012)

“n.s” Not stated

13

Table S9. Average concentrations (ng/L) of POPs in surface water resources in various regions of China

Sampling site in China Sampling year

DDT s (ng/L)

HCHs (ng/L)

References

Xiamen Harbor, China 1998 1.51 8.55 (Zhou et al., 2000)

Daya Bay 1999 188 285 (Zhou et al., 2001)

Shenzhen River 1994 190 220 (Yang et al., 1997)

Dasha 1994 40 150 (Yang et al., 1997)

Pearl River outlets 2006 3.89 3.69 (Guan et al., 2009)

South China Sea 2005 0.47 1.68 (Zhang et al., 2007)

Pearl River Delta (wet weather) 2009 1 3.19 (Qiao et al., 2010)

Pearl River Delta (Dry weather) 2009 0.4 1.43 (Qiao et al., 2010)

Pearl River (Wet weather) 2001 0.58 11.8 (Yang et al., 2004)

Pearl River (Dry weather) 2001 7.81 46.1 (Yang et al., 2004)

Baietang 2001 1.25 29.9 (Luo et al., 2004)

Macao Harbor 2001 18.1 17.71 (Luo et al., 2004)

Dongguan, rural pond 2007 1.46 0.81 (Zhang et al., 2011)

Shunde, rural pond 2007 0.69 0.57 (Zhang et al., 2011)

Shallow Chinese Lake 2009 11.655 16.62 (He et al., 2012)

Huaihe river, East China 2007 12.49 4.29 (Feng et al., 2011)

Baiyangdian Lake in North China 2008 11.28 6.18 (Dai et al., 2011)

Honghu Lake 2005 3.52 4.35 (Yuan et al., 2013)

Qiantang River, East China 2005 4.895 27.375 (Zhou et al., 2006)

Daliao River estuary of Liaodong Bay, Bohai Sea 2007 1.7 10.2 (Tan et al., 2009)

Beijing Guanting reservoir 2003-04 23.29 17.82 (Xue et al., 2005)

Suburb of Beijing 2006 5.213 34.2 (Chen et al., 2008)

Minjiang River Estuary 1999 142 205.5 (Zhang et al., 2003)

lower reaches of Yangtze River 2010 1.17 2.52 (Tang et al., 2013)

Taihu Lake region 2000 1307.7 5220 (Feng et al., 2003)

Tonghui River of Beijing 2002 37.17 350.03 (Zhang et al., 2004)

Jiulong River Estuary 1999 14.3 71.1 (Maskaoui et al., 2005)

Qiantang River, China 2005-06 12.32 44.46 (Zhou et al., 2008)

Yangtze River catchment of Wuhan, China 2005 1.49 6.37 (Tang et al., 2008)

Jiangsu Reach of Huaihe River 2002-03 10.59 3.13 (Wang et al., 2009)

Peacock River Drainage Basin in Xinjiang 2006 16.57 8.71 (Chen et al., 2011)

Taihu Lake, China 2010 94.86 0.97 (Wang et al., 2012)

Lake Small Baiyangdian, North China 2007 0 1.59 (Wang et al., 2013)

Jinjiang River mainstream to Quanzhou Bay 2011 3.56 14.04 (Yang et al., 2013)

Lake Chaohu 2009 5.9 2 (Liu et al., 2013)

River Wuchuan, Southeast China 2000 95.95 49.54 (Zhang et al., 2002)

Lake Chaohu, China 2010 1.91 1.76 (Liu et al., 2012)

References

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Table S10. Average concentrations (ng/g lipid wt.) of POPs in human milk samples from various regions of China

Sampling Site (China) Year DDTs HCHs References

Beijing (n=10) ng/g lipid 2007 - 485 (Fujii et al., 2012)

Beijing (n=10) ng/g lipid 2008 - 890

Central Taiwan (n=36) 2001 333 3.4 (Chao et al., 2006)

Taiwan (n=106) 1981 3595 - (Li et al., 1983)

Beijing (n= 60) 2008 1458 - (Fujii et al., 2011)

Beijing (n=25) 2007 1300 570 (Haraguchi et al., 2009)

Beijing (n=60) 1998 2040 1180 (Yu et al., 2003)

Beijing (n=59) 1993 3590 - (Yu et al., 2006)

Dalian (n=20) 2002 2100 1400 (Kunisue et al., 2004)

Shenyang (n=20) 2002 870 550

Pingqiao (n=16) 2003 1324 193.25 (Zhao et al., 2007)

Luqiao (n=5) 2005 1528 348.91

Guangzhou (n=30) 2004 2464 80.1 (Qu et al., 2010)

Hong Kong (n=316) 2001 1500 - (Hedley et al., 2010)

Hong Kong (n=26) 1999 3270 1011 (Poon et al., 2005)

Hong Kong (n=132) 1999 2900 950 (Wong et al., 2002)

Guangzhou (n=54) 2000 3600 1100

Hong Kong (n=316) 2001 - 942.4 (Hedley et al., 2006)

China (n=1237), 12 provinces 2007 527.2 231.8 (Zhou et al., 2011)

Beijing (n=40) 2006 - 310 (Yu et al., 2009)

Shenyang (n=36) 2006 - 360

Beijing 1982 - 6970 (Yu et al., 2006)

Shijiazhuang, China 2002-03 3330 109 (Sun et al., 2005)

Tangshan, China 2002-03 1916 21.2

Tianjin 2006-07 582.6 246.5 (Leng et al., 2009)

Yantai 2006-07 773.3 636.4

Beijing 2000-01 719.1 169 (Yao et al., 2005)

16

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Table S11. Average concentrations (ng/g) of POPs in biota samples from various regions of China

Sampling Site (Organism) Year DDT HCH References

Coast of Guangdong (Oyster) 1983 128 173 b

Coast of Guangdong (Oyster) 1989 26.9 8.3 (Jia et al., 1996)

Coast of Guangdong (Oyster) 1991 3.8 3.1 (Jia et al., 1996)

17

Coast of Guangdong (Oyster) 2005 4.3 0.25 (Gan et al., 2009)

Wu Kai Sha, Hong Kong(Mussel) 1983 1121 - (Phillips, 1985)

Wu Kai Sha, Hong Kong(Mussel) 2003 75 - (Liu and Kueh, 2005)

PRD, Coastal Cities (Mollusk) 2004-05 42.3 0.5 (Guo et al., 2007)

PRD, Coastal Cities (Shrimp) 2004-05 5.77 0.24 (Guo et al., 2007)

PRD, Coastal Cities (Crab) 2004-05 12.8 0.74 (Guo et al., 2007)

PRD, Coastal Cities (Fish) 2004-05 32.2 1.16 (Guo et al., 2007)

Daya Bay (Shrimp) 2003 10 0.07 (Guo et al., 2008)

Daya Bay (Crab) 2003 57 0.23 (Guo et al., 2008)

Daya Bay (Fish) 2003 231.8 0.385 (Guo et al., 2008)

PRE (Shrimp) 2004 17 0.16 (Guo et al., 2008)

PRE (Crab) 2003 111 0.6 (Guo et al., 2008)

PRE (Fish) 2004 143.9 0.965 (Guo et al., 2008)

Hong Kong (Freshwater fish) 2004 4.61 - (Cheung et al., 2007)

Hong Kong (Freshwater fish) 2009 29.3 1.22 (Wang et al., 2011)

Hong Kong (Marine fish) 2004 19.8 - (Cheung et al., 2007)

Hong Kong (Marine fish) 2009 112 1.92 (Wang et al., 2011)

Shantou harbor 2010 19.07 2.21 (Shi et al., 2013)

Haimen Bey 2010 11 2.63

Dalian 2002 32.82 1.17 (Yang et al., 2006)

Tianjin 2002 8.05 0.43

Shanghai 2002 19.83 0.5

Guangdong (Mandrin Fish) 2008 160 22 (Qiu et al., 2012)

Taihu Lake (Mandrin Fish) 2008 220 18

Liaoning Province, China 2007 18.75 1.02 (Liu et al., 2010)

Quanzhou Bay 2005 23.76 0.274 (Yatawara et al., 2010)

Xinghua Bay 2005 26.51 0.48

Yangtze River, Jiangsu area (Fish) 2004-05 0.035 0.0145 (Hu et al., 2009)

Yangtze River, Jiangsu area (benthos) 2004 0.041 0.018

Qiantang River (Fish) 2006 3721.9 1993.5 (Zhou et al., 2008)

Qiantang River (Tonglu and Hangzhou area) (Fish)

2005 13.83 3.332 (Zhou et al., 2007)

Lake Tai 2000 740 57 (Nakata et al., 2005)

Jinshan (Hangzhon Bay) 2001 1417.7 20.08

Taihu Lake (Ctenopharyngodon idellus, Megalobrama amblycephala, Cyprinus carpio, Hypophthalmichthys molitrix, Hemiculter leucisculus, Acheilognathus macropterus, Hypophthalmichthys nobilis, Saurogobio dabry, Hyporhamphus intermedius, Toxabramis swinhonis, Protosalanx hyalocranius, Neosalanx taihuensis Chen, Chanodichthys mongolicus, Chanodichthys dabry, Paracanthobrama guichenoti)

2009 255.86 20.74 (Wang et al., 2012)

bInvestigation Office for Coastal Resources in Guangdong Province, 1987

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