7
Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants M. BASKARAN* Department of Geology, Wayne State University, 0224 Old Main Building, Detroit, MI 48202, USA The sources of inorganic pollutants to the Arctic areas are reviewed using previously published results. The removal of particle-reactive pollutants is discussed using thorium scavenging as an analog. The scavenging of 234 Th from the upper water column (100 m) and sediment inventory of 230 Th from the deep Arctic waters is compared to dierent ocean basins in the subarctic areas. Such a comparison shows that 234 Th is in equilibrium with its parent, 238 U, in certain regions of the Canada Basin of the Arctic Ocean, while it is deficient in other regions of the arctic as well as in sub-polar ocean basins. This implies that the particle- reactive pollutants in the deep Arctic of the Canada Basin are less likely to be removed from the deep waters and will eventually be transported out of this area. We have uti- lized the 230 Th inventory in sediments from the Arctic area to determine the removal rates of particle-reactive nuc- lides. The 230 Th inventory in the deep Arctic Ocean of the Canada Basin is much lower than the Norwegian Sea and the Fram Strait of the Arctic as well as all other sub-polar world oceans. These observations suggest that any pollu- tants into the deep Arctic areas of the Canada Basin are less likely to be removed locally and may be transported out of this area. In those areas, the colloidal material could potentially play a major role in the removal of particle-reactive contaminants. Ó 2001 Elsevier Science Ltd. All rights reserved. Introduction The organic and inorganic pollutants in the Arctic are primarily introduced through discharges into Arctic rivers (from sewage and industrial euents) and/or through runo, atmospheric fallout and from the water mass transport from the North Atlantic Ocean. Of these pollutants, the particle-reactive ones are removed pri- marily by the removal of particles (sedimentation) while those that have low particle reactivity, follow the water masses and eventually exported out of the Arctic to other oceanic regimes. Biological processes and abio- logical particles primarily remove the particle-reactive pollutants by scavenging. Most of the water flow into the arctic is derived from the North Atlantic that comes from the direction of oshore America and Western Europe. The inflows and outflows to the Arctic Ocean are given in Table 1. The northward flow through the Fram Strait is esti- mated to be 12:7 10 6 m 3 s 1 12:7 Sv. The in- flow from the Pacific through the Bering Strait is about 9% of the water that flows through the Fram Strait (Tolmazin, 1985). It is probable that millions of tons of pollutants of agrochemical and industrial ori- gin from America and Western Europe reach the Arctic through the Fram Strait. The riverine flow from Arctic rivers is estimated to be 0:15 m 3 s 1 while the amount of precipitation directly into the Arctic waters is estimated to be 0:114 m 3 s 1 (Tolmazin, 1985). The five major rivers, the Yenisey, Ob, Koly- ma, Lena and Mackenzie rivers drain a continental area of more than 10 7 km 2 (Rey, 1982). The six Arctic seas that receive euents from Russia are: White sea, Barents Sea, Kara Sea, East Siberian Sea, Laptev Sea and Chukchi Sea. During the annual maximum of sea-ice cover, the pack ice reaches an area of 10 7 km 2 , which is 30% of the world’s sea ice. In the Arctic Ocean, the shallow seas (4:1 10 6 km 2 ) are seasonally ice-covered and the deep basins (8:2 10 6 km 2 ) are usually covered by 3–5 m of ice throughout the year (Wheeler et al., 1997). Ice-cover prevents the atmospherically delivered pollutants from directly reaching the water-column. The melting of the ice and the displacement of the ice-cover, either by wind or moving ice along with ice-rafting of bottom sedi- ments in shallow seas (as well as lakes), eventually leads to the redistribution of sediments as well as sediment- sorbed particle-reactive pollutants (Nichols, 1967; Her- manson, 1990). In addition, ice rafting has been reported to be the dominant mechanism responsible for the transport of fine-grained contaminant-laden sedi- ments from coastal zones to the deep Arctic Basin (e.g., Barnes et al., 1982; Kempema et al., 1989; Reimnitz Marine Pollution Bulletin Vol. 42, No. 1, pp. 16–22, 2001 Ó 2001 Elsevier Science Ltd. All rights reserved Printed in Great Britain 0025-326X/01 $ - see front matter PII: S0025-326X(00)00194-6 *Tel.: +1-313-577-3262. E-mail address: [email protected] (M. Baskaran). 16

Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

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Page 1: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

Scavenging of Thorium Isotopes in theArctic Regions: Implications for theFate of Particle-reactive PollutantsM. BASKARAN*Department of Geology, Wayne State University, 0224 Old Main Building, Detroit, MI 48202, USA

The sources of inorganic pollutants to the Arctic areas arereviewed using previously published results. The removalof particle-reactive pollutants is discussed using thoriumscavenging as an analog. The scavenging of 234Th from theupper water column (�100 m) and sediment inventory of230Th from the deep Arctic waters is compared to di�erentocean basins in the subarctic areas. Such a comparisonshows that 234Th is in equilibrium with its parent, 238U, incertain regions of the Canada Basin of the Arctic Ocean,while it is de®cient in other regions of the arctic as well asin sub-polar ocean basins. This implies that the particle-reactive pollutants in the deep Arctic of the Canada Basinare less likely to be removed from the deep waters and willeventually be transported out of this area. We have uti-lized the 230Th inventory in sediments from the Arctic areato determine the removal rates of particle-reactive nuc-lides. The 230Th inventory in the deep Arctic Ocean of theCanada Basin is much lower than the Norwegian Sea andthe Fram Strait of the Arctic as well as all other sub-polarworld oceans. These observations suggest that any pollu-tants into the deep Arctic areas of the Canada Basin areless likely to be removed locally and may be transportedout of this area. In those areas, the colloidal materialcould potentially play a major role in the removal ofparticle-reactive contaminants. Ó 2001 Elsevier ScienceLtd. All rights reserved.

Introduction

The organic and inorganic pollutants in the Arctic areprimarily introduced through discharges into Arcticrivers (from sewage and industrial e�uents) and/orthrough runo�, atmospheric fallout and from the watermass transport from the North Atlantic Ocean. Of thesepollutants, the particle-reactive ones are removed pri-marily by the removal of particles (sedimentation) whilethose that have low particle reactivity, follow the watermasses and eventually exported out of the Arctic to

other oceanic regimes. Biological processes and abio-logical particles primarily remove the particle-reactivepollutants by scavenging.

Most of the water ¯ow into the arctic is derivedfrom the North Atlantic that comes from the directionof o�shore America and Western Europe. The in¯owsand out¯ows to the Arctic Ocean are given in Table 1.The northward ¯ow through the Fram Strait is esti-mated to be �12:7� 106 m3 sÿ1�� 12:7 Sv�. The in-¯ow from the Paci®c through the Bering Strait isabout 9% of the water that ¯ows through the FramStrait (Tolmazin, 1985). It is probable that millions oftons of pollutants of agrochemical and industrial ori-gin from America and Western Europe reach theArctic through the Fram Strait. The riverine ¯owfrom Arctic rivers is estimated to be 0:15 m3sÿ1 whilethe amount of precipitation directly into the Arcticwaters is estimated to be � 0:114 m3sÿ1 (Tolmazin,1985). The ®ve major rivers, the Yenisey, Ob, Koly-ma, Lena and Mackenzie rivers drain a continentalarea of more than 107 km2 (Rey, 1982). The six Arcticseas that receive e�uents from Russia are: White sea,Barents Sea, Kara Sea, East Siberian Sea, Laptev Seaand Chukchi Sea. During the annual maximum ofsea-ice cover, the pack ice reaches an area of 107 km2,which is 30% of the world's sea ice.

In the Arctic Ocean, the shallow seas (4:1� 106 km2)are seasonally ice-covered and the deep basins(8:2� 106 km2) are usually covered by 3±5 m of icethroughout the year (Wheeler et al., 1997). Ice-coverprevents the atmospherically delivered pollutants fromdirectly reaching the water-column. The melting of theice and the displacement of the ice-cover, either by windor moving ice along with ice-rafting of bottom sedi-ments in shallow seas (as well as lakes), eventually leadsto the redistribution of sediments as well as sediment-sorbed particle-reactive pollutants (Nichols, 1967; Her-manson, 1990). In addition, ice rafting has beenreported to be the dominant mechanism responsible forthe transport of ®ne-grained contaminant-laden sedi-ments from coastal zones to the deep Arctic Basin (e.g.,Barnes et al., 1982; Kempema et al., 1989; Reimnitz

Marine Pollution Bulletin Vol. 42, No. 1, pp. 16±22, 2001

Ó 2001 Elsevier Science Ltd. All rights reserved

Printed in Great Britain

0025-326X/01 $ - see front matterPII: S0025-326X(00)00194-6

*Tel.: +1-313-577-3262.E-mail address: [email protected] (M. Baskaran).

16

Page 2: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

et al., 1993; P®rman et al., 1995; Cooper et al., 1998;Landa et al., 1998).

The primary productivity is maximum during the ice-free, three summer months and the productivity is nearzero during the remaining nine months. A sediment trapdeployed in the Eastern Chukchi Sea (66°370 N) indi-cated that the average mass ¯ux during the ice-covermonths (measured in February) was about 10% of themagnitude of the mass ¯ux during the ice-free months.The dust particles that are delivered to the sea surfaceare retained on the sea ice-cover; thus the suspendedparticle concentration in the ice-cover months is muchlower than in most temperate regions. The particleconcentration in the deep (>3000 m water depth) Arctic(Canada Basin) is �5 lg lÿ1, (Bacon et al., 1989b)compared with 102±103 lg lÿ1 in other places. Since theparticles play a major role in the removal of particle-reactive pollutants, lower particle concentration plays amajor role in decreased removal rates of pollutants.

Particle-reactive Radionuclide Scavenging

Quantitative information on the intensity of scav-enging can be estimated from the disequilibrium be-tween the pairs 234Th and 238U, as well as 230Th and 234U.It has been shown that in the upper 100 m of subarcticwaters, the activity of 234Th is not in equilibrium with itsparent 238U, which is attributed to the removal of 234Thby particles (both abiotic and biotic) on the time scale ofdays to months (Bhat et al., 1969; Coale, 1985, 1987;Baskaran et al. (1995) and the references therein). Thedisequilibrium between 234Th and 238U in the arcticwaters will yield information on the rates of removal ofparticle-reactive pollutants from the Arctic waters. Theresidence time of 230Th in the open ocean is <100 yr(Anderson et al., 1983a,b), which is much shorter thanits half-life (75 200 yr). After its removal from the watercolumn by sorption onto particles, 230Th reaches thesediment. Thus, if the 230Th sorbed particles reach thesediment, where 230Th was removed, then its de®ciencyin the water column (234U±230Th) should be found in thesediment. The ratio of 230Th inventory in sediments to

the production of 230Th is a measure of vertical scav-enging of 230Th in that particular site. In areas wherelateral advection is high and/or the scavenging is veryslow, it is likely that most of in situ-produced 230Th islaterally transported to other oceanic regimes.

In this paper, a review of the sources of pollutants tothe Arctic is attempted. In addition, the disequilibriumbetween 234Th and 238U, as well as the residence times ofdissolved and particulate 234Th in the upper 100 m watercolumn of the major ocean basins is compared to thedeep Arctic basin. The sediment inventory of 230Th inthe world-ocean is compared to the corresponding val-ues in the Canada and Nansen Basins of the Arctic aswell. The goals and objectives of this paper are todelineate the di�erences in scavenging intensity of par-ticle-reactive nuclides between the subarctic and Arcticwaters as well as the di�erences between di�erent basinswithin the Arctic region.

Sources and Fate of Pollutants to the Arctic

Atmospheric input of pollutants in to the Arctic watersThe Arctic atmosphere is expected to be relatively

pollution-free due to its remoteness and distance frommajor population and industrial centers in the Arctic.However, atmospheric transport of contaminants maybe an unde®ned source of contaminants as has beenreported. The Arctic atmosphere is very hazy duringwinter and early spring. This haze appears to be a carrierof acidity, trace metals, organics, etc., derived fromlong-range transport of midlatitude pollution products(Rahn, 1981; Barrie, 1986; Talbot et al., 1992). The ®l-ters that were used to collect aerosols in the Arcticduring winter were found to be gray in color as opposedto the summer aerosols, which are colorless. This graycolor was attributed to the sooty carbon derived fromthe lower latitudes (Rahn, 1981; Barrie, 1986; Talbotet al., 1992). In marine environment, the atmosphericaerosols that are primarily removed by wet precipitationand dry fallout, deposit into the pack ice and are sub-sequently released into the water column. Due to thesmaller size of the Arctic aerosols (because these aero-sols are well-aged and are derived from midlatitudes),the dry fallout should be of less importance; on the otherhand, low amount of precipitation will make the wetdeposition less important. Rahn (1982) concluded thatdry and wet deposition is likely to have approximatelythe same relation in the Arctic as in midlatitudes.

The concentrations of vanadium in the aerosols havepreviously been used as a pollutant index. The twomajor sources of vanadium to the aerosols includesmoke as a result of combustion of fossil fuels and thesoil dust. Higher concentrations of vanadium and sul-fate (SO2 derived from the mid-latitudes and are sub-sequent conversion to sulphate) in the Arctic aerosolsduring winter were observed. It has been reported that90±95% of the vanadium in the Arctic aerosols duringwinter is pollution-derived (Rahn, 1982). In addition,

TABLE 1

Water mass balance for the Arctic Ocean (Tolmazin, 1985).

In¯uxes Transport (Sv) Percent of total

In¯ux from Atlantic Ocean 12.68 89.4In¯ux from Paci®c Ocean 1.14 8.8Precipitation 0.114 0.8River runo� 0.149 1.0

Total 14.1 100.0

Out¯owsDischarge into Atlantic Ocean13.8

98.2

Transport of ice 0.19 1.4Evaporation 0.034 0.4

Total 14.0 100.0

17

Volume 42/Number 1/January 2001

Page 3: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

210Pb in Arctic aerosols during the winter months atBarrow, Alaska are highest compared to values fromother places (Rahn and McCa�rey, 1980). The 222Rnexhalation rate from the ocean surface is about twoorders of magnitude slower than that of the continents(Turekian et al., 1977; Baskaran and Naidu, 1995 andthe references therein). Thus, if these aerosols were de-rived from the marine air, the 210Pb concentration wouldbe much lower. The Rn exhalation rate from the per-mafrost-laden soils is considerably lower than the valuesreported for other continental settings (Baskaran andNaidu, 1995). From these observations, it is likely thatmost of the 210Pb is derived from the horizontal advec-tion from middle latitudes within the lower layers of thetroposphere.

Another evidence for horizontal advection is sug-gested by the concentrations of 7Be in aerosols. The 7Bedata for Arctic sites show strong seasonal variationswith peak concentrations in the late winter or earlyspring (Feely et al., 1989). The peak concentration of7Be in air samples coincides with arrival of Arctic hazethat is derived from mid latitude regions of Asia, Europeand North America (Rahn, 1981). It is believed that 7Be(and likely 210Pb) enters the lower troposphere of theArctic as a result of horizontal advection from middlelatitudes within the lower layers of the troposphere(Feely et al., 1989). Thus, it is likely that 210Pb producedfrom degassed 222Rn in the Arctic is not only from the222Rn that emanated from the soil in the Arctic (which islikely to be a minor component), but also from thehorizontal advection from middle latitudes within thelower layers of the troposphere. More recent study byBaskaran and Shaw (2000) indicates that the contami-nant-laden aerosols in the Alaskan Arctic region have arelatively longer residence time during the wintertime.

Riverine input of pollutants to the Arctic watersMost of the riverine input into the Arctic Ocean

comes from the former USSR territories. The total an-nual riverine ¯ow into the Arctic Ocean is estimated tobe 3:75� 1012 m3, which is about 2% of the oceanic¯ow into the Arctic Ocean from the North Atlantic andabout three times greater than the annual precipitationinto the Arctic ocean (Dorsey and Peterson, 1976; Rahn,1982). The relative amounts of pollution through at-mosphere, rivers and oceanic input can be evaluatedfrom a consideration of the inputs of Pb, given in Rahn(1982), into the Arctic. The annual input of Pb from theworld ocean, mainly through the North Atlantic, is es-timated to be 4:1� 103 metric tons (MT) and is about athird of the riverine input (11� 103 MT). The averageannual atmospheric input is also signi®cantly lower thanthe world ocean input (0:88� 103 MT).

Role of sea ice in the transport of contaminants in theArctic Ocean

Ice rafting is a dominant mechanism responsible forthe transport of ®ne-grain-laden contaminants from

coastal zones to the deep Arctic Basin (Barnes et al.,1982; Kempema et al., 1989; Landa et al., 1998). Forexample, ®ne ice crystals that form in suspension insupercooled, turbulent water (known as Frazil ice) hasbeen shown to scavenge ®ne-grained sediments as wellas particle-reactive contaminants from the water col-umn. Transport of continental shelf sediments in sea icefrom shelf areas to the deeper basins could play a sig-ni®cant role in biogeochemical cycling of radionuclidesand other contaminants.

Scavenging Rates of Particle-reactive Pollutants

The scavenging of particle-reactive pollutants in theArctic Ocean critically depends on suspended particleconcentrations in the water column. In areas, where theparticle concentrations are high, the particle-reactivepollutants are rapidly transferred to the sediments. Ithas been shown that the removal behavior of 228Th fromthe water column by the rapid attachment to suspendedparticles and subsequent removal to the sediments isanalogues to Fe, Cr(III) and Po from the water column(Santschi et al., 1984). The production, transport andsettling of particles in polar oceans involves intriguingproblems. The seasonal variations in primary produc-tivity are very large due to solar insolation (heat enteringthe atmosphere, ocean and land from the sun) patternsin the Polar Regions. It has been shown that the prin-cipal components of polar ocean ¯uxes are controlled bybiological interactions in the surface layers, even thoughsedimentation of coarse ice-rafted rock detritus involvesonly physical processes (Honjo, 1990).

The intensity of scavenging can be investigated usingthe disequilibrium between 234Th and its parent, 238U. Inmost world oceans, in the upper 100 m of the watercolumn, there is a de®ciency of 234Th with respect to238U. This de®ciency can be used to investigate the ex-tent of disequilibrium and to determine scavenging rateconstants. The published data on 234Th de®ciency fromthe world ocean, including one station from the Arctic,are presented in Table 2. The average residence time ofdissolved (ss) and particulate Th (sp) in the upper 100 mis calculated using the equations

ss � 234Thd= �238U�

±234Thd�kTh

� �1�and

sp � 234Thp=f �238U� ÿ 234Thd ÿ 234Thp

�kThg; �2�

where kTh is the 234Th decay constant (0.029 dÿ1), �238Ud�and �234Thd� are 238U and 234Th dissolved activity con-centrations (dpm lÿ1), respectively, and 234Thp are theparticulate 234Th concentrations.

The calculated average residence times of dissolvedand particulate 234Th for the upper 100 m of the worldocean are also presented in Table 2. The deep CanadianBasin Arctic is the only place where 234Th is in radio-active equilibrium with 238U. However, recent studies

18

Marine Pollution Bulletin

Page 4: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

TABLE

2

Inventories

ofparticles(l

gcmÿ2),dissolved

andparticulate

234Th(dpm

cmÿ2)and

238U�d

pm

cmÿ2)andaverageresidence

times

ofdissolved

andparticulate

234Thin

theupper

100m

ofthemajorocean

basins.

Area

Particle

inventory

(lg

cmÿ2)

Dissolved

234Th

inventory

(dpm

cmÿ2)

Particle

234Th

inventory

(dpm

cmÿ2)

238U

inventory

(dpm

cmÿ2)

234Thde®ciency

(dpm

cmÿ2)

Dissolved

234Th

residence

time(d)

Particulate

234Th

residence

time(d)

Reference

Paci®c±VERTEX

II�1

8°N

109°W

NA

14.99�1.02

3.73�0.22

24.31

5.59�1.04

56�11

23�4

Coale

andBruland

(1987)

Paci®c±VERTEX

III

�16°N

107

°WNA

14.51�

0.61

3:3

9�

0:1

224.28

6:3

8�

0:6

252�

51

8�

2Coale

andBruland

(1987)

Paci®c±VERTEX

IV�2

8°N

155

°WNA

20:2

0�

0:5

12:7

6�

0:1

824.87

1:9

1�

0:5

4150�

23

50�

15

Coale

andBruland

(1987)

EasternTropicalPaci®c

11°310 N

87°16W

(628m)

NA

17.26

)23.59

6.33

95

)BaconandRutgers

vander

Loe�

(1989a)

GulfofMexico

470(summer)

19:4

6�

1:1

51:3

9�

0:0

625.67

4:8

2�

1:1

5109�

33

10�

2Baskaranet

al.(1996)

(26°410 N

;94°590 W

(1500m)

700(spring)

16.90�

0.86

0:9

1�

0:0

525.32

7:5

1�

0:8

670�

12

4�

1Baskaranet

al.(1996)

NorthAtlantic

47°05.40 N

;19°55.1W0

20:1�

2:6

3:5

0�

0:4

224.7

1:1

0�

2:6

3152�

88

111�

266

Buesseleret

al.(1992)

47°05.40 N

;19°55.1W0

16:5�

2:0

5:1

8�

0:5

024.7

3:0

2�

2:0

670�

19

60�

41

47°05.40 N

;19°55.1W0

15:5�

1:3

3:4

1�

0:3

524.7

5:7

9�

1:3

559�

10

20�

547°05.40 N

;19°55.1W0

13:6�

0:8

3:4

6�

0:3

224.7

7:6

4�

0:8

643�

46�

2CESAR

IceCamp,Arctic

Ocean

85°5

00 N

108

°500 W

54.3

22.4

0.33

22.7

)0.03

2597

)Baconet

al.(1989b)

19

Volume 42/Number 1/January 2001

Page 5: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

have indicated that there is active scavenging in theChukchi plateau due to higher suspended particle con-centrations and particle ¯uxes (Moran et al., 1997; Ed-monds et al., 1998). In areas where suspended particleconcentrations are very low (as well as low sedimenta-tion rates, as reported by Ku and Broecker (1967);Finkel et al. (1977); and Bacon et al. (1989b)), it is likelythe colloidal material will play a signi®cant role in metalscavenging. Wheeler et al. (1996) have reported thedissolved organic carbon concentrations (which is usedas a proxy for marine colloids, as most of the colloidalmaterial is organic in composition) comparable to mostother ocean basins. The dissolved residence time, cal-culated using Eq. (1), is the longest for the CESAR IceCamp station in the Canada Basin. This observation isin contrast with the results of Cochran et al. (1995), whofound that Th residence times in the Nansen Basinsurface waters were comparable to the values obtainedfor open North Atlantic Ocean waters (Broecker et al.,1973; Li et al., 1980). This di�erence between the Nan-sen Basin surface water and Canada Basin water is at-tributed to the di�erences in the particles ¯uxes betweenthe two basins and/or the di�erences in the ventilationtime scales between the two basins (Cochran et al.,1995). The suspended particle inventory in the watercolumn at this station is approximately an order ofmagnitude higher than the values reported for the Gulfof Mexico (Baskaran et al., 1996).

The slow removal of these particle-reactive nuclideswill result in the building up of these nuclides in thewater column and is likely to result in a low inventory ofparticle-reactive radionuclides in sediments. For exam-ple, 230Th, which is a decay product from the dissolved234U, is produced at a known rate given by the relation:

N � 280Z�atoms cmÿ2 minÿ1�;

where N is the standing crop production of 230Thexcess

and Z is the water depth in km. In situ scavenging bysuspended particles and subsequent settling of theseparticles requires that sediments contain all the 230Th. Inareas, where there is a slow removal of particle-reactiveradionuclides, the measured inventory should be lessthan the theoretically predicted inventory.

Several researchers have reported that unusual phys-ical characteristics, such as seasonal or permanent icecover, very limited primary productivity (and low sus-pended particle concentration), wide continental shelvesand di�erences in the characteristics of glacio-marinesuspended matter, result in relatively slow removal ratesfor biochemically active and particle-reactive trace ra-dionuclides in high-latitude oceans, such as the ArcticOcean (Ku and Broecker, 1967; Finkel et al., 1977;Moore and Smith, 1986; Bacon et al., 1989b; Darbyet al., 1989). It has been reported that the sediment in-ventory of 230Th from Canada Basin were only about30% of what was expected from the overhead produc-tion from the water column (Ku and Broecker, 1967).Finkel et al. (1977), based on 10Be measurements on twosediment cores from Canada Basin of the Arctic (80°N),showed that the deposition rates of 10Be in the Arctic areabout 3±5 times lower than those observed for otheroceanic regimes. This was partly attributed to the de®-ciency of particulate scavengers. Bacon et al. (1989b)reported that the surface water (85°500N, 108°500W) wascharacterized by an exceptionally low rate of Th scav-enging, even in comparison with other oligotrophicoceans. This slow scavenging of Th results in higher230Th concentrations in the water column and Baconet al. (1989b) reported substantially higher 230Th con-centrations compared to other ocean basins at compa-rable depths.

TABLE 3

Measured and expected inventories of 230Th and scavenging e�ciency in sediment cores from the world ocean.

Area Sedimentary 230Thinventory (dpm cmÿ2)

Production of 230Thinventory (dpm cmÿ2)

Scavenginge�ciencya (%)

References

Atlantic and Indian Ocean(compiled data)2000±3000 m 770� 110 800 96:3� 13:83400±4600 m 835� 200 1220 68:4� 16:4 Kadko (1980)4600±5800 m 1110� 135 1540 72:1� 8:7

Norwegian Sea 68°29.70N 0°49.10E(2802 m)

664� 15 785 84:6� 1:9 Scholten et al. (1994a)

Norwegian±Greenland Sea 72°1.80N9°15.90E (2518 m)

866� 13 705 123� 2 Scholten et al. (1994a)

Greenland Sea 76°31.20N 3°57.50E(2485 m)

441� 8 696 63:4� 1:2 Scholten et al. (1994a)

Arctic Ocean 77°380N 173°430W(1856 m)

120 520 23.1 Finkel et al. (1977)

Arctic Ocean 88°350N 149°270W(2871 m)

200 804 24.9 Finkel et al. (1977)

a Scavenging e�ciency � (sediment 230Th inventory/production of 230Th inventory)� 100.

20

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Page 6: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

The sediment inventory of 230Th for the world oceanis presented in Table 3. The scavenging e�ciency[� (sediment inventory of 230Th/production of 230Thinventory) �100] in the subpolar oceans varies between68% and 96% (Kadko, 1980). The scavenging e�ciencyis notably low in the Canada Basin. However, it is in-teresting to note that the scavenging e�ciency of 230Thin the Nansen Basin is comparable to subpolar regions.This di�erence in the scavenging e�ciency between theNansen Basin and Canada Basin of the Arctic could beeither due to di�erences in the particle concentrationsand/or ventilation rates. One can infer some observa-tions based on the sedimentation rates from these areas,even though the extensive data base on the particleconcentrations from Arctic Basins do not exist. Thesedimentation rates in the Arctic Ocean, obtained usingexcess 230Th, extrapolated ages from 14C dates andstratigraphic chronologies using d18O isotopes are pre-sented in Table 4. The average sedimentation rate in theCanada Basin is between 0.09±0.24 cm/103 yr (0.09±0.24cm kyÿ1, Ku and Broecker, 1967; Finkel et al., 1977)while the values in high-latitude areas in the Norwe-gian±Greenland Sea and Nansen Basin are approxi-mately an order of magnitude higher (1.3±4.4 cm kyÿ1,Scholten et al., 1990, 1994a,b). Since the sedimentationrates in the Nansen Basin are about an order of mag-nitude higher than the Canada Basin, it is likely that thelow inventory of 230Th in the Canada Basin is likely dueto the low particle ¯ux in that area.

The mean residence times of the Arctic waters spanover three orders of magnitude, ranging from less than ayear to several hundred years (Schlosser et al., 1993).From the observations of Wallace et al. (1987, 1992) ithas been shown that the freon inventories in the watercolumn of the central Nansen Basin are relatively highcompared to the central Canada Basin, indicating rela-tively rapid ventilation in the Nansen Basin comparedwith the Canada Basin (Cochran et al., 1995). Thus, it isnot clear which of the two factors (particle concentra-tions and ventilation rates) that control the removal of

Th and other particle-reactive pollutants in these twoArctic Basins are dominant. More simultaneous studiesdealing with the particle concentrations and their ¯uxesand Th isotope measurements in the Arctic water col-umn and determination of ventilation rates in theseplaces are needed to address this question.

Conclusions

This study clearly shows that there is a distinct dif-ference in the scavenging of Th isotopes, and by impli-cation, other particle-reactive pollutants, between theCanada Basin and the Nansen Basin of the Arctic. Thescavenging e�ciency of 230Th in both regions, for ap-proximately the same latitude, di�ers considerably. Thisdi�erence is attributed to the low particle ¯ux inferredfrom the di�erences in sedimentation rates and/or dif-ferences in the ventilation rates of the two basins. Fromthe published data on the sedimentation rates in thesetwo basins, it appears that di�erences in particle ¯ux isprobably the primary reason for the slow scavenging ofparticle-reactive nuclides in the Canada Basin.

This work was in part supported by the National Science Foundation(grant number: NSF-OPP-9996337).

Anderson, R. F., Bacon, M. P. and Brewer, P. G. (1983a) Removal ofTh-230 and Pa-231 from the open ocean. Earth and PlanetaryScience Letters 62, 7±23.

Anderson, R. F., Bacon, M. P. and Brewer, P. G. (1983b) Removal ofTh-230 and Pa-231 at ocean margins. Earth and Planetary ScienceLetters 66, 73±90.

Bacon, M. P. and Rutgers van der Loe�, M. R. (1989a) Removal ofthorium-234 by scavenging in the bottom nepheloid layer of theocean. Earth and Planetary Science Letters 92, 157±164.

Bacon, M. P., Huh, C.-A. and Moore, R. M. (1989b) Vertical pro®lesof some natural radionuclides over the Alpha Ridge, Arctic Ocean.Earth and Planetary Science Letters 95, 15±22.

Barrie, L. A. (1986) Arctic air pollution: an overview of currentknowledge. Atmospheric Environment 20, 643±663.

Barnes, P. W., Reimnitz, E. and Fox, D. (1982) Ice rafting of ®ne-grained sediment, a sorting and transport mechanism, Beaufort Sea,Alaska. Journal of Sedimentary Petrology 52, 493±502.

TABLE 4

Sedimentation rates in the deep Arctic Basins obtained using 230Thexcess,14C and stratigraphic chronology using d18O isotopes.

Area Depth (m) Sedimentation rates (cm kyÿ1) References

Norwegian Sea 68°29.70N; 0°49.10E 2802 2.0 Scholten et al. (1994a)

Norwegian Sea 2281 1.59 Scholten et al. (1994a)70°18.30N; 3°7.40W

Norwegian±Greenland Sea 72°1.80N 9°15.90E 2518 4.37 Scholten et al. (1994a)

Greenland Sea 76°31.20N 3°57.50E 2485 1.25 Scholten et al. (1994a)

Fram Strait±Nansen Basin 78°300N; 02°E �3000 2±3 Scholten et al. (1990)

Canada Basin±Arctic Ocean 77°380N 173°430W 1856 0.24a Finkel et al. (1977)

Canada Basin±Arctic Ocean 82°560N 155° 540W 3437 0.20 Ku and Broecker (1967)

Canada Basin±Arctic Basin 88°350N 149°70W 2871 0.09a Finkel et al. (1977)

a Linear sedimentation rates were calculated from the porosity and mass accumulation rates.

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Page 7: Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

Baskaran, M. and Naidu, A. S. (1995) 210Pb-derived chronology andthe ¯uxes of 210Pb and 137 Cs isotopes into continental shelfsediments, East Chukchi Sea, Alaskan Arctic. Geochimica Cosmoc-hima Acta. 59, 4435±4438.

Baskaran, M. and G. E. Shaw (2000) Residence time of Arctic hazeaerosols using the concentrations and activity ratios of 210 Po, 210 Pband 7Be. Journal of Aerosol Science (in press).

Baskaran, M., Santschi, P. H., Guo, L., Bianchi, T. S. and Lambert, C.(1996) 234Th: 238U disequilibria in the Gulf of Mexico: theimportance of organic matter and particle concentration. Conti-nental Shelf Research 16, 353±380.

Bhat, S. G., Krishnaswami, S., Lal, D., Rama and Moore, W. S. (1969)234Th 238U ratios in the ocean. Earth and Planetary Science Letters5, 483±491.

Broecker, W. S., Kaufman, A. and Trier, R. M. (1973) The residencetime of thorium in surface sea water and its implications regardingthe fate of reactive pollutants. Earth and Planetary Science Letters20, 35±44.

Buesseler, K. O., Bacon, M. P., Cochran, J. K., and Livingston, H. D.(1992) Carbon and nitrogen export during the JGOFS NorthAtlantic bloom experiment estimated from 234Th-238U disequilibria.Deep-Sea Research 39, 1115±1137.

Coale, K. H. and Bruland, K. H. (1985) 234Th±238U disequilibria withinthe California Current. Limnology and Oceanography 30, 22±33.

Coale, K. H. and Bruland, K. H. (1987) Oceanic strati®ed euphoticzone as elucidated by 234Th: 238U disequilibria. Limnology andOceanography 32, 189±200.

Cochran, J. K., Hirschberg, D. J., Livingston, H. D., Buesseler, K. O.and Key, R. M. (1995) Natural and anthropogenic radionuclidedistributions in the Nansen Basin, Arctic Ocean: scavenging ratesand circulation time scales. Deep-Sea Research 42, 1495±1517.

Cooper, L. W., Larsen, I. L., Beasley, T. M., Dolvin, S. S., Grebmeier,J. M., Kelley, J. M., Scott, M. R. and Johnson-Pyrtle, A. (1998) Thedistribution of radiocesium and plutonium in sea ice-entrainedArctic sediments in relation to potential sources and sinks. Journalof Environmental Radioactivity 39, 279±303.

Darby, D. A., Naidu, A. S., Mowatt, T. C. and Jones, G. (1989)Sediment composition and sedimentary processes in the ArcticOcean. In The Seas Climatology, Oceanography, Geology, andBiology, ed. Y. Herman, pp. 657±720. Van Nostrand Reinhold,New York.

Dorsey, H. G. and Peterson, W. H. (1976) Tritium in the Arctic Oceanand East Greenland Current. Earth and Planetary Science Letters32, 342±350.

Edmonds, H. N., Moran, S. B., Ho�, J. A., Smith, J. N. and Edwards,R. L. (1998) Protoactinium-231 and thorium-230 abundances andhigh scavenging rates in the Western Arctic Ocean. Science 280,405±407.

Feely, H. W., Larsen, R. J. and Sanderson, C. G. (1989) Factors thatcause seasonal variations in Beryllium-7 concentrations in surfaceair. Journal of Environmental Radioactivity 9, 223±249.

Finkel, R., Krishnaswami, S. and Clark, D. L. (1977) 10Be in ArcticOcean Sediments. Earth and Planetary Science Letters 35, 199±204.

Hermanson, M. H. (1990) 210Pb and 137Cs chronology of sedimentsfrom small, shallow Arctic lakes. Geochimica Cosmochimica Acta54, 1443±1451.

Honjo, S. (1990) Particle ¯uxes and modern sedimentation in the Polarregions. In Polar Oceanography-Part-B: Chemistry, Biology, andGeology, ed. W. O. Smith, pp. 687±739. Academic Press, New York.

Landa, E. R., Reimnitz, E., Beals, D. M., Pochkowski, J. M., Winn,W. G. and Rigor, I. (1998) Transport of 137Cs and 239;240Pu with ice-rafted debris in the Arctic Ocean. Arctic 51, 27±39.

Kadko, D. (1980) 230Th 226Ra, and 222Rn in abyssal sediments. Earthand Planetary Science Letters 49, 360±380.

Kempema, E. W., Reimnitz, E. and Barnes, P. W. (1989) Sea icesediment entrainment and rafting in the Arctic. Journal ofSedimentary Petrology 59, 308±317.

Ku, T. L. and Broecker, W. S. (1967) Rates of sedimentation in theArctic Ocean. In: Progress in Ocenography, vol. 4, pp. 95±104.Pergamon Press, Oxford and New York.

Li, Y.-H., Feely, H. W. Toggweiler, J. R. (1980) Ra-228 and Th-228concentrations in GEOSECS Atlantic surface waters. Deep-SeaResearch 27A, 545±555.

Moore, R. M. and Smith, J. N. (1986) Disequilibria between 226Ra,210Pb and 210Po in the Arctic Ocean and the implications forchemical modi®cation of the Paci®c water in¯ow. Earth andPlanetary Science Letters 77, 285±292.

Nichols, H. (1967) The disturbance of Arctic lake sediments by`bottom ice': a hazard for palynology. Arctic 20, 213±214.

P®rman, S. L., Eicken, H., Bauch, D. and Weeks, W. F. (1995) Thepotential transport of pollutants by Arctic sea ice. Science of theTotal Environment 159, 129±145.

Rahn, K. A. (1981) Relative importances of North America andEurasia as sources of Arctic aerosol. Atmospheric Environment 15,1447±1455.

Rahn, K. A. (1982) On the causes, characteristics and potentialenvironmental e�ects of aerosols in the Arctic atmosphere. In TheArctic Ocean, ed. L. Rey, pp. 163±195. Wiley, New York.

Rahn, K. A. and McCa�rey, R. J. (1980) On the origin and transportof the winter Arctic aerosols. Ann. N. Y. Acad. Science 338, 486±503.

Reimnitz, E., McCormick, M., McDougall, K. M. and Brouwers, E.(1993) Sediment export by ice rafting from a coastal polyna, ArcticAlaska, USA. Arctic and Alpine Research 25, 83±98.

Rey, L. (1982) The Arctic Ocean: a `Polar Mediterranean'. In TheArctic Ocean, ed. L. Rey, pp. 29±41. Wiley, New York.

Santschi, P. H., Nixon, S., Pilson, M. and Hunt, C. (1984) Accumu-lation of sediments, trace metals (Pb, Cu) and hydrocarbons inNarragansett Bay, Rhode Island. Estuarine and Coastal ShelfScience 19, 427±449.

Schlosser, P., Swift, J. H. and Lewis, D. (1993) Large-scale circulationof the Arctic Ocean: implications for pollutant transport. InProceedings of the Radioactivity and Environmental Security in theNew Research and Policy Priorities in the Arctic and North Atlantic,Woods Hole Oceanographic Institution, Massachusetts, USA, pp.285±299.

Scholten, J. C., Botz, R., Mangini, A., Paetsch, H., Sto�ers, P. andVogelsang, E. (1990) High-resolution Th-230(ex) stratigraphy ofsediments from high-latitude areas (Norwegian Sea, Fram Strait).Earth and Planetary Science Letters 101, 54±62.

Scholten, J. C., Botz, R., Mangini, A., Paetsch, H., Sto�ers, P. andVogelsang, E. (1994a) High resolution 230Thex stratigraphy ofsediments from high-latitude areas (Norwegian Sea, Fram Strait).Earth and Planetary Science Letters 101, 54±62.

Scholten, J. C., Botz, R., Paetsch, H. and Sto�ers, P. (1994b) 230Thex

¯ux into Norwegian±Greenland Sea sediments: evidence for lateraltransport during the past 300 000 years. Earth and Planetary ScienceLetters 121, 111±124.

Talbot, R. W., Vijgen, A. S. and Harriss, R. C. (1992) Soluble speciesin the Arctic summer troposphere: acidic gases, aerosols, andprecipitation. Journal of Geophysical Research 97, 16 531±16 543.

Tolmazin, D. (1985) Elements of Dynamic Oceanography. Allen &Unwin, Winchester, MA.

Wallace, D. W. R., Moore, R. M., and Jones, E. P. (1987) Ventilationof the Arctic Ocean cold halocline: rates of diapycnal and isopycnaltransport, oxygen utilization, and primary production inferredusing chloro¯uromethane distributions. Deep-Sea Research 34,1957±1979.

Wallace, D. W. R., Schlosser, P., Krysell, M. and Bonish, G. (1992)Halocarbon ratio and tritium/3He dating of water masses in theNansen Basin, Arctic Ocean. Deep-Sea Research 39, S435, S458.

Wheeler, P. A., Gosselin, M., Sherr, E., Thibault, D., Kirchman, D. L.,Benner, R. and Whitledge, T. E. (1996) Active cycling of organiccarbon in the central Arctic Ocean. Nature 380, 697±699.

Wheeler, P. A., Watkins, J. M. and Hansing, R. L. (1997) Nutrients,organic carbon, and organic nitrogen in the upper water column ofthe Arctic Ocean: implications for the sources of dissolved organiccarbon. Deep-Sea Research 44, 1571±1592.

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Marine Pollution Bulletin