PCBs and chlorinated hydrocarbon pesticides in Antarctic atmosphere and hydrosphere

Chemosphere,Vol.12,No.2,pp 277-288,1983 Printed in Great Britain

0045-6535/83/020277-12503.00/0 ©1983 Pergamon Press Ltd.

PCBS AND CHLORINATED HYDROCARBON PESTICIDES IN ANTARCTIC ATMOSPHERE AND HYDROSPHERE Shinsuke Tanabe~ Hideo Hidaka and Ryo Tatsukawa Department of Environment Conservation, Ehime University, Tarumi 3-5-7, Matsuyama 790, Japan Abstract. PCBs and chlorinated hydrocarbon pesticides such as DDTs and HCHs (BHCs) were measured in air, water, ice and snow samples collected around the Japanese research stations in Antarctica and adjacent oceans during December 1980 to March 1982. The atmospheric concentrations of chlorinated hydrocarbons decreased in the transport process from northern lands to Antarctica, but the compositions of PCBs, DDT compounds and HCH isomers were relatively uniform throughout this process. Regional and seasonal variations were found in aerial concentrations of these pollutants at Syowa Station and adjacent seas in Antarctica. Chlorinated hydrocarbons were also detected in snow, ice, lake water and sea water samples, in which rather high concentrations were found in snow and ice samples. This suggests that snow and ice serve as media of supply of these pollutants into Antarctic marine environment. Most interestingly, the concentrations of DDTs and higher chlorinated biphenyls were much lower in sea water under fast ice than in that from outer margin of pack ice. This indicates that the active removal of these pollutants is occurred in the sea under fast ice, and that is strongly associated with high primary productivity. It is, therefore, presumed that the concentrations of PCBs and DDTs in marine organisms living under fast ice in Antarctica could be lower than those in other oceans. i.

INTRODUCTION Studies of the PCB and DDT pollution in Antarctica began with their detec-

tion in the wildlife (Sladen et al., 1966; George and Frear, 1966; Tatton and Ruzicka, 1967; Risebrough et al., 1968) and snow (Peterle, 1969) in the late 1960's.

This finding ensured the worldwide dispersion of these pollutants, and

successively new subjects were generated concerning their transport pathway and entire behavior in the Antarctic environment including atmosphere and hydrosphere. The determination of chlorinated hydrocarbons in Antarctic air and water will contribute to the comprehensive description of their global distribution and also provide basal information for the evaluation of their bioaccumulation in Antarctic ecosystems. The present paper deals with a general pollution of chlorinated hydrocarbons in Antarctic atmosphere and hydrosphere.

In the research, an intensive study has

been made by measuring the concentrations of PCBs, DDT compounds (including p,p'DDE, pjp'-DDT and o,p'-DDT) and HCH (BHC) isomers (including ~, ~ and [ isomers) in air, water, ice and snow samples collected from the Japanese Antarctic research stations and adjacent oceans during December 1980 to March 1982.

Our main con-

cerns are; (i) atmospheric transport process of chlorinated hydrocarbons to Antarctica, (2) regional and seasonal variations of their aerial concentrations in Antarctica, and (3) their behavior indigenous to Antarctic hydrosphere. Recent

277

278

studies

demonstrated

tribution 1981).

Also

which suggests Antarctica.

the

the

over

aerial

gaps.

lands

characteristic

survey,

resulting the

specific

distribution

the

locality

to Antarctica

natural

and behavior

global

1982a,

from northern

variation

amount,

the

with

conditions of these

dis-

o f PCBs, DDTs a n d

(Tanabe et al.,

pollutants

process,

from the

for

Bidleman et al.,

concentrations

Ocean

of these

be extended

transport

and Giam, 1981;

significant

transport

should

In addition,

(Atlas

the Antarctic

transport

aerial

hydrocarbons

use in northern

of atmospheric

hydrocarbons

in air

In this

chlorinated

prevalence

in our previous

HCHs w e r e f o u n d

poral

the

of chlorinated

1982b), lands

to

of airbone

fluxes

and season

of their

some s p a t i a l

in Antarctica

pollutants

of

and temmay i n d u c e

in Antarctic

environment. 2.

SAMPLE Air,

sea water,

lake

water,

ice

a n d snow s a m p l e s

were collected

Syowa Station [69°00'S, 59a55'E) as shown in Fig. i.

around

the

Surface and deep snow were

also sampled at the Mizuho Station (70°42'S, 44°20'E).

Besides land-based sta-

tions in Antarctica,

air and surface water were sampled from the Southern Ocean

on t h e

of research

cruise

routes

Chlorinated the

air

1/min.

pumps. for

the

hydrocarbons Approximately collection

vessels

in air

a s shown i n F i g .

were trapped

1 0 0 0 m3 o f a i r

2.

on p o l y u r e t h a n e

was d r a w n a t

o f PCBs a n d DDT c o m p o u n d s ,

foam by using

a flow rate

and about

of 550-650

200 m3 o f a i r

at

25-27 i/min, for HCH isomers. Sea and lake water under ice sheet were collected by a suction pump. ocean surface water was sampled by a all-metal bucket on board.

Open

Both snow and ice

samples were stocked in airtight polyethylene containers and then melted under room temperature.

About 200 to 1200 1 of water samples were obtained and passed

through Amberlite XAD-2 resin columns. Details of sampling method and discussion of collection efficiency for chlorinated hydrocarbons are given in our previous papers

(Tanabe et at., 1982a,

1982b). 3.

CHEMICAL ANALYSIS Chlorinated hydrocarbons trapped on polyurethane foam and Amberlite XAD-2

resin were eluted with acetone and ethanol respectively.

These solutions were

stocked in tightly sealed glass bottles and shipped to the laboratory. nated hydrocarbons in crude extracts were transferred to hexane.

Chlori-

Hexane solution

was concentrated to 10 ml and then cleaned up by shaking with 5 % fuming sulfuric acid. in

Then, the final hexane extract was further concentrated to 100 21 solution

a microconcentrator under a stream of purified nitrogen gas. Samples were determined by a gas chromatograph-mass

with a selected-ion monitor

spectrometer equipped

(Shimadzu GC-MS 9020 DF) and occasionally analyzed by

an electron-capture gas chromatograph

(Shimadzu GC-SA).

The columns were 2 mm

i.d. x 5 m long and packed with purified Apiezon L grease for PCB determinations,

279

i

I

i

68 ° 55'S-

a Kitano-ura/ Cove

69 °

00'

I

T

90°W ~ . ~

90~/

Syowa Station ~ o

/

180° 05'

i0' Langhovde

0 15'

,

Lake Nurume ~

5 i0 km , , 39°20'E 30' ,, ,,

~"cr~/~-.,~" ~'I ~ , 40' 50'

Figure I. A map showing sample collec tion sites around Syowa Station (69°00'S, 39°35'E), Antarctica.

20°S

, f 40 °

60 °

40°W

0°

40 °

80 °

120 °

160 °

160°E

160°W

Figure 2. Survey cruise routes. [A] anb [B] show the cruise routes of the Icebreaker Fuji during Feb. to Mar. 1982 and the TIS Umitaka-Maru during Dec. 1980 to Feb. 1981 respectively. Air and surface sea water samples were collected along the cruise routes.

280

and 2 mm i.d. x 1.8 m long and packed with 2 % QF-I + 1.5 % OV-17 for DDT compound and HCH isomer determinations. Details of determination procedures and measurement conditions were the same as those reported previously

(Tatsukawa e~ al., 1979).

Contaminations from sampling equipments,

glasswares, adsorbents and solvents

were checked preliminarily and found to be negligible. of PCBs, ZDDT

Overall procedural blanks

(sum of p,p'-DDE, pjp'-DDT and o,p'-DDT) and ZHCH

(sum of ~, ~ and

[ isomers) were less than 2 pg/m 3, 0.I pg/m ~ and 0.5 pg/m 3 for air samples respectively, and less than 5 pg/l, 0.2 pg/l and I pg/l for water samples respectively.

Background levels of aerial chlorinated hydrocarbons in the laboratory

of Syowa Station were also checked and found to be similar to those in outdoor samples. 4.

RESULTS AND DISCUSSION

4. I. Atmospheric Transport to Antarctica In order to make clear the transport pathway and process of chlorinated hydrocarbons to Antarctica, we first described their latitudinal distributions in air over the ocean between Syowa Station and Mauritius (Fig. 3).

The concentra-

tions of atmospheric PCBs, £DDT and £HCH tended to decline toward the Antarctica, although ZHCH was exceptionally high around 61°S latitude.

This declivity sug-

gests that the low latitudes serve as a major source of these pollutants for their transport to Antarctica.

In fact, chlorinated hydrocarbon pesticides such

as DDT and HCH are now consumed mainly in the developing countries in the tropics. Though there is little information on PCB use in the tropical regions, PCBs are most likely to be used in various materials and equipment without any restrictions.

A recent rice bran oil incident in Taiwan (Chen et aZ., 1980, 1981) is an

evidence for the current use of PCBs in the low latitude countries. In contrast to their concentrations,

little variation was found in the com-

positions of HCH isomers, DDT compounds, PCB congeners and its chlorine contents (Fig. 4).

A reasonable explanation for this is already given elsewhere

et al., 1982a, 1982b).

(Tanabe

Extensive use of lindane as well as technical HCH in the

tropics and southern hemisphere accounts for the high proportion of ~ and isomers all over the southern ocean.

Similarity between the composition of

aerial DDT compounds presented here and the formulation of DDT used for agriculture and malaria control suggests the active use of DDT in the tropics.

Abundance

of lower chlorinated biphenyls in open ocean atmosphere may be attributed to their relatively high vapor pressures. In summary, the aerial concentrations of chlorinated hydrocarbons dissipasively decreased in the transport process from northern lands to Antarctica, but their qualitative variations were rather small.

It is well known that chlorinated

hydrocarbons in open ocean atmosphere are present primarily in vapor phase (Giam et al., 1980; Atlas and Giam, 1981; Bidleman et al., 1981; Bidleman and Leonard,

281

1982).

Therefore, the fate and behavior of aerial chlorinated hydrocarbons

depend on the wet deposition and/or the gas exchange at air/sea interface. The uniform composition of aerial chlorinated hydrocarbons found here may imply that the washout rate by rainfall and/or the gas exchange rate at sea surface are almost constant in the world ocean.

3o01 PCBs

°A

......

,,

200

0 rj

h

/\

100

\\

~

20 °

I

I

30 °

40 °

0

0

A

-

0 ~ ~ 0 . I

I

50 °

60 °

O

70°S

Latitude

Figure 3. Latitudinal variations of ZHCH (sum o£ ~, ~ and ~ isomers), ZDDT (sum of pjp'-DDE, pjp'-DDT and ojp'-DDT) and PCB concentrations in open ocean air between Syowa Station (69°00'S, 39°35'E) and Mauritius (20°10'S, S7°30'E).

Latitude

HCH isomer

DDT compound

PCB congener Chlorine 4 5 6 C1 content(%) 45.8

pjp'- pjp'- o,p'68°-69°S

~

o( ~

DDE ~

66°-67°S

~

~

59°-63°S

~

/

[]

~\\\\\~1

54 ° - 6 0 °S

~

~

vA

t.\\\\\\\\~:.:.m

45.3

4 5 o _ .54 o S

~

~

r/,a

t,,\\\\\\\xl:.l

44.1

36°-45oS

~

~

VA

kX\\X~l:.:ll

43,6

27°-36°S

~

~

".'-"

45.8

20°-27°S

~

mr-

V~

k\\\X'l:.:.:ll

i

O

S

|

i

l

[

|

50

'

,

.

•

l

|

100 0

DDT

DDT

2 ~

5

~ W/A

|

i

~ i

i

I

50

.

i

.

t

|

|

100 0

44.1

,

,

•

I

i

50

i

i

i

43.9

44.8

i

100

F i g u r e 4. L a t i t u d i n a l variations o f HCH i s o m e r , DDT compound a n d PCB c o n g e n e r c o m p o s i t i o n s i n o p e n o c e a n a i r b e t w e e n Syowa S t a t i o n a n d M a u r i tius.

282

4.

2. R e g i o n a l Table

cides

and Seasonal

1 shows the

in air

samples

collected

An a p p a r e n t

difference

In general,

higher

(155 ° - 164°E) ration

off

indicate

lands

of these

chemicals

is

seas

the

the

Another

than

in the

Although rather

Recently,

chlorinated

in Arctic,

i n summer t h a n

of snowfall

during

ation

during

cause have

(1982}

less

rations

high

likelihood

in this

of being

Overall, chlorinated of the

it

amount,

a n d on t h e on.

found

reported

Thus,

on l a n d s used

various

and season

that

of Islands.

was a l s o

according

recog-

(Fig.

to the

the austral

seasonal

5).

chemicals, summer.

variation

there

chlorinated 5.

of aerial

in summer,

as well

are

lower

concent-

seasonal

variIn

which might PCBs

but

concent-

still

higher

from the active

factors

amounts

i n same s e a s o n .

on l a n d s

wind,

their

to Antarctica.

evaporation

due to high

and seasonal

on t h e

larger

hydrocarbons

Furthermore,

season,

regional

for

may e x t e n d

atmosphere

use

levels

are

sources

of their

Indian

19801

regions,

aerial

be caused

such as prevailing

the

Balleny

i n Syowa S t a t i o n

particularly

depends

over

to

were apparently

lands

could

mainly

o f PCBs.

variation

during

the

in

and from

concentrations

in a limited

This

case

wind

found

According

concentration

which accounts

in Antarctic

probably

factors

in the

different

period,

can be concluded

locality

natural

Islands)

Coast and near

seasonal

a s shown i n F i g .

from its

hydrocarbons

high

obtained

in northern

applied

i n summer.

o f PCBs i n t o a t m o s p h e r e i n summer s e a s o n .

the

In Antarctic

concentrations

were found

also

in winter.

are

the

i n w h i c h HCH i s o m e r

autumn to winter

pesticides

their

the prevailing

(Tanabe and Tatsukawa,

Sabrina

were slightly

of the use of chemicals

general,

off

hydrocarbons

autumn to winter.

t o be r e m o v e d b y s n o w f a l l rations

explains

seas

use

wind to

hydrocarbons

and Balleny

oceans

were generally

Oehme a n d S t r a y

from

the present

o f DDTs a n d HCHs i n a i r

variation,

patterns

concentrations

levels

may b e p r o b a b l e

aerial

organochlorines higher

however, regional

the varied

high

the

as the

These results

of prevailing

Ocean respectively.

in other

This

over

A PCB c o n c e n t -

hydrocarbons

chlorinated

Coast

Islands

a n d Amundsen Bay) m i g h t b e t r a n s p o r t e d

those

1982).

in air

explanation,

As w e l l

Sabrina

locations.

Balleny

regions.

In Antarctica,

Therefore,

(off

at various

Presumably,

direction

variations.

concentration

much h i g h e r

pesticides

complicated.

pesti-

same s e a s o n .

in Antarctica. in other

chlorinated

and the

Ocean and the Atlantic

Bidleman and Leonard,

nized

these

the year.

Syowa S t a t i o n

Indian

studies,

Ocean are

rather lands

f r o m 121°E t o 164°E

through

these

is

in northern

(off

those

pathway of aerial

to Antarctica

throughout

39°E t o 50°E recent

transport

hydrocarbon the

were found near

(121°-125°E) than

at

was o b s e r v e d

of pesticides

Coast

seem to have led

northwest

the

Sabrina

Atmosphere

locations

concentrations

C o a s t was h i g h e r

the

northern Antarctica

in their

and off

in Antarctic

o f PCBs a n d c h l o r i n a t e d

from different

concentrations

Sabrina

that

Variations

concentrations

variations

of chemicals as their

snowfall,

temperature of aerial inclusive

vapor pressures,

temperature

and so

283

Table i. Regional variations of ZHCH, EDDT and PCB concentrations (pg/m ~) in air samples collected from adjacent seas of Antarctica. Location

Sampling date

EHCH

ZDDT

PCBs

off Sabrina Coast a (61o_65oS, 121o 125oE)

Jan.

'81

120

240

180

near Balleny Islands a (60o_67oS, 155o_164oE)

Jan.

'81

170

190

64

off Syowa Station b (68o_69os, 39oE)

Feb.

'82

49

20

81

near Amundsen Bay b (66oS, 47o_50OE)

Feb.

'82

44

22

96

a Collected by Umitaka-Maru b Collected by Fuji cruise.

cruise.

180 A 160

It

It

J,,..o__

140 .-,

120

O

i00

~

~

/i"',

EHCH

\o

d

80

o u

60

I;

,,

40

/k

,t".-.- -. .

20

/

\ / \ /

~

"

/,

O

40/ °" \ _

\ ?

0

/

A I

~

-O..~lt/"

I

1

I

I

I

I

I

I

I

I

I

I

J '81

F

M

A

M

J

J A Month

S

O

N

D

-A PCBs

I

i

J '82

F

Figure 5. Seasonal variations of ZHCH, ZDDT and PCB concentrations in air collected from Syowa Station, Antarctica.

4. 3. Specific Behavior Concentrations samples are presented concentrations

in A n t a r c t i c

Hydrosphere

o f ZHCH, £DDT a n d PCBs i n s n o w , i c e , in Table

of these

2.

pollutants

p l i e s t h a t snow a n d i c e a c t marine environment. A l t h o u g h a few w o r k e r s

Snow a n d i c e

in comparison with water

as media of s u p p l y of t h e s e so f a r

sea water

samples contained

measured the

and l a k e w a t e r much h i g h e r

samples.

pollutants

concentrations

This

im-

into Antarctic

o f PCBs a n d DDTs

284

Table

2. Concentrations (pg/l) of ZHCH, ZDDT and PCBs in Antarctic lake water and sea water.

Sample Sampling

Snow Mizuho Station ,, Tottuki

Sampling

station

date

snow,

ice,

PCB C1 c o n t . (%)

£HCH

ZDDT

PCBs 160

43.1

(surface) a

May

'81

2300

15

(deep) a

May

'81

1500

9.0

220

42.8

2800

17

160

44.2

4900

16

I000

41.6

2200

Ii

610

40.9

310

41.4

Nov.

Point

'81

Sept.

Lake Nurume Ice Tottuki Point

'81

July-Sept.

'81

Lake Nurume

Nov.

'81

2000

9.8

Sea water b Tottuki Point

July

'81

570

1.3

54

37.9

Oct.

'81

210

1.5

35

38.4

Jan.

'82

570

1.5

69

39.3

Oct.

'82

330

1.3

48

41.2

Langhovde Kitano-ura Cove Lake water b Lake Nurume Sea water c 64°55'S, 124°40'E

Jan.

'81

930

5.4

52

46.4

62°37'S,

157°38'E

Jan.

'81

290

15

42

47.4

62°00'S,

160°06'E

Peb.

'81

290

21

72

46.5

a The age of surface and deep snow were estimated from a report of Watanabe and Yoshimura (1972), and given as 1980 and approximate 1960 respectively. b Collected

from under fast ice.

c Collected

from outer margin of pack ice by Umitaka-Maru

in Antarctic centration the

snow s a m p l e s , levels.

there

r a n g e o f 490 t o 630 p g / k g

300 p g / k g o f PCBs i n s u r f a c e were nearly higher

the

at

hydrocarbon

w h e r e a s LDDT l e v e l s

Syowa S t a t i o n

pollutants

there

was n o t

concentrations.

The m o s t i n t e r e s t i n g

finding

ples,

w h i l e ZDDT c o n c e n t r a t i o n s in surface

water

and

p,p'-DDT)

conwithin

a n d o f 30 t o

Their

PCB l e v e l s were much

a n d d e e p snow s a m p l e s c o l l e c t e d suggests

to Antarctica

since

the

in sea water

load of these

1960's.

comparison of chlorinated

were n o t under

from

in chlorinated

steady

samples under fast

Z HCH c o n c e n t r a t i o n s from outer

difference

that

was made i n t h e

in between sea water

margin of pack ice.

on t h e i r

concentrations

a t Doumer I s l a n d

found any significant This fact

outer

than those

the

and Mizuho S t a t i o n .

surface

has been transported

carbon concentrations

reported

snow s a m p l e s a t Doumer I s l a n d .

In comparison between the Mizuho S t a t i o n ,

r e m a i n some c o n t r a d i c t i o n s (1976)

o f DDTs (sum o f p , p ' - D D E

same o f o u r s ,

than those

still

Risebrough et aZ.

cruise.

fast

ice

and that

so d i f f e r e n t

i n b o t h sam-

i c e were e v i d e n t l y

margin of pack ice.

hydro from lower

PCB c o n c e n t r a t i o n s

285

were nearly at the same level in both samples, but its chlorine contents were apparently lower in under fast ice than in outer margin of pack ice (Table 2). Then, when compared the PCB concentrations in respect of chlorine numbers, much low concentrations were found in higher chlorinated biphenyls in the samples from under fast ice (Table 3).

Moreover, a composition of PCB isomers and congeners

in sea water from under fast ice showed smaller proportion of higher chlorinated biphenyls as compared with those in snow and fast ice which serve as a source of PCB supply into sea water (Fig. 6).

We have noted in a previous paper that less

water soluble chlorinated hydrocarbons with high affinity to suspended materials are readily removed from surface water by sinking particles, and that active removal of these chemicals is strongly associated with the primary productivity in the oceans (Tanabe and Tatsukawa, MS).

Holm-Hansen et aZ. (1977) reported that

the primary productivity in Ross Sea was several times higher in water under fast ice than in water outer margin of pack ice.

These facts, therefore, strongly

support the idea that DDT compounds and higher chlorinated biphenyls with high affinity to suspended materials are rapidly removed from surface to deeper layers in the water column by sinking particles resulting from the active primary productivity under fast ice.

This active vertical transport seems to be responsible

for the low concentrations of these pollutants in sea water under fast ice.

Same

explanation is applicable to water samples from Lake Nurume where both the concentration of £DDT and the chlorine content of PCBs were also low (Table 2). It is well known that DDTs and higher chlorinated biphenyls are very accumulative in the organisms.

The low concentration levels of these pollutants in sea

water under fast ice strongly suggest that DDT and PCB concentrations in marine organisms living under fast ice in Antarctica would be relatively lower than those in other oceans.

Biological studies in Antarctica will appear elsewhere

(Subramanian et al., MS; Hidaka et al., MS).

Table 3. Concentrations (pg/l) of PCEs in respect of chlorine numbers in surface sea water from the Antarctic Ocean. Location 2 C1 5 Cl 4 C1 $ C1 6 Cl Total Under fast ice Tottuki Point

26

21

4.8

1.8

<0.2

54

Langhovde

16

15

4.2

1.3

<0.2

35

Kitano-ura Cove

25

53

9.6

1.4

<0.2

69

5.7

O u t e r margin of pack ice a 64°55'S, 124°40'E

11

17

12

8.2

62°57'S, 157°58'B

8.0

14

II

7.1

1.7

42

62°00'S, 160°06'E

18

26

15

ii

2.3

72

a Collected

by U m i t a k a - M a r u

cruise.

52

286

;now

C1 c o n t e n t :

Sea

44.2

1.0

water

C1 c o n t e n t :

37.9

%

1.0

= 0 U o

> O.S o

IJ,J,,l,,,, |

3l

2

I

.ll

I,III.. II

..

41 s l 6 I 7181g Cl

Fast

0

>0.5

ice

,..,.,

31 41

......

sl

617181~

C1 number

number

CI c o n t e n t :

40.9

1.0

J O u o

>

0.5

I!,'r'1,iJ,,,,,,,,.... 2

31 41 s l

6

17181

CI n u m b e r

Figure 6. PCB isomer and congener compositions in snow, fast ice and sea water samples collected from Tottuki Point near Syowa Station, Antarctica. Sea water was sampled under fast ice. Each bar shows the each peak on mass fragmentogram of PCBs. Details of each peak and its chemical structure are given in our previous report (Tanabe et aZ. 1981).

ACKNOWLEDGEMENTS This study was performed under two projects of the 22nd Japanese Antarctic Research Expedition (JARE-22) and the Biological Investigation of Marine Antarctic Systems and Stocks (BIOMASS).

We are pleased to acknowledge the considerable

support of Professor T. Torii, Chiba Institute of Technology, Dr. T. Hoshiai, National Institute of Polar Research, and Professor T. Yoshida, Tokyo University of Fisheries, for our participation to these projects.

The authors are grateful

to Dr. Y. Yoshida, National Institute of Polar Research, and Professor M. Murano, Tokyo University of Fisheries, for their kind arrangements and encouragements for sampling.

We would like to thank all members of wintering party of JARE-22 and

of BIOHASS project for their advices and cooperations.

Thanks are also due to

the officers and crew of the Icebreaker Fuji and T/S Umitaka-Maru for their assistance on board. This work was supported in part by a Grant-in-Aid for Scientific Research from the Ministry of Education, Science and Culture of Japan.

287

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(Received in Japan 8 December 1982)

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