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Observations at Cape Grim, Tasmania, 1998-2000

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Observations at Cape Grim, Tasmania, 1998-2000 '19-99, !! Journalof AtmosphericChemistry 452 2003. 79 tlft O 2003Kluwer Academic Publishers. Printed in theNetherlands. Regional Sourcesof Methyl Chloride, Chloroform and DichloromethaneIdentified from AGAGE Observationsat CapeGrim, Tasmania, 1998-2000 M. L. COXl'', G.A.STURROCK3'4,P. J. FRASER3,S. T. SIEMS2, P. B. KRUMMEL3 and S. O'DOHERTYS l Now ot the Centrefor Atmospheric Chemistty, York universi4t, North York, Ontario, Canada 2^Departmentof Mathematics and Stati.stics,Monash University, Clayton, Victoria, Australia s.AtmosphericResearch, CSIRO, Aspendale, Victoria, Australia +Now at School of Environmental Sciences,University of East Anglia, Norwich, U.K. 5School of Chemistry, University of Bristol, Bristol, U.K. (Received: 12 April 2001; accepted:2 November 2002) Abstract. There are large uncertaintiesin identifying and quantifying the natural and anthropogenic sources of chloromethanes- methyl chloride (CH:CI), chloroform (CHC1:) and dichloromethane (CHzCl), which are responsiblefor about 75Voof the total chlorine in the stratosphere.We report two years of in situ observationsof these speciesfrom the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania(41" S, 1450E). The averagebackground levels of CH3CI, CHC13and CH2CL2during 1998-2000were 551 + 8, 6.3 + 0.2 and 8.9 { 0.2 ppt (dry air mole fractions expressedin parts per 1012)respectively, with a two-year averageamplitude of the seasonalcycles in background air of 25, 1. 1 and 1.5 ppt respectively.The CH3CI and CHCI3 records at Cape Grim show clear episodesof elevatedmixing ratios up to 1300 ppt and 55 ppt respectively, which are highly correlated,suggesting common source(s).Trajectory analysesshow that the sources of CH3CI and CHCI3 that are responsible for these elevated observations are located in coastal- terrestrial and/or coastal-seawaterregions in Tasmania and the south-eastetnAustralian mainland. Elevated levels of CH2C12 (up to 70 ppt above background) are associatedmainly with emissions from the Melbourne/Port Phillip region, a large urban/industrial complex (population 3.5 million) 300 km north of Cape Grim. Key words: chloromethanes,methyl chloride, chloroform, dichloromethane, Cape Grim Baseline Air Pollution Station, baseline data, annualcycle, trajectory analysis,pollution events,coastal source reglons. 1. Introduction Stratosphericchlorine accounts for 757o of halogen (chlorine, bromine) induced ozoneloss (Madronich et a\.,1999).Methyl chloride(CH3C1), chloroform (CHCI3) anddichloromethane (CH2C12) are relatively short-lived (1.3, 0.5 and0.4-0.5 years respectively) chloromethanesthat contribute about l57o of stratosphericchlorine (Schauffleret al., 1993 Kurylo et al. , 1999).Over the coming decadesthe contribu- 80 M.L.coxETAL. tion of anthropogenichalocarbons (chlorofluorocarbons, halons etc.) to ozone loss will decline (Montzka et al., 1999) due to production limits set under the Montreal Protocol. At the same time naturally produced chloromethaneswill become rela- tively more important (Madronich et al.,1999). Although the CH3CI and CHCI3 sourcesare largely natural, human induced changesto their emissionsmay result from land-useand climate changes.A more detailed knowledge of the sourcesand sinks of these chloromethanesis required in order to assesstheir contribution to ozone depletion via human-inducedperturbations to their emissions. In general,the mixing ratios of CH3CI are higher in the marine boundary layer (MBL) than in the free troposphereand, in the MBL, the highest concentrationsare found in the tropics and the lowest at high latitudes (Khalil and Rasmussen,1999a). Estimatesof the global averagemixing ratios of CH3CI in the MBL rangefrom 550 to 600 ppt (Khalil andRasmussen,1999a; Kurylo et a1.,1999);the averagemixing ratio in the northern hemisphere(NH) is similar to the southernhemisphere (SH). CH3CI levels were present at about 907oof current levels during the early part of the20th century(Butler et a1.,1999). The identified global sourcesof CH3CI (Table I) are tropical biomass burning (40-507o,Rudolph et aI.,1995), the oceans(I0-30Vo,Tait et aI.,1994; Moore e/ al., 1996),salt-marshes (xljEo, Rhew er aI.,2000), wood-rottingfungi and other tropical terrestrial sources (5-I0Vo, Watling and Harper, 1998; Yokouchi et al., 2000) and anthropogenicprocesses including combustion of fossil fuels and waste (5-I5Vo, McCulloch et al., 1999;Butler, 2000). The combinedmagnitude (2 Tg yr-1) and range (1-3 Tg y.-t) of the identified CH3CI sourcesare significantly less than the magnitude (4 Tg yr-1; and range (3-5 Tg yr-t) of the known sinks (seeTable I), suggestingthere are missing and/or underestimatedCH3CI sources. The uncertainty range of the combined CH3CI sinks (l25Vo) is significantly less than that of the sources(l507o). The global averagemixing ratio of CHCI3 in the MBL rangesfrom 10 to 20 ppt and NH mixing ratios are about a factor of 2 higher than those in the SH (Elkins e/ al., 1998;Khalil and Rasmussen,1999b; O'Doherty et a1.,200I). Oceanicemis- sions are reportedto be about 607oof the global source(Keene et a1.,1999,Table I) and forest soils about 30Vo (Hoekstra et al., I998a,b; Frank and Frank, 1990; Haselmannet a1.,2000a,b; Dimmer et a1.,200I). The observedinter-hemispheric gradient of CHCI3 arguesagainst the notion that the ocean is the dominant source of CHCI3, suggesting alarger role for land based (largely NH) sourcesand/or a diminished role for oceanic (largely SH) sources.A recent modelling study us- ing global CHCI3 data does not support a lnge ocean source, but rather a large soil source(O'Doherty et a1.,2007). Kleiman and Prinn (2000) showedthat the high levels of CHCI3 observed on the coast 10 km north-east of Boston cannot be simulated using only anthropogenicemissions, indicating that natural coastal sourceswere important. Anthropogenic CHCI3 sources (I}Vo) include emissions from chlorination processes(pulp/paper manufacture,water/sewerage treatment) and fugitive releasesfrom industrial processes(Aucott et a1.,1999). REGIONALSOURCES OF METHYL CHLORIDE,CHLOROFORM AND DICHLOROMETHANE 8 1 Table L Estimates of global annual sources and sinks for CH3C1, CHCI3 and CH2C12 (Tg/yr) (adaptedfrom Keene et al.,1999) Source Best Range Sink Best Range estimate estlmate CHjCl Biomass burning 0.91 0.65-t.12 Troposphere 3.41 2.84.6 1.0 0.7-r3a,b Stratosphere 0.28 Open ocean 0.65 0.37-0.94 Soil 0.26 0.5 0.3-0.6a'b Salt marsh 0.17 0.07-0.44c Ocean 0.2 0.1-0.3a Fungi/soils 0.16 0.04-0.47 Fossil fuel combustion (1) 0.11 0.01-0.20 Waste incineration (2) 0.05 0.01-0.08 Fresh water wetlands 0.05 Industry (3) 0.01 Totalindustry(1+2+3) 0.17 0.3 0.24.44 Total 2.1 r.z-J.3 Total 4.2 3.4-5.4 2.2 1.5-3.3a Source-sink 2.r CHCIj Ocean 0.36 0.2r-0.5r Troposphere 0.46 0.4-0.6 Fungi/soils 0.20 0.114.45 Stratosphere <0.01 Industry 0.07 0.04-0.10 0.06a Total 0.63 0.36-1.06 Total 0.46 0.4-0.6 Source-sink o.t7 CH2C12 Industry 0.58 0554.62 Troposphere 0.59 0.53a Ocean 0.19 0.10-0.29 Stratosphere 0.01 Biomass burning 0.06 0.05-0.07 Total 0.83 0.70-0.98 Total 0.60 Source-sink 0.23 a Kurylo et aL (1999). b Butler (2000). c Rhew et al. (2000). 82 M.L.coxErAL. The global averagemixing ratio of CHzClz in the MBL rangesfrom 20-30 ppt, with NH mixing ratios a factor of 2-3 higher than those in the SH (Elkins et al., 1998; Khalil, 1999; Kurylo et al., 1999).The major sourcesare anthropogenic (about J}Vo,-lable I) from foam plastic production, metai cleaning and other sol- vent uses, consistent with the observed inter-hemispheric gradient. The natural sourcesinclude the ocean and biomassburning (about 25Voand 57o rcspectively- 'poorly Keeneet al., t999), althoughthe oceansource is reportedto be constrained' (Baker et a1.,200I). In this paper 25 months (March 1998-March 2000) of CH3C1,CHCI: and CH2CI2 data are reported from the AGAGE in situ gas chromatography-mass spectrometry(GC-MS) instrument located at Cape Grim, Tasmania(40'41'S; 1444I' E) (Prinn et a1.,2000). Backgrounddata and seasonalvariability, repre- sentativeof the SH mid-tatitudes, are identified and compared to other reported atmosphericchloromethane data. Trajectory analysistechniques are used to iden- tify local chloromethanesource regions and inter-speciescorelations to identify possible common sources.The identities of the chloromethane sources are sug- gested from local knowledge of the soufce regions and by reference to source identiflcation studiesin the literature. 2. Experimental 2.T. INSTRUMENTATION, CALIBRATION AND DATA INTERCOMPARISONS In situ GC-MS chloromethanemeasurements (6 per day) commenced in March 1998 at Cape Grim, which is situated on the northwest colner of Tasmania(Fig- ure 1). The instrumentation consistsof a Carboxen-filled micro-trap (20 p'l) in an adsorption(-55'C) - desorption(240"C) systemfor air-sampling(Nafion dried, 2litres per measurement,40 minutes trapping time) coupled to a HP 6890/5973 GC-MS using analysis techniques developed at the University of Bristol (UB) (Simmondset al., 1995;Sturrock et al., 1998;Prinn et al., 2000). Approximately 3500 calibrated measurementsof the chloromethanesale re- ported. Minor data gaps are due to instrument servicing and downtime. Monthly mean precisions (Vo standarddeviation) achievedin 1998 for about 150 standard measurementsper month were0.4Vo(CH3C1), 1.17o (CHC1:) and 0.9Vo(CHzCl), while the variability in backgroundambient air measurementswere l.3Vo,4Vaand 3qorcspectively (Sturrock et aL.,2001). All ambient air chloromethanemeasurements are referencedto bracketing sam- ples of working or tertiary standardsthat are preparedby cryo-trapping 1400 litres of ambient background Cape Grim air into electro-polished 35litre stainless steel cylinders (3000 kPa). After about 3 months of use, when the pressurehas dropped to 300 kPa, the tertiary standardis inter-comparedwith, and exchanged for a new tertiary standard.Chloromethane mixing ratios are assignedto the ter- tiary standardsby comparison wilh secondary standardswhich are 1400 litres of dried, background Trinidad Head (California, U.S.A.) air, compressed into REGIONALSOURCES OF METHYL CHLORIDE,CHLOROFORM AND DICHLOROMETHANE 83 a c) - J 143 144 tl3"nii,13" 148 14s r'LT Figure l.
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