GEOPHYSICAL RESEARCH LETTERS, VOL. 25, NO. 19, PAGES 3547-3550, OCTOBER 1, 1998 Methane in surface waters of the Arabian Sea H.W.Bange, R.Ramesh, • S.Rapsomanikis, 2andM.O.Andreae Biogeochemistry Department,Max PlanckInstitutefor Chemistry,Mainz, Germany Abstract. More than 2000 measurementsof atmosphericand dissolvedmethane (CH4) were performed in the central and northwestern Arabian Sea as part of the GermanJGOFS Arabian Sea ProcessStudy during three cruisesin March, May/June, and June/July1997. Mean CH4 saturationsin the surfacewatersof the centralArabianSeawere in the rangeof 103-107%. Significantly enhancedsaturations were observedin the coastalupwellingarea at the coastof Oman (up to 156%) and in an upwellingfilament (up to 145%). The CH4 surfaceconcentrations in the upwelling areawerenegativelycorrelatedto seasurfacetemperatures. Areaweighted,seasonallyadjustedestimatesof the sea-air fluxes of CH4 gave annual emissionsfrom the Arabian Sea of 11-20 Gg CH4, suggestingthat previouslyreportedvery high surface CH4 concentrations might be atypical owing to the interannual variabilityof the Arabian Sea and that the emissionsderivedfrom themareprobablyoverestimates. andthe southwest(SW) monsoonperiodsof 1997. Basedon our data we presentan area-weighted,seasonallyadjustedCH4 flux estimatefor the ArabianSea.The threecruiselegswerepart of the 1997 German JGOFS (Joint Global Ocean Flux Study) Arabian Sea ProcessStudy and took place during March (leg SO117), May/June(leg SO119), and June/July(leg SO120) on the GermanresearchvesselR/V $onne.Legs SO117 and SO119 coveredmainly the central Arabian Sea, whereasleg SO120 focusedon the coastalupwelling area off the Arabian Peninsula (Figure 1). 30 t •• _ Gulf ofOmen Persian Gulf ARABIA Introduction z Atmospheric methane(CH4) is a greenhouse gasandplaysan importantrole in both tropospheric and stratospheric chemistry [Cicerone and Orerntand, 1988; LelieveM et al., 1993]. Therefore,it is necessary to evaluatethe contributionsof natural and anthropogenic sourcesto estimatethe global budgetof atmospheric CH4. The world'soceans,asa naturalsourceof CH4, playonlya minorrole in the globalbudgetof atmospheric CH4 [Hein et at., 1997; Matthews,1994]. However,recentglobal estimates of the oceanicCH4 emissions differ considerably and 20 Musc•i'•-•'"" / "• gr. OMA"/• I• .AST"'"• '• INIA I SOMALIA / -SAST 10 o (a) [/ Arabian Sea 30 , rangefrom0.4 to 15 Tg CH4yr-• [Bangeet at., 1994;Bateset (b) al., 1996],indicatinga needfor furtherstudy. Biologicallyproductive regions(e.g.,shelfareas)whichcover only about 16% of the world's ocean area appearto be responsible for about75% of the oceanicCH4emissions [Bange et al., 1994]. The ArabianSeahasonly a smallportionof shelf areas;however,it is one of the most biologicallyproductive regionsof the world'soceans.Sincethe studyof Owenset al. [ 1991] in 1986,it wasspeculated thattheArabianSea,especially its upwelling-dominated northwestern part,represents a hot spot for CH4 emissions,making a substantialcontributionto the globalbudgetof oceanicemissions. Herewe presentmorethan2000 measurements of atmospheric and dissolvedCH4 in the ArabianSeaduringthe intermonsoon ARA . 2o OMAN •' • transect lO t? •-u-• Djibouti • INDIA 17 .. Arabian Sea •,- 0 40 • I • 50 I 60 70 8O Longitude, OE • Institutefor OceanManagement, AnnaUniversity, Chennai,India. 2nowat: Laboratoryof AtmosphericPollutionScienceand Technology, DemokritosUniversityof Thrace,Xanthi,Greece. Copyright1998 by the AmericanGeophysicalUnion. Figure 1. Cruisetracksof the R/V $onne:(a) leg SO119, from Muscat (Oman) to Muscat, May/June 1997, (b) leg SOl17 (dashedline) from Cochin (India) to Muscat, March 1997; leg SO120 (solid line) from Muscatto Djibouti, June/July1997. The cruisetracksshownindicatethe partsof the legs when CH4 was measured.The positionsof some prominentstationsand cruise Papernumber98GL02710. features 0094-8534/98/98GL-02710505.00 coastalupwellingduringthe SW monsoon. 3547 are marked. The hatched area indicates location of 3548 BANGE ET AL.: METHANE IN SURFACE WATERS OF THE ARABIAN SEA 2OO Methods " -4'-'""/' ""' '"' -''''"'e"" '"ø•' "- ...... (a) -.- • ,-, .. ,.,,,..,"' CH4 wasdeterminedwith a gaschromatograph equippedwith o• 180 ," a flame ionizationdetector.Furtherdetailsof the analysissystem • O 160 EAST SAST are describedin Bange et al. [1994]. Seawaterwas pumped • NAST I CASTWAST P01 continuously from a depthof approximately6.5 m into a shower 30 , 26 filament K03 22 t typeequilibrator developed by R. F. Weiss(Scripps Institution of 2]• Oceanography, La Jolla, CA). Duringthe threelegs,the mean differencesbetweenthe watertemperatureat the seachestandthe continuously recordedwatertemperature in the equilibratorwere in the rangeof-0.003 to -0.05 øC. Concentrations andresulting saturation values were corrected for these differences. A series of measurementson seawaterand ambient air followed by two standards (1.70 _+2 % and 3.06 + 2 % ppmCH4 in syntheticair) I 100 '-'Itt•' o o o .9.o • '• .9.o .9.o • I • ' 10 ... 20O : 180 was repeatedevery 80 min. The gravimetricallypreparedgas standards were calibrated by the manufacturer (DEUSTE Steininger GmbH,MQhlhausen, Germany)againststandards from the U.S. National Institute of Standards and Technology (Gaithersburg, MD). The analyticalprecision,calculatedas the ratio of the standarddeviationof the atmosphericmeasurements to the mean atmosphericmixing ratio, was 1.6% (SOl19, SO120). The mean relative errorsof the CH4 saturationand concentration,were 2.2% and 1.6% during legs SOl19 and .9.o drift study transect dnft study (b) 30 i' :;: ::i:: j:i ! : : ' •, ' "' '•'l .. ;", : i :\.."o ':' ','.'-,.,-5,.'v":"F'",,'-'/-";-'-;-' •6o ' 140 ,',: '•; ' "';" t :" ' B C ! 120 14 100 • : o o o ,- ,- ,- o o , 10 o o date, 1997 SO120,respectively. Dueto technicalproblems theprecisionand relativeerrorsduringleg SO117 were approximately twice those Figure2. CH4 saturations (solid lines) and sea surface for the legsSO119 and SO120. Saturationvalues(expressed in temperatures(dashedlines) during (a) leg SOl19 and (b) leg %, i.e., 100% = equilibrium) were calculatedby applyingthe solubility equation of Wiesenburg and Guinasso [1979]. Continuoustime series of seawatertemperature,salinity, and wind speedwereobtainedfromthe ship'srecords. SO120. For orientation,prominentstationsand cruise features aremarked(seeFigure 1). features of the SW monsoon triggered upwelling off Oman [Elliott and Savidge,1990]. In the centralArabian Sea (Figure 2a) we observedno trend The observedmeanatmosphericCH4 dry mole fractionswere for the CH4 saturations.Even at stationP01 when we touchedthe 1.81 + 0.06 ppm (March) and 1.69 + 0.03 ppm (May-July). Due beginning of coastal upwelling, no increase in the CH4 to the seasonalnorthwardshift of the intertropicalconvergence saturationswas detectable.In contrast,when we found a filament, zone, which is most pronouncedduringthe SW monsoonin the a narrow band of upwelled water from the coast [Elliott and summermonths,air massessampledduringMay-July were from Savidge, 1990], centeredapproximatelyat 20.5øN, 60.5øE, the the southernhemisphere,whereasthose sampledduring March CH4 concentrationsduring a 2-day survey were negatively werefrom the northernhemisphere. From 14 May until the onset correlatedwith sea surfacetemperatures.Maximum saturations of the SW monsoonon 23 May we observeda trend from 1.80 to (up to 145%) were measuredat stationK03 (23.4øN,60.1øE) 1.69 ppmCH4, indicatingthe transitionfrom northernto southern located at the entrance to the Gulf of Oman. In the coastal hemisphereair masses.The observedatmosphericvaluesare in upwelling area (Figure 2b), which was investigatedduring leg agreementwith CH4 measurementsat the baselinemonitoring SO120 (June/July),we generallyfound elevatedCH4 saturations stationsMace Head, Ireland and Cape Grim, Tasmania.Monthly associatedwith low sea surfacetemperatures.Maximum CH4 mean values (excludingdata biasedby pollution events)were saturations (up to 156%) were observedin the northernpart of 1.803+ 0.013 ppm (Mace Head,March 1997) and 1.693+ 0.003 the coastalarea.EnhancedCH4 valueswere alsofoundduringa ppm(CapeGrim, May-July 1997).Thesevalueswerecalculated drift studyin the coastalupwelling(19-30 June,continued4-7 from the Advanced Global Atmospheric Gases Experiment July), whereassignificantlylower saturationswere observedat (AGAGE)dataset(updated versionfrom18May 1998)available the transectto the centralArabianSea(Figure2b). from the anonymoustip site cdiac.esd.ornl.edu (subdirectory Figure 3 shows a plot of SST vs. CH4 concentrationto With the exceptionof /pub/ale_gage_Agage/Agage/monthly) at the Carbon Dioxide illustratethe role of upwellingprocesses. the data from stationK03, high CH4 surfaceconcentrations are InformationAnalysisCenterin OakRidge,Tennessee. Mean CH4 water concentrations in the centralArabian Sea associatedwith low SST. Interestingly,the regressionlines are were2.09+ 0.30nmolL-• (March)and1.82+ 0.09nmolL-] aboutthe samefor both the coastalupwellingand the filament, (May/June). Enhanced values (mean2.25+ 0.10nmolL-], despitethe factthattheyarewell separatedfeatures.The negative mightbe dueto June/July) were foundin the coastalupwellingarea.Figure2 correlationbetweenSST and CH4 concentrations shows the CH4 saturationsduring legs SOl19 and SO120 the mixing of upwelled water masses with high CH4 Results and Discussion togetherwiththe seasurfacetemperatures (SST) asan indicator concentrations and water masses from the central Arabian Sea for upwelledwatermasses, whichcouldbe easilyidentifiedby with low CH4 concentrations.It seemsthat CH4 is formedin situ watertemperatures lowerthan30 øC(SO119)or 28 øC(SO120). in the subsurfacelayer [Owenset aL, 1991; Patra et al., 1998] Temperature differences up to 10øC betweennearshore (i.e., andthenbroughtto the surfacein the courseof upwellingevents freshlyupwelled)andoffshoresurfacewatersare characteristicduring the SW monsoon.As there was no indication from BANGE ET AL.: METHANE IN SURFACE WATERS OF THE ARABIAN SEA CH4 oxidation.However, in the adjacentnorthernand southern areasPatraet al. [ 1998]foundmeanCH4saturations in the range of 202 to 222%, so that downwelling would lead to CH4 enrichment becauseof the subsequent horizontaltransportof CH4 enriched water masses. Moreover, CH4 oxidation in oceanic surfacewatersis usuallytoo slow to representa significantsink for dissolvedCH4 [donesand Amador, 1993; dones, 1991]. Filaments, characteristicfeatures of the SW monsoon, show widthsup to 150 km and can extendup to 400 km offshorefrom the coastof the Arabian Peninsula[Arnoneet al., 1998]. As 3.0 coastal upwelling 2.8 n n 2.4 xx 2.2 SO1•9 •.•o _•••,• ..... Eq • .6 1.4 i 16 o o • I 18 • I 20 • I 22 • I 24 • •, . x i.x a • cen•al Mabi• Sea • I 26 I I 28 • I 30 3549 • 32 indicatedby 'our data,they are able to transportCH4 enriched SST, øC surfacewatersoffshore(Figure2a). Thus,filamentstructures lead Figure3. Dissolved CH4 concentrationvs. sea surface to CH4 supersaturationthan undersaturation in the central in temperaturein the coastalnorthwesternArabian Sea during the ArabianSeaduringthe SW monsoon.High surfacesaturations as foundby SW monsoon1997. Opentrianglesindicatedatafrom May/June the centralArabianSea duringthe intermonsoon, (leg SO119), asterisksindicatedatafrom stationK03 (June,leg Patra et al. [1998], might be an indication of a considerable SOl19), and open squaresindicate data from June/July(leg interannualvariabilityof the Arabian Sea. SO120). Eq indicatesthe theoreticalequilibriumconcentrations CH4 air-sea exchange.The CH4 exchangeflux density,F in calculatedwith mean atmosphericdry mole fractionsof 1.7 ppm pmol m-2S-1,Canbeparameterized asF = kw(C•- C,,),where kw and 1.8 ppm CH4, respectively.The parametersof the linear is the gas transfercoefficient,C• is the seawaterconcentration, regressions are:y= -0.090x+ 4.446,r2= 0.62,n = 539(SO119) calculated usingthe andy =-0.091x + 4.402,r2 = 0.76, n = 47 (SO120);both andC,,is theequilibriumwaterconcentration atmosphericdry mole fraction.To calculatekw,we correlationsare significant at the 0.1% level. The two large corresponding used the tri-linear kw/windspeed relationshipfrom Liss and circlesindicatepossiblemixing endmembersat 28-31 øC (central Merlivat [1986] (hereinafter referred to as LM86) or, ArabianSea)and 18 øC (upwelling)[Elliott and Savidge,1990]. alternatively,the quadratickw/windspeedrelationshipestablished by Wanninkhof [1992] (hereinafterreferredto as W92). The coefficients kwwereadjustedby multiplyingwith (Sc/600)-"(n = _<3.6ms-1 andn = 0.5 forwindspeeds > temperaturedata for upwellingat stationK03 at the time of our 2/3 forwindspeeds -øsforW92.ScistheSchmidt measurements, these enhancedCH4 concentrationsmight result 3.6ms-1)forLM86and(Sc/660) from CH4 enrichedwatersfrom the Gulf of Oman. numberfor CH4 andwascalculatedusingempiricalequations for An overview of the mean saturationsfor variousregionsof the the kinematicviscosityof seawater[Siedler and Peters, 1986] Arabian Sea is given in Table 1. The data from the central and the diffusivity of CH4 in water [dahne et al., 1987]. The Arabian Sea are in very good agreementwith data from the measuredwind speedswere normalizedto 10 m heightby using Pacific and Atlantic Oceans [Bates et al., 1996; Conrad and the relationshipof Garratt[ 1977]. In orderto obtainan estimateof the annualCH4 emissions,we Seiler, 1988], but our saturationvalues are considerablylower than thosepublishedpreviouslyfor the Arabian Sea. The first structuredour data into those from the central Arabian Sea, the CH4 measurementfrom the Arabian Sea was reported by coastal upwelling areas, and the filament (i.e., open ocean Lamontagneet al. [1973]. They measured168% saturationin a upwelling) area. Then, we calculatedmean flux densitiesand regimesfrom the observed single sample from the central Arabian Sea sampledin June emissionsfor the threeoceanographic 1967. Owenset al. [1991] reportedfor the central(on a transect flux densities(Table 2). We assumedthat our measurements are along 67øE) and northwesternArabian Sea (i.e., the coastal representativefor the intermonsoon (Oct.-May) and SW upwellingarea and the Gulf of Oman) an averageCH4 surface monsoon(June-Sept.).By addingthe seasonalemissionslistedin saturationof 192 + 34% during the decline of the SW monsoon Table 2, we obtainmean annualCH4 emissionsin the rangefrom in September/October 1986. Recently,Patra et al. [1998] found 11 (LM86) to 20 Gg CH4 (W92). Our estimateis considerably in the central and easternArabian Sea mean values of 140 + 37%, lower than > 40 Gg and 30-50 Gg of Owens et al. [1991] and 173 + 54%, and 200 + 74% in February/March1995, April/May Patra et al. [1998], respectively.Their higher estimatesare the 1994, and July/August 1995, respectively. Summarizing the result of extrapolatinghigh CH4 concentrationsfrom upwelling results from the various CH4 measurementsin the Arabian Sea, areas.Extrapolationof our flux densitydata from the upwelling we foundsubstantialdifferenceswhich might be partly causedby area(Table 2), usingthe areavalue of Owenset al. [1991] (1.56 x m2),whichwasalsoapplied byPatraet al. [1998],indicates the interannualvariability of the Arabian Sea and/or different 1012 spatialdata coverage.For example,the data from Owens et al. the annual emissionswould be in the range of 13-22 Gg CH4. [1991] are biasedby the fact that 8 from 13 samplingstations were locatedin the CH4 enrichedwatersof the Gulf of Oman and Table 1. Mean CH4 SurfaceSaturations(% + 1(•) in the Arabian in the upwellinginfluencedareaoff Oman. We observed no overall seasonal trend for the central Arabian Sea (Table 1). A possibleseasonalitymight be maskedby the differentarea coverageof the cruisesand by the scatterof the data for March as indicated by the relatively high standard deviation (Table 1). In contrast,Patra et al. [1998] found an overall seasonalshift of the CH4 saturationsalong 64øN from 96% (SW Monsoon) to 166 + 3% (Intermonsoon).Patra et al. [1998] arguedthat the observedundersaturation,which is based on two observationsonly, might be causedby downwellingand Sea. The Numbers in Parenthesis Indicate the Number of Measurements. March 1997 May/June1997 June/July1997 CentralArabianSea 106 + 12 (135) 107 + 4 (254) 103 + 2 (74) Coastalupwelling • 107+ 2 (6) 116+ 8 (463) Filament • 113 + 5 (46) not measured Entranceto Gulf of Oman not measured 124 + 9 (47) 124 + 7 (3) 3550 BANGE ET AL.: METHANE IN SURFACE WATERS OF THE ARABIAN SEA Table2: MeanCH4emissions fromtheArabian Seaduring1997. References Amone, R.A., R.W. Gould, J. Kindle, P. Martinolich,K. Brink, and C. Area a Fluxdensity b Emissions b Lee, Remotesensingof coastalupwellingand filamentsoff the coast 1012 m2 pmolm-2s-1 GgCH4 of Oman(abstract),Oceanogr.,11 (No. 2 Supplement), 33, 1998. Bange,H.W., U.H. Bartell, S. Rapsomanikis, and M.O. Andreae, Intermonsoon Methane in the Baltic and North Seas and a reassessment of the ArabianSea(central+ upwelling) 7.0 2.0 / 3.7 4.7 / 8.8 marineemissionsof methane,Global Biogeochem.Cycles,8, 465480, 1994. SW Monsoon Central Arabian Sea 6.3 4.2 / 7.9 4.5 / 8.4 CoastalUpwelling 0.2 15.9/ 27.9 0.5 / 0.9 Filaments 0.5 12.3 / 21.6 1.0 / 1.8 SUM (= annualmean) 10.7/ 19.9 a Data taken from KOrtzingeret al. [1997] (central Arabian Sea includesthe Gulf of Oman). Bates,T.S., K.C. Kelly, J.E. Johnson,andR.H. Gammon,A reevaluation of the openoceansourceof methaneto the atmosphere, or. Geophys. Res., 101, 6953-6961, 1996. Cicerone, R.J., and R.S. Oremland, Biogeochemicalaspects of atmospheric methane,GlobalBiogeochem. Cycles,2, 299-327, 1988. Conrad,R., andW. Seiler,Methaneand hydrogenin seawater(Atlantic Ocean),Deep-SeaRes.,35, 1903-1917, 1988. Elliott,A.J., andG. Savidge,Somefeaturesof the upwellingoff Oman,or. Mar. Res., 48, 319-333, 1990. • Firstvaluecalculated according toLissandMerlivat[1986];second Garratt,J.R., Reviewof the dragcoefficientsoveroceansand continents, valuecalculatedaccordingto Wanninkhof[1992]. Mo. Weath.Rev., 105, 915-929, 1977. Hein, R., P.J.Crutzen,andM. Heimann,An inversemodelingapproach to investigatethe global atmosphericmethane cycle, Global Biogeochem. Cycles,11, 43-76, 1997. Althoughthis is an overestimation dueto neglectof seasonal Jahne,B., G. Heinz, and W. Dietrich, Measurementsof the diffusion variability,this value is still significantlylower than the coefficientsof sparinglysolublegasesin water,or. Geophys.Res.,92, we certainlyoverestimate the emissionsfor the open ocean 10,767-10,776, 1987. Jones, R.D., Carbon monoxide and methane distribution and consumption in the photiczone of the Sargasso Sea,Deep-SeaRes., 38, 625-635, 1991. Jones, R.D., and J.A. Amador, Methane and carbon monoxide upwellingareasbecauseof the high temporaland spatial variabilityof filamentstructures, and (3) we cautionthat our production, oxidation,and turnovertimes in the CaribbeanSea as influencedby the OrinocoRiver, or. Geophys.Res., 98, 2353-2359, previously published values.Ourannualestimate 11-20GgCH4 (Table2) exhibitsthreepointsof uncertainties: (1) we haveno datafrom the Somaliand the westernIndian shelfupwelling,(2) estimateis basedon data from two seasonswithin the sameyear and thus doesnot take into accountthe interannualvariabilityof 1993. KOrtzinger, A., L. Mintrop, andJ.C. Duinker,StrongCO2emissions from the Arabian Sea during the South-WestMonsoon, Geophys.Res. the Arabian Sea. Lett., 24, 1763-1766, 1997. Lamontagne, R.A., J.W. Swinnerton,V.J. Linnenbom,and W.D. Smith, Methaneconcentrations in variousmarine environments, or. Geophys. Conclusions Res., 78, 5317-5325, 1973. Lelieveld,J., P.J. Crutzen,and C. Brtihl, Climateeffectsof atmospheric Summarizingthe resultsof variousCHn measurements in the methane,Chemosphere, 26,739-768, 1993. surface water of the Arabian Sea, we conclude that the Liss, P.S., and L. Merlivat, Air-sea exchangerates:Introductionand synthesis, in TheRole of Air-Sea Exchangein GeochemicalCycling, considerable temporaland spatialvariabilityof the hydrographic edited by P. Buat-M6nard, pp. 113-127, D. Reidel Publishing settingsmay lead to significantinterannualdifferencesand thus, Company,Dordrecht,1986. complicatesdirect comparisons.The area-weighted,seasonally Matthews, E., Assessmentof methane sourcesand their uncertainties, adjustedestimateof the annual CH4 emissionsfrom the Arabian PureandAppl. Chem.,66, 154-162, 1994. Sea(givenin Table 2) suggests thatpreviouslyreportedveryhigh Owens, N.J.P., C.S. Law, R.F.C. Mantoura, P.H. Burkill, and C.A. Llewellyn,Methane flux to the atmospherefrom the Arabian Sea, surfaceconcentrations are atypicaland that the emissionsderived from them are probablyoverestimates. The Arabian Sea, which covers2% of the world's oceanarea,may contributeabout0.1% to the global oceanicCH4 emissions,if Bange et al.'s [1994] estimateof 15 Tg CH4 for the global flux is used.On the other hand , the Arabian Sea's contribution, if we use Bates et al's [1996] estimate, would amount to 4% of the global flux. However, sincethe estimateof Bates et al. [1996] did not take into account coastal areas, we feel that it represents a considerableunderestimationof the global oceanicsource.Thus, we concludethat the role of coastal upwelling areas in the Arabian Sea for the global oceanicCH4 emissionsis probably negligible. Acknowledgments. We thank G. Schebeskeand T. Kenntner for technicalassistance and acknowledge the help of othercolleagues, and the officers and crews of the R/V Sonne. Thanks are due to the chief scientistsW. Balzer (SOl17), V. Ittekkot (SOl19), and B. Zeitzschel (SO120). Specialthanksare due to T.S. Rhee, U. SchtiBler,A. Deeken, Nature, 354, 293-296, 1991. Patra, P.K., S. Lal, S. Venkataramani, M. Gauns, and V.V.S.S. Sarma, Seasonalvariability in distribution and fluxes of methane in the ArabianSea,or. Geophys.Res., 103, 1167-1176, 1998. Siedler,G., and H. Peters,Propertiesof sea water, in Oceanography, Landolt-B6rnsteinNew Ser., Group V, vol. 3a, edited by J. Sandermann, pp. 233-264, SpringerVerlag,New York, 1986. Wanninkhof,R., Relationshipbetweenwind speedand gas exchange overthe ocean,d. Geophys.Res.,97, 7373-7382, 1992. Wiesenburg,D.A., and N.L. GuinassoJr., Equilibrium solubilitiesof methane,carbonmonoxide,hydrogenin waterandseawater, or. Chem. Eng. Data, 24, 356-360, 1979. M.O. AndreaeandH.W. Bange,Max PlanckInstitutefor Chemistry, Biogeochemistry Department, PO Box 3060, D-55020 Mainz, Germany. (e-mail:bange•mpch-mainz.mpg. de) R. Ramesh, Institute for Ocean Management,Anna University, Chennai 600 025, India. S. Rapsomanikis, Laboratory of Atmospheric PollutionScienceand Technology,Departmentof EnvironmentalEngineering,Demokritos supporton board.We thank C. Strametzfor help with the manuscript. Universityof Thrace,GR-67100Xanthi,Greece. and the team of the R/V Sonne scientific-technical service for their The investigations were financially supported by the German Bundesministeriumflit Bildung, Wissenschafi, Forschung und TechnologiethroughGrant No. 03F0183G and by the Max Planck Society. (Received April 1, 1998;revisedJuly20, 1998; acceptedAugust13, 1998)
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