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Characteristics of PAHs, PCDD/Fs, PCBsand PBDEs in the Sediment of LakeBaikal, RussiaGon Ok a , Galina Shirapova b , Galina Matafonova b , Valeriy Batoevb & Seok hyung Lee aa Department of Environment Atmospheric Science, Graduate Schoolof Earth Environmental Engineering, and Dioxin Research Center,Pukyong National University, Busan, Koreab Baikal Institute of Nature Management SB RAS, Ulan-Ude, RussiaPublished online: 27 Mar 2013.

To cite this article: Gon Ok , Galina Shirapova , Galina Matafonova , Valeriy Batoev & Seok hyungLee (2013) Characteristics of PAHs, PCDD/Fs, PCBs and PBDEs in the Sediment of Lake Baikal, Russia,Polycyclic Aromatic Compounds, 33:2, 173-192, DOI: 10.1080/10406638.2013.764540

To link to this article: http://dx.doi.org/10.1080/10406638.2013.764540

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Polycyclic Aromatic Compounds, 33:173–192, 2013Copyright C© Taylor & Francis Group, LLCISSN: 1040-6638 print / 1563-5333 onlineDOI: 10.1080/10406638.2013.764540

Characteristics of PAHs,PCDD/Fs, PCBs and PBDEs in theSediment of Lake Baikal, Russia

Gon Ok,1 Galina Shirapova,2 Galina Matafonova,2

Valeriy Batoev,2 and Seok hyung Lee1

1Department of Environment Atmospheric Science, Graduate School of EarthEnvironmental Engineering, and Dioxin Research Center, Pukyong NationalUniversity, Busan, Korea2Baikal Institute of Nature Management SB RAS, Ulan-Ude, Russia

The levels of PAHs, PCDD/Fs, PCBs, and PBDEs in Lake Baikal were monitored forthe first time using deep water sediment. The sediment samples were collected from 15stations in four regions of Lake Baikal: Ol’khon Island (n = 8), the Angara River estuary(n = 2), the Selenga River delta (n = 2), and the Baikal pulp and paper mill (BPPM)(n = 3). The highest average concentrations of PCDD/Fs (20.24 pg/g d.w.) and PCBs(68.72 ng/g d.w.) were found at Ol’khon Island. The highest total PBDE concentrationswere found at BPPM, with a mean concentration of 575.76 pg/g d.w. For PCBs, PCB-52,and PCB-69 were dominant, making up 11% of the total 209 PCB congeners. BDE-209 contributed 60% of PBDEs in Lake Baikal. According to the TPEQ concentrationof PAHs, PAHs contributed the most to Lake Baikal contamination. The sources ofcontamination of PAHs, PCDDs, and PCBs in Lake Baikal are identified as combustion,runoff from the use of the pesticides (PCP) and insulating oil, specifically for PCBs. Thesource of PBDEs is assumed to be production, use and disposal of products containingPBDEs, in addition to atmospheric long-range transport and deposition.

Key Words: Dioxins, Lake Baikal, lake sediment, PAHs, PBDEs

INTRODUCTION

Lake Baikal is the deepest lake in the world and contains 20% of the unfrozenfresh water available on Earth. Designated as a UNESCO World Heritage Site,Lake Baikal is recognized for its unique ecosystem (1).

Recently, changes in ecology and abiotic variables raised awareness aboutglobal warming. Moore et al. proposed that, because of anthropogenic stresses,

Received 11 August 2012; accepted 6 January 2013.Address correspondence to Gon Ok, Department of Environment Atmospheric Science,Graduate School of Earth Environmental Engineering, and Dioxin Research Center,Pukyong National University, Nam-gu Daeyeon 3-dong 599-1, Busan 608-737, Korea.E-mail: gonok@pknu.ac.kr

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174 G. Ok et al.

the function of Lake Baikal’s ecosystem would worsen along with melting per-mafrost (2). Lake Baikal has over 300 inflow tributaries, and the only outflowtributary is the Angara River. The Selenga River, the main inflow tributary,provides 57% of water to Lake Baikal, and is known as one of the significantsources of lake pollution (3, 4). Ol’khon island is the only inhabited island inlake Baikal that is also a main tourist destination for Lake Baikal tourism. Thetourism activities in the island have shown to result in environmental impact(5).

Since then, organic pollutants were found in air, water, soil, and the Baikalseal (6–12). The Baikal pulp and paper mill (BPPM) was built directly on thesouthern shore in 1966 and is considered to be a major source of polychlo-rinated dibenzo-p-dioxin and dibenzo furan (PCDD/Fs) and polychlorinatedbiphenyl (PCB) contamination in Lake Baikal (1, 11).

In Russia, the levels of PCBs and DDT started to decrease with the re-striction of their production and use (13). However, in the past 20 years, thelevels of brominated flame retardants (BFRs) in the environment have beenincreasing in Russia, with their increasing use (14, 15).

Of particular note is a study that used the Baikal seal as an indicator ofthe significance of polybrominated diphenyl ether (PBDE) contamination inLake Baikal (16, 17). PBDEs are an emerging POP that is commonly used inpaint, textiles, and electronic devices. Recent studies suggest the severe tox-icity of PBDEs. Studies with mice exposed to PBDEs indicated that PBDEscause learning and motor disabilities, and that such deficits become more seri-ous as the animals grow older (18, 19).

Polycyclic aromatic hydrocarbons (PAHs) are unintentionally producedPOPs that can be released into the environment during human activities suchas during industrial combustion (20). Like dioxins and PCBs, PAHs are car-cinogenic and cause development of benign and malignant tumors in experi-mental animals (20). In order to protect the habitats of Lake Baikal and resi-dents of the area who are using lake water as their water source, this study ofPOPs in Lake Baikal is significant. So far, there are a limited number of studieson POPs in Lake Baikal and its basin using sediments as an analytical matrix,and there is no study as of yet on POPs in the deep-water sediments of LakeBaikal (1, 7). In the present work, the contamination levels and the sources ofPCDD/Fs, PCBs, and PAHs in the Lake Baikal ecosystem were monitored, forthe first time, using deep-water sediments. These newly obtained data couldserve as a basis for assessment of sources of Lake Baikal pollution and providea record of pollution.

MATERIALS AND METHODS

Sample CollectionThe sediment samples were collected from 15 stations in four regions of

Lake Baikal: Ol’khon Island (n = 8), the Angara River estuary (n = 2), the

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PAHs, PCDD/Fs, PCBs and PBDEs Contamination in Lake Baikal 175

Figure 1: Sampling station at Lake Baikal.

Selenga River delta (n = 2), and near the Baikal pulp and paper mill (BPPM)(n = 3). The samplings stations, diving depths, and their specific locations areshown in Figure 1. All the samples were collected by two manned submersibles,“Mir” (the P.P. Shirshov Institute of Oceanology of the Russian Academy ofSciences) during the first international expedition in 2008.

Sample Extraction and PretreatmentSediment samples were freeze dried and organic compounds were ex-

tracted for 16 h with toluene using the Soxhlet extraction method.For the analysis of PCDD/Fs, a labeled and internal standard (EPA-1613,

LCS, and EPA-1613 ISS, Wellington Laboratories Inc., Canada) was used. Theextracts were cleaned using a multilayered silica gel column consisting of 2 gof anhydrous sodium sulfate, 0.6 g of silica gel, 3 g of 2% KOH, 0.6 g of silicagel, 4 g of 44% H2SO4, 4 g of 22% H2SO4, 0.6 g of silica gel, 2 g of 10% AgNO3,and 2 g of anhydrous sodium sulfate. The eluate used was 160 mL of n-hexane.The eluent was then cleaned again using an activated alumina column chro-matograph loaded with 10 g of alumina activated at 600◦C for 24 hours. Theelution was held with 70 mL of 3% dichloromethane in n-hexane for the firstfraction, and in 80 mL of 50% dichloromethane in n-hexane, for the secondfraction.

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176 G. Ok et al.

For the dioxin like-PCBs (DL-PCBs) analysis, the samples were spikedwith a labeled standard (68A-LCS, Wellington Laboratories Inc.) and an inter-nal standard (68A-IS, Wellington Laboratories Inc.). The samples were thencleaned with a multilayered silica gel column layered the same way as thatused for cleaning for the analysis of dioxins. For the analysis of the 209 PCBcongeners, a standard solution M-1668A-1-5-0.01X (Accu Standard, USA) wasused (21–25).

The samples used for PAH analyses were spiked with the labeled stan-dard solutions (ES-2528, CIL, Inc., USA). For cleaning, an activated silica gelcolumn chromatograph (70–230 mesh, neutral, Merck) filled with silica gel ac-tivated at 600◦C for 2 h was used. For the first and second fractions, 10 mLof n-hexane and 100 mL of 10% dichloromethane in n-hexane were used aseluents, respectively (25, 26). The elution from the second fraction was con-centrated for the instrumental analysis. For the analyses of PBDEs, the la-beled and internal standard solutions (BFR-LCS, Wellington, and BFR-ISS,Wellington Laboratories Inc.) were spiked, and cleaned with a multilayeredsilica gel column in common with the pretreatment of PCDD/Fs. The eluateused for cleaning PBDEs was a 120 mL solution of 10% dichloromethane inn-hexane (24).

Instrumental AnalysisThe instrumental analyses of PCDD/Fs and PCBs were conducted using

high-resolution gas chromatography (6890N GC, Agilent, USA) and mass spec-trometry (JMS-700D, JEOL, Japan). The instrumental conditions for the anal-yses of PCDD/Fs and PCBs were as detailed in Ok et al. (24). In the caseof PAHs, high-resolution gas chromatography and mass spectrometry (6890NHRGC/MSD, Agilent, USA) were used (25, 26). The instrumental conditionsfor PAH analysis were set as suggested by Kim et al. (26).

RESULTS AND DISCUSSION

Persistent Organic Pollutants—PCDD/Fs, PCBs, DL-PCBs, PBDEsAmong the four sampling regions, Ol’khon Island had the highest total

PCDD/DF homolog concentrations, with a mean concentration of 20.3 pg/g d.w.,a minimum concentration of 9.6 pg/g d.w., and a maximum concentration of50.2 pg/g d.w (Table 1). The highest total toxicity equivalent (TEQ) concen-tration was also found at Ol’khon Island with a mean concentration of 0.35pg–WHO98TEQ/g d.w, and a range of 0.10–0.90 pg–WHO98TEQ/g d.w. Com-pared with sediments from Saginaw Bay (86.2 pg/g d.w.) and Spanish River

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Tab

le1:

Co

nc

en

tra

tion

(pg

WH

O98

-TEQ

/g.d

.w)

of

PC

DD

/DFs

an

dP

CBs

inLa

keBa

ika

lse

dim

en

ts

Isla

nd

Olk

ho

n(n

=8)

Sele

ng

ariv

erd

elta

(n=

2)A

ng

ara

rive

rest

ua

ry(n

=2)

BPP

M(n

=3)

Me

an±S

DR

an

ge

Me

an±S

DR

an

ge

Me

an±S

DR

an

ge

Me

an±S

DR

an

ge

PCD

Ds

2,3,

7,8,

-T4C

DD

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

0.01

0±

0.01

80.

0001

–0.0

311,

2,3,

7,8-

P5C

DD

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

1,2,

3,4,

7,8-

H6C

DD

0.00

4±

0.01

10.

0001

–0.0

31<

0.00

01<

0.00

01<

0.00

01<

0.00

010.

001

±0.

003

0.00

01–0

.004

1,2,

3,6,

7,8-

H6C

DD

0.00

6±

0.01

80.

0001

–0.0

51<

0.00

01<

0.00

01<

0.00

01<

0.00

010.

003±

0.00

50.

0001

–0.0

091,

2,3,

7,8,

9-H

6CD

D0.

008

±0.

017

0.00

01–0

.050

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

1,2,

3,4,

6,7,

8-H

7CD

D0.

025

±0.

011

0.01

1–0.

045

0.01

8±

0.01

20.

009–

0.02

60.

013

±0.

005

0.01

0–0.

017

0.03

0±

0.01

60.

017–

0.04

8O

CD

D0.

002

±0.

002

0.00

1–0.

008

<0.

0001

0.00

02–0

.000

70.

0004

±0.

000

0.00

04–0

.000

40.

0007

±0.

0002

0.00

05–0

.001

PCD

Fs2,

3,7,

8-T4

DF

0.00

4±

0.00

90.

0001

–0.0

260.

003

±0.

004

0.00

01–0

.006

0.01

1±

0.00

10.

010–

0.01

20.

042

±0.

034

0.00

4–0.

071

1,2,

3,7,

8-P

5CD

F0.

004

±0.

005

0.00

01–0

.015

0.00

01±

0.00

10.

0001

–0.0

010.

003

±0.

001

0.00

3–0.

004

0.00

1±

0.00

10.

0001

–0.0

022,

3,4,

7,8-

P5C

DF

0.05

7±

0.07

10.

0001

–0.2

010.

005

±0.

007

0.00

01–0

.010

0.01

3±

0.01

80.

0001

–0.0

25<

0.00

01<

0.00

011,

2,3,

4,7,

8-H

6CD

F0.

004

±0.

009

0.00

01–0

.025

<0.

0001

<0.

0001

0.00

7±

0.00

40.

004–

0.01

1<

0.00

01<

0.00

011,

2,3,

6,7,

8-H

6CD

F0.

005

±0.

009

0.00

01–0

.027

<0.

0001

<0.

0001

0.00

8±

0.00

50.

005–

0.01

1<

0.00

01<

0.00

011,

2,3,

7,8,

9-H

6CD

F<

0.00

01<

0.00

01<

0.00

01<

0.00

010.

001

±0.

002

0.00

01–0

.003

<0.

0001

<0.

0001

2,3,

4,6,

7,8-

H6C

DF

0.00

01±

0.00

10.

0001

–0.0

02<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

011,

2,3,

4,6,

7,8-

H7C

DF

0.00

4±

0.00

70.

0001

–0.0

190.

001

±0.

001

0.00

0–0.

002

0.00

2±0.

001

0.00

1–0.

003

0.00

1±

0.00

10.

001–

0.00

21,

2,3,

4,7,

8,9-

H7C

DF

0.00

1±

0.00

20.

0001

–0.0

05<

0.00

01<

0.00

010.

0003

±0.

0001

0.00

03–0

.000

4<

0.00

01<

0.00

01O

CD

F0.

0001

±0.

0001

0.00

01–0

.000

2<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01N

on-

ort

hoPC

Bs3,

3’,4

,4’-

T4C

B(#

77)

0.00

2±

0.00

10.

001–

0.00

40.

001

±0.

0001

0.00

1–0.

001

0.00

1±

0.00

010.

001–

0.00

10.

003

±0.

001

0.00

2–0.

004

3,4,

4’.5

-T4C

B(#

81)

0.00

3±

0.00

10.

001–

0.00

40.

001

±0.

0001

0.00

1–0.

001

0.00

1±

0.00

010.

001–

0.00

10.

003

±0.

001

0.00

2–0.

004

3,3’

,4,4

’,5-

P5C

B(#

126)

0.09

1±

0.08

90.

0001

–0.2

690.

038

±0.

021

0.02

3–0.

053

0.06

4±

0.01

40.

054–

0.07

4<

0.00

01<

0.00

01

3,3’

,4,4

’,5,

5’-H

6CB

(#16

9)0.

019

±0.

019

0.00

01–0

.058

0.00

5±

0.00

50.

002–

0.00

80.

010

±0.

005

0.00

6–0.

014

0.00

5±

0.00

50.

0001

–0.0

10

Mo

no-o

rtho

PCBs

2,3,

3’,4

,4’-

P5C

B(#

105)

0.01

9±

0.00

90.

011–

0.03

50.

010

±0.

001

0.01

0–0.

011

0.01

0±

0.00

10.

009–

0.01

00.

022

±0.

011

0.01

3–0.

033

2,3,

4,4’

,5-P

5CB

(#11

4)0.

011

±0.

006

0.00

4–0.

019

0.00

6±

0.00

10.

005–

0.00

70.

006

±0.

003

0.00

4–0.

009

0.01

2±

0.00

70.

006–

0.02

0

2,3’

,4,4

’,5-

P5C

B(#

118)

0.08

7±

0.07

60.

036–

0.26

20.

035

±0.

001

0.03

4–0.

036

0.03

0±

0.00

50.

026–

0.03

30.

069

±0.

033

0.04

1–0.

105

2’,3

,4,4

’,5-

P5C

B(#

123)

0.00

1±

0.00

10.

0001

–0.0

020.

0001

±0.

0001

0.00

01–0

.000

10.

0001

±0 .

0001

0.00

01–0

.000

10.

001

±0.

001

0.00

1–0.

002

2,3,

3’,4

,4’,

5-H

6CB

(#15

6)0.

006

±0.

004

0.00

3–0.

013

0.00

3±

0.00

010.

003–

0.00

30.

003

±0.

001

0.00

2–0.

003

0.00

7±

0.00

50.

003–

0.01

3

2,3,

3’,4

,4’,

5’-H

6CB

(#15

7)0.

001

±0.

001

0.00

1–0.

003

0.00

01±

0.00

010.

0001

–0.0

001

0.00

1±

0.00

010.

0001

–0.0

010.

001

±0.

001

0.00

01–0

.003

(Co

ntin

ue

do

nn

ext

pa

ge

)

177

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Tab

le1:

Co

nc

en

tra

tion

(pg

WH

O98

-TEQ

/g.d

.w)

of

PC

DD

/DFs

an

dP

CBs

inLa

keBa

ika

lse

dim

en

ts(C

on

tinu

ed

)

Isla

nd

Olk

ho

n(n

=8)

Sele

ng

ariv

erd

elta

(n=

2)A

ng

ara

rive

rest

ua

ry(n

=2)

BPP

M(n

=3)

Me

an±S

DR

an

ge

Me

an±S

DR

an

ge

Me

an±S

DR

an

ge

Me

an±S

DR

an

ge

2,3′ ,4

,4′ ,5

,5′ -H

6CB

(#16

7)0.

003

±0.

008

0.00

01–0

.022

0.00

01±

0.00

010.

0001

–0.0

001

0.00

01±

0.00

010.

0001

–0.0

001

0.00

01±

0.00

010.

0001

–0.0

001

2,3,

3’,4

,4’,

5,5’

-H7C

B(#

189)

0.00

01±

0.00

010.

0001

–0.0

001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

Ho

mo

log

T4C

DD

0.39

7±

0.63

90.

0001

–1.9

550.

411

±0.

298

0.20

0–0.

621

0.44

6±

0.01

60.

435–

0.45

80.

231

±0.

147

0.10

9–0.

394

P5C

DD

<0.

0001

<0.

0001

0.06

4±

0.09

00.

0001

–0.1

270.

249

±0.

076

0.19

6–0.

303

<0.

0001

<0.

0001

H6C

DD

0.61

3±

1.20

40.

0001

–3.5

540.

506

±0.

715

0.00

01–1

.011

0.93

7±

0.68

10.

455–

1.41

80.

450

±0.

398

0.00

01–0

.755

H7C

DD

4.21

8±

2.13

81.

921–

8.24

32.

990

±1.

914

1.63

7–4.

344

2.54

4±

1.07

81.

782–

3.30

64.

515

±2.

310

2.73

4–7.

126

OC

DD

11.4

13±

8.97

95.

192–

29.7

484.

598

±2.

996

2.47

9–6.

716

4.05

6±

0.30

83.

838–

4.27

46.

513

±2.

096

4.58

3–8.

743

Tota

lPC

DD

s16

.641

±12

.565

7.79

4–43

.499

8.56

8±

5.41

84.

737–

12.3

998.

232

±2.

159

6.70

6–9.

759

11.7

09±

4.66

77.

507–

16.7

31T4

CD

F1.

596

±1.

738

0.00

01–5

.133

0.54

9±

0.77

60.

0001

–1.0

971.

711

±0.

699

1.21

7–2.

205

2.01

0±

1.21

90.

688–

3.09

1P

5CD

F0.

605

±0.

723

0.00

01–2

.194

0.07

5±

0.10

60.

0001

–0.1

500.

621

±0.

387

0.34

8–0.

895

0.24

1±

0.28

60.

000–

0.55

7H

6CD

F0.

199

±0 .

390

0.00

01–1

.128

<0.

0001

<0.

0001

0.36

8±

0.33

40.

132–

0.60

4<

0.00

01<

0.00

01H

7CD

F0.

632

±1.

023

0.00

01–3

.061

0.10

7±

0.15

10.

0001

–0.2

130.

291

±0.

160

0.17

7–0.

404

0.14

5±

0.07

20.

063–

0.19

7O

CD

F0.

575

±0.

626

0.00

01–1

.666

0.25

7±

0.20

90.

109–

0.40

50.

103

±0.

146

0.00

01–0

.206

0.10

2±

0.08

90.

0001

–0.1

63To

talP

CD

Fs3.

607

±4.

250

0.42

6–12

.922

0.98

8±

0.82

40.

405–

1.57

03.

094

±1.

726

1.87

4–4.

314

2.49

8±

1.63

30.

752–

3.98

7To

tal

PC

DD

/DFs

(pg

/g.d

.w)20.2

48±

15.8

689.

259–

50.1

959.

556

±6.

241

5.14

3–13

.969

11.3

27±

0.43

411

.020

–11.

633

14.2

07±

3.65

610

.263

–17.

483

Mo

no

-CBs

0.00

2±

0.01

0.00

01–0

.02

0.00

3±

0.00

40.

0001

–0.0

1<

0.00

01<

0.00

010.

005

±0.

008

0.00

01–0

.01

Di-C

Bs5.

09±

3.46

1.56

–12.

975.

34±

1.25

4.46

–6.2

33.

11±

2.52

1.33

–4.8

94.

97±

1.88

3.74

–7.1

3Tr

i-CBs

17.6

5±

6.81

12.1

2–29

.84

12.4

1±

1.92

11.0

6–13

.77

6.16

±3.

613.

61–8

.71

15.4

0±

5.43

12.1

4–21

.66

Tetr

a-C

Bs27

.59

±12

.01

16.8

3–49

.72

19.0

0±

4 .53

15.7

9–22

.20

11.9

7±

5.55

8.05

–15.

8925

.99

±8.

6519

.82–

35.8

9Pe

nta

-CBs

14.7

9±

6.86

9.66

–28.

319.

32±

2.68

7.43

–11.

214.

94±

1.98

3.54

–6.3

410

.93

±4.

985.

77–1

5.71

He

xa-C

Bs3.

27±

1.83

1.44

–6.7

42.

33±

0.91

1.69

–2.9

71.

08±

0.01

1.07

–1.0

92.

40±

1.39

1.15

–3.9

0H

ep

ta-C

Bs0.

32±

0.19

0.17

–0.6

40.

18±

0.06

0.14

–0.2

20.

13±

0.00

10.

13–0

.13

0.29

±0.

170.

16-0

.48

Oc

ta-C

Bs<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01N

on

a-C

Bs<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01D

ec

a-C

Bs0.

01±

0.01

0.00

01–0

.02

<0.

0001

<0.

0001

0.00

3±

0.00

50.

0001

–0.0

1<

0.00

01<

0.00

01To

tal

PC

Bs(n

g/g

.d.w

)68

.72

±28

.66

43.3

5–11

6.83

48.5

8±

11.3

440

.56–

56.6

027

.38

±13

.63

17.7

5–37

.02

59.9

9±

21.9

543

.04–

84.7

8

WH

O98

TEQ

PC

DD

s0.

045

±0.

056

0.01

4–0.

180

0.01

8±

0.01

20.

010–

0.02

60.

014

±0.

005

0.01

0–0.

017

0.04

6±

0.02

60.

018–

0.07

0P

CD

Fs0.

080

±0.

087

0.00

01–0

.224

0.00

9±

0.01

30.

0001

–0.0

190.

046

±0.

003

0.04

4–0.

049

0.04

4±

0.03

50.

005–

0.07

3N

on

-ort

ho

PC

Bs0.

115

±0.

096

0.00

3–0.

312

0.04

5±

0.02

60.

027–

0.06

40.

077

±0.

019

0.06

3–0.

090

0.01

0±

0.00

70.

005–

0.01

8M

on

o-o

rth

oP

CBs

0.12

9±

0.09

10.

059–

0.32

30.

055

±0.

003

0.05

3–0.

058

0.04

9±

0.00

70.

044–

0.05

40.

112

±0.

057

0.06

3–0.

175

Tota

lTEQ

(pg

-WH

O98

TEQ

/g.d

.w)

0.34

90±

0.26

420.

1019

–0.8

976

0.15

72±

0.04

370.

1263

–0.1

297

0.18

56±

0.00

350.

1831

–0.1

881

0.23

75±

0.19

450.

0813

–0.4

554

178

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PAHs, PCDD/Fs, PCBs and PBDEs Contamination in Lake Baikal 179

Figure 2: Homolog concentration of PCDD/Fs in Lake Baikal sediment.

(79.6 pg/g d.w.) in Lake Huron, and Na-PCP-contaminated Dongting Lake sed-iment, where I-TEQ concentration was 11 pg I–TEQ/g d.w., dioxin levels inLake Baikal sediments were considerably lower (27, 28).

The PCDD/DF levels in Lake Baikal are similar to levels found in sedi-ments of a rural lake in Finland (35 pg/g d.w.) (29). In this study, the sum ofPCDD concentrations was higher than those of PCDFs, and highly chlorinatedcompounds such as OCDD were dominant. OCDD contributed 52% of the to-tal concentration (Figure 2). The dominance of OCDD have been reported invarious lake sediments such as Lake Huron and Lake Superior (27). The highcontribution (56–91%) of OCDD was observed in sediments of Nanpaiwu Riverand Bohai Bay in China, the areas with serious PCP contamination (30). Basedon various studies conducted present study and the others, the dominance ofOCDDs in Lake Baikal sediment is assumed to be caused by the use of pesti-cides, such as PCP (27, 30).

Overall, the profile of 2,3,7,8-substances showed the dominance of1,2,3,4,6,7,8-HpCDDs among the PCDDs, and 2,3,4,7,8-PeCDFs among PCDFs(Figure 3). The highest PCDF contribution was found at the Angara Riverhead (sites K and L). Such a pattern is similar to the pattern of dioxins ob-served in the soils of the cities of Irkutsk, Angarsk, and Usol’ye, areas in whichthe Angara River flows through. Generally, the dominance of 2,3,4,7,8-PeCDFis observed during combustion processes. The fly ash from the combustion ofbagasse have shown the dominance of 2,3,4,7,8-PeCDF (31). Based on theseresults, the main sources of dioxins at Ol’khon Island, the Angara River head,and the Selenga River delta are assumed to be runoff from soil contaminatedby PCP and the air deposition from combustion and open burning of wasteresidues.

As shown in Table 1, the total concentration of the 209 PCB congenersranged from 17.8–116.8 ng/g d.w. The regional trend in the 209 PCB congeners

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180 G. Ok et al.

Figure 3: Profile pattern of 2,3,7,8- substances in Lake Baikal sediment.

was as follows: Ol’khon Island (68.7 ng/g d.w.) > BPPM (60.0 ng/g d.w.) > Se-lenga River delta (48.6 ng/g d.w.) > Angara River head (27.4 ng/g d.w.).

The total PCB levels at Ol’khon Island were around twice higher thanthose in eastern Lake Erie (36 ng/g). The levels at Lake Baikal were con-siderably lower than those at central Lake Erie (100 ng/g) and Lake Ontario(100 ng/g) (31). Compared with Lake Michigan where the total PCBs levelswere 7400 ng/g d.w., Lake Baikal sediments were significantly lower and didnot exceed Canadian sediment quality guidelines (34, 35).

Among the 209 PCB congeners, PCB-52 and PCB-69 were dominant, com-prising 11% of the total 209 PCB congeners. Furthermore, PCB-5, PCB-8, PCB-28, PCB-32, and PCB-70 comprised a further 5–6% of the total concentration.The TEQ concentrations of PCB-126 among the non-ortho-PCBs, and PCB-118among the mono-ortho-PCBs prevailed (Figure 4). Such a pattern is similarto those observed in the Baikal seal and in Sovol, the commercial mixture ofPCBs (36, 37). In Sovol, the predominant PCB congeners are PCB-77 (non-ortho-PCBs); PCB-105, PCB-118, PCB-156 (mono-ortho-PCBs), and PCB-95,PCB-101, PCB-110, PCB-138, and PCB-153 (non-DL PCBs). The contributionfrom Sovol to DL-PCB contamination of Lake Baikal was assumed based onthe 0.0038% DL-PCBs content present in Sovol (37). The profile pattern ofPCBs without the application of TEF in both Lake Baikal sediments and Sovolshowed the dominance of PCB-118 and PCB-105. In Lake Baikal sediments,tetra-PCBs made the highest contribution. Among di-PCBs, PCB-5 and PCB-8made up 6% of the total PCBs. When observing the overall contribution of thePCB congeners in this study, the trends were similar to the patterns observedfor Aroclor 1221 and 1248 and Clophen A-30 and A-40 (Figure 5) (37). Based onthe results of this study and the previous study completed by Takasuga et al.,it is possible to suggest that Sovol plays a major role as one of the sources ofPCB contaminations in Lake Baikal in addition to other sources of PCBs, such

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PAHs, PCDD/Fs, PCBs and PBDEs Contamination in Lake Baikal 181

Figure 4: WHO-TEQ concentration of DL-PCBs in Lake Baikal sediment.

as technical PCB mixture compounds (37). Overall, 60% of contamination inLake Baikal is contributed by DL-PCBs, and the contributions of dioxins andDL-PCBs were in the following order: DL-PCBs > PCDFs > PCDDs (Figure 6).

Since the mid-1980s, PBDEs have been pointed out as one of the ubiqui-tous environmental contaminants. With the banning of PBDE marketing andthe use of PentaBDE and OctaBDE throughout the European Union countries

Figure 5: Contribution ratio of DL-PCB congeners (without the application of ToxicEquivalency Factor) in Lake Baikal (this study) and Sovol (37).

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182 G. Ok et al.

Figure 6: Contribution ratio of PCDD/Fs and DL-PCBs.

in 2004, PBDE levels in Europe are expected to decrease (38). Even so, theconcentration of PBDEs is rapidly increasing in Arctic biota, and this patternis expected to continue in the near future. The production of the commercialformulation PentaBDE mix, which is continuously being produced in over 95%of North America is known to have a great impact on long-range atmospherictransportation (14).

The results of the PBDE analyses on sediment from four regions in LakeBaikal are shown in Table 2. The average concentration of the sum of 40 PB-DEs was highest at BPPM (575.8 pg/g d.w.), around 2.5-fold lower than for thesediments of Lake Superior (1.4 ng/g d.w.), and significantly higher than forthe sediments of Verbania R. Toce, Italy (0.060 ng/g d.w.) (39, 40).

In Lake Baikal, 60% of the PBDEs are contributed by BDE-209 with amean concentration of 0.22 pg/g d.w. PBDE-47 and BDE-99 contributed 11%and 10%, respectively. The dominance of DecaBDE was also observed in otherstudies; in the Lake Maggiore basin of Italy and Switzerland, DecaBDE com-prised 97% of the sum PBDEs because of the use of the DecaBDE formulation,and it comprised 80% of the sum of BDEs in the Elbe River (41–43). Based onthis result, it is possible to assume that the PBDE chemical that contaminatesLake Baikal is brominated Deca-BDE. 90% of Deca-brominated chemicals areknown to comprise BDE-209 (44).

Generally, the sources of PBDEs are production and use of residential elec-tronic devices in big cities and industrial areas. Therefore, the concentrationof PBDEs was expected to be higher in the areas of Lake Baikal that are closeto the big cities. Other than some contribution of industrial use of electronicsand machine at the Paper Mill, the exact source of PBDE in Lake Baikal couldnot be explained in present study.

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Tab

le2:

Co

nc

en

tra

tion

(pg

/g.d

.w.)

of

PBD

Esin

Lake

Baik

als

ed

ime

nts

Isla

nd

Olk

ho

n(n

=8)

BPP

M(n

=3)

Sele

ng

ariv

er

An

ga

raR

ive

rM

ea

n±S

DR

an

ge

de

lta(n

=1)

est

ua

ry(n

=1)

Me

an±S

DR

an

ge

PBD

EsBD

E-1

2.54

±6.

730.

0001

–7.8

1<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-2

5.30

±5.

830.

0001

–14.

34<

0.00

01<

0.00

014.

92±

8.52

0.00

01–1

4.76

BDE-

36.

82±

6.18

0.00

01–1

5.96

<0.

0001

<0.

0001

4.05

±7.

010.

0001

–12.

14BD

E-7

3.39

±1.

641.

68–5

.78

1.17

2.16

2.90

±1.

411.

85–4

.50

BDE-

10<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-15

7.25

±3.

264.

46–1

2.27

3.94

3.34

5.37

±2.

084.

02–7

.77

BDE-

171.

51±

1.02

0.00

01–3

.08

0.37

1.42

1.07

±1.

120.

0001

–2.2

3BD

E-28

4.14

±2.

900.

0001

–8.9

22.

583.

633.

19±

1.12

2.34

–4.4

6BD

E-30

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

<0.

0001

BDE-

4739

. 53

±14

.88

23.4

1–66

.54

50.3

167

.28

31.9

3±

13.1

917

.00–

42.0

2BD

E-49

3.63

±2.

731.

75–9

.66

2.72

2.63

2.11

±0.

601.

64–2

.79

BDE-

663.

23±

2.24

0.00

01–6

.24

1.60

<0.

0001

1.39

±1.

200.

0001

–2.1

6BD

E-71

0.44

±0.

630.

0001

–1.4

9<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-77

1.63

±2.

540.

0001

–7.2

1<

0 .00

01<

0.00

01<

0.00

01<

0.00

01BD

E-85

0.83

±2.

200.

0001

–5.8

1<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-99

36.7

5±

15.4

120

.47–

56.7

330

.20

91.6

622

.71

±8.

8612

.74–

29.6

9BD

E-10

08.

05±

3.38

3.74

–12.

705.

9217

.82

3.87

±3.

410.

0001

–6.4

2BD

E-11

90.

33±

0.88

0.00

01–2

.32

<0.

0001

<0.

0001

<0.

0001

<0.

0001

BDE-

126

1.10

±2.

910.

0001

–7.7

1<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-13

8<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-13

9<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-14

0<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-15

31.

54±

2.43

0.00

01–6

. 49

1.12

9.96

1.78

±1.

540.

0001

–2.6

7BD

E-15

42.

14±

2.78

0.00

01–6

.55

4.24

8.83

3.49

±1.

142.

26–4

.51

BDE-

169

0.08

±0.

200.

0001

–0.5

3<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-17

10.

04±

0.09

0.00

01–0

.25

<0.

0001

<0.

0001

<0.

0001

<0.

0001

BDE-

180

0.11

±0.

280.

0001

–0.7

5<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-18

30.

33±

0.60

0.00

01–1

.55

<0.

0001

<0.

0001

0.70

±1.

210.

0001

–2.1

0BD

E-18

40.

06±

0.17

0.00

01–0

.44

<0.

0001

<0.

0001

<0.

0001

<0.

0001

(Co

ntin

ue

do

nn

ext

pa

ge

)

183

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Tab

le2:

Co

nc

en

tra

tion

(pg

/g.d

.w.)

of

PBD

Esin

Lake

Baik

als

ed

ime

nts

(Co

ntin

ue

d)

Isla

nd

Olk

ho

n(n

=8)

BPP

M(n

=3)

Sele

ng

ariv

er

An

ga

raR

ive

rM

ea

n±S

DR

an

ge

de

lta(n

=1)

est

ua

ry(n

=1)

Me

an±S

DR

an

ge

BDE-

191

0.10

±0.

260.

0001

–0.6

8<

0.00

01<

0.00

01<

0.00

01<

0.00

01BD

E-19

60.

34±

0.66

0.00

01–1

.75

1.36

<0.

0001

1.65

±2.

850.

0001

–4.9

4BD

E-19

70.

17±

0.29

0.00

01–0

.62

<0.

0001

<0.

0001

0.54

±0.

940.

0001

–1.6

3BD

E-20

10.

17±

0.44

0.00

01–1

.17

<0.

0001

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0001

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30.

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0.59

0.00

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.56

1.34

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0001

1.22

±2.

110.

0001

–3.6

6BD

E-20

40.

17±

0.44

0.00

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.17

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0001

<0.

0001

1.46

±2.

530.

0001

–4.3

8BD

E-20

50.

17±

0.46

0.00

01–1

.21

<0.

0001

<0.

0001

<0.

0001

<0.

0001

BDE-

206

4.38

±10

.32

0.00

01–2

7.63

<0.

0001

18.9

325

.89

±44

.85

0.00

01–7

7.68

BDE-

207

2.87

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710.

0001

–17.

98<

0.00

0115

.64

22.3

0±

38.6

20.

0001

–66.

89BD

E-20

82.

31±

6.11

0.00

01–1

6.15

<0.

0001

0.00

13.4

6±

23.3

20.

0001

–40.

38BD

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916

0.88

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0–43

8.28

125.

1218

8.32

418.

30±

399.

9711

3.84

–871

.28

Tota

lPBD

Es30

2.59

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2.77

163.

88–6

95.7

423

2.01

431.

6457

5.76

±51

2.93

181.

16–1

155.

58

184

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PAHs, PCDD/Fs, PCBs and PBDEs Contamination in Lake Baikal 185

Table 3: Concentration of PAHs in sediments from various lakes worldwide

Lake PAHs (ng/g.d.w) Reference

Baikal Lake 219.81∼1255.56 This studyLaja Lake (Chile) 226 (45)Galletue Lake (Chile) 279 (45)Icalma Lake (Chile) 3182 (45)Larto Lake (rural LA, USA) 100 (46)Lake in Adirondack region (USA) 2500–4000 (47)Lake located at northern Great Lakes (USA) 300–1800 (47)Lake in northern Florida (USA) 750–1450 (47)Lake in northern New England (USA) 2000–2800 (47)

PAHsThe concentration of total PAHs (16 compounds) in Lake Baikal deep-water

sediments ranged from 219.8–1255.6 ng/g, with a mean of 452.2 ng/g. The aver-age concentration of total PAHs was highest at site G. The average concentra-tion of total PAHs at site H and site O were 876.7 and 501.8 ng/g, respectively.

Compared with other studies on PAHs in major lakes worldwide, PAH con-centrations in Lake Baikal sediments were about twice that in Laja Lake andGalletue Lake in Chile, and within a similar range with a lake located inthe northern Great Lakes in USA (Table 3) (45, 47). When the contributionof PAH compounds were compared by the number of rings, the dominanceof the two-ringed compound (naphthalene) and the three-ringed compound(phenanthrene) were 35% and 34.7%, respectively. The high contribution ofnaphthalene and phenanthrene is assumed to be caused by agricultural andindustrial activities from nearby areas, since dominance of naphthalene andphenanthrene is often observed after open backyard burning (48). Further-more, PAHs in sediments often consist of higher molecular weight compoundsrather than lower molecular weight compounds (48). However, in Lake Baikalsediments, the contribution of low molecular weight compounds was higherthan that of the high weight molecular compounds (Figure 7a). Such a patternin Lake Baikal sediments is similar to the trend commonly observed duringlow-temperature combustions, such as in open-burning incinerators (45).

Figure 7: Concentration and profile pattern of total PAHs in (a) PAHs-TPEQ, (b) PAHs-dioxinTEQ, and (c) Lake Baikal sediment.

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186 G. Ok et al.

In the present study, the relative carcinogenicity of PAHs has also beenevaluated based on the toxic potency equivalency factor (TPEF) (49–52). Fur-thermore, the relative toxic equivalency factor (TEF) of PAHs was also sug-gested based on 2,3,7,8-Tetrachlorodibenzo-p-dioxin(TCDD) (52).

The toxicity of PAHs, toxic potency equivalent quantity (TPEQ) in LakeBaikal sediment was assessed using the TPEF suggested by Malcom andDobson (51). PAHs-TPEQ in Lake Baikal sediment ranged from 0.4–7.9 ngPAHs-TPEQ/g, with an average of 2.3 ng PAHs-TPEQ/g.

Overall, PAHs-TPEQ concentrations were high at sites G, H, andO, and the dominant compounds with the application of TPEQ weredibenz(a,h)anthracene and benzo(a)pyrene (Figure 7b). With the application ofthe relative toxic equivalency factors suggested by Klimm et al., PAHs-dioxinTEQ ranged from 2.0–56.0 pg PAHs-dioxin TEQ/g, with a mean of 16.0 pg PAHs-dioxin TEQ/g (53). Furthermore, the concentration of PAHs-dioxin TEQ showeda similar pattern to the total PAHs and PAHs-TPEQ (Figure 7c). The concen-tration of PAHs-dioxin TEQ was also highest at sites G and O, similar to thePAHs-TPEQ value.

With the application of toxic potency, PAHs contribute the most to LakeBaikal contamination compared to PCDD/Fs and DL-PCBs (Figure 8). Thus,the importance of assessing total toxicity and the risk of compound mixturesin the lake sediment is suggested (54).

For additional source identification, diagnostic analyses that use the ratioof certain PAH compounds were conducted. The ratios of AnT to PhA and FluA

Figure 8: Toxic Potency of PCDD/Fs, DL-PCBs and PAHs-dioxin TEQ in Lake Baikal sediment.

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PAHs, PCDD/Fs, PCBs and PBDEs Contamination in Lake Baikal 187

Figure 9: Diagnostic analysis of PAHs source identification.

to FluA+Pyr in all areas were over 0.1 and below 0.4, respectively. Since theratio of InP/(InP+BghiP) was over 0.5, it is reasonable to assume that thesources of PAH contamination in Lake Baikal are the combustion of fossil fuels,lumber and grassland (Figure 9).

Principal Components Analysis (PCA)For clear source identification, principal components analysis was used.

As seen in Figure 10a, DL-PCBs, PCBs, dioxins, and PAHs share the samesource of pollution, such as industrial combustion and runoff of PCP from in-dustrial areas. However, pollution from PBDEs has its own origin. As a sourceof PBDE contamination in Lake Baikal sediment, the uses and production ofPBDE-containing products are suggested. Generally, certain PBDE congeners

Figure 10: Principal Component Analysis (PCA) plot of (a) PCDD/Fs, PCBs, DL-PCBs, PBDEs.and dioxins and (b) 40 PBDE congeners.

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188 G. Ok et al.

are added to certain products. For example, PentaBDE is often used in mat-tresses and carpets, OctaBDE is often used in radio and ABS plastics, whileDecaBDE is contained in microelectronic trays. However, the exact type ofproduct that may cause the contamination is uncertain. As shown in Figure10b, PC1 and PC2 have an accounting ratio of 25.7%, and there is no specificgroup of PBDE congeners.

CONCLUSION

From the results, it is concluded that the source of dioxin contamination inLake Baikal is runoff from PCP-contaminated soil, air deposition, and com-bustion of waste residues, and contamination caused by pulp bleaching at thepaper mill. The concentration of PCDD/Fs is considerably lower than that inthe Great Lakes and PCP-contaminated lakes in China (30).

As for PCDD/Fs, the highest concentration of PCBs was found at Ol’khonIsland. PCB concentrations from Lake Baikal sediment are quite low. Basedon the similarities in the profile pattern of PCBs in Lake Baikal sedimentand that at Sovol, it has been suggested that Lake Baikal contamination ofPCBs is due to the use of technical PCB mixtures such as Aroclor. With theapplication of toxic potency, PAHs-TPEQ contributed the most to Lake Baikalcontamination compared to other compounds examined in this study. From theresults, the source of PAH contamination in Lake Baikal is suggested as agri-cultural and industrial activities. PBDE levels in Lake Baikal sediment werelower than those of the Great Lakes. Like many other major lakes worldwide,DecaBDE was dominant. The dominance of DecaBDE seems to be caused bythe use and production of electronic devices in big cities near the lake. How-ever, the exact source of general PBDE contamination in Lake Baikal is un-known, since the significant and direct influence of specific industries was un-noticeable in profile pattern or from PCA plots. Generally, the concentrationsof persistent organic pollutants were lower than from other major contami-nated lakes around the world. However, considering the fact that Lake Baikalsediment shows signs of dioxin, PCB, PBDE, and PAH contamination causedby the pulp industry and the use of pesticides and other agricultural activities,there are potential risks of contamination to Lake Baikal in the future. Thus,further monitoring of POPs in biota and the environment of Lake Baikal willbe necessary.

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