ENVINET Technical Task: LONGE-RANGE TRANSPORT. REPORT for the Technical task within ENVINET

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1 REPORT for the Technical task within ENVINET Long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions 1

2 PARTICIPATING INSTITUTIONS Ny-Ålesund: Zeppelin mountain atmospheric research station, Norwegian Institute for Air Research (Norway) and Meteorological Institute at Stockholm University (Sweden) N.C.S.R. Demokritos, Athens (Greece) Ny-Ålesund: German Koldewey Research station Mace Head atmospheric research station, University of Ireland, Galway Jungfraujoch atmospheric research station, University of Bern and EMPA (Switzerland) Sonnblick research station and Technical University Vienna (Austria) Zackenberg research station, Danish Polar Centre (Denmark and Greenland) Dunstaffnage, marine research laboratory Scottish Association of Marine Research Ny-Ålesund: Sverdrup research station, Norwegian Polar Institute (Norway) Abisko biological research station (Sweden) ALOMAR: Andenes (Norway) FMI-ARC: Sodankylä (Finland) Kristineberg marine research station (Sweden) Arctic Monitoring and Assessment Programme (AMAP) EXPERTS INVOLVED Dr. Roland Kallenborn, Christian Dye Dr. Konstantinos Eleftheriadis, Dr. Roland Neuber Prof. Dr. S. Gerard Jennings, Dr. Carsten Junker Prof. Dr. Erwin Flückinger, Dr. Martine de Mazière, Dr. Brigitte Buchmann Prof. Dr. Hans Puxbaum, Dr. Maria Löfflund, Dr. Michael Staudinger, Dr. Heidi Bauer. Dr. Morten Rasch, Dr. Knut Falk Prof. Dr. Graham Shimmield, Dr. Tracy Shimmield Dr. Jon-Børre Ørebæk, Dr. Elisabeth Cooper, Dr. Stig Falk-Petersen Prof. Dr. Terry Callaghan Dr. Michael Gausa, Torbjørn Adolfsen Dr. Esko Kyro Dr. Odd Lindahl, Dr Åke Grandmo Dr. Simon Wilson 2

3 Table of Content OBJECTIVES AND GOALS... 4 BACKGROUND AND STRATEGIES... 4 LONG-RANGE TRANSPORT... 4 PARTICLES AND AEROSOLS... 5 CLIMATE CHANGE... 6 ACTIVITIES AND STATUS... 7 DATABASE... 7 Concluding remarks PARTICLES TRANS-BOUNDARY EXCHANGE Expected results BIOTURBATION AND REDISTRIBUTION HARMONISATION Perspectives and future co-operation Expected results INITIATIVES AND ACHIEVEMENTS MULTI-DISCIPLINARY LINKAGES WITHIN THE TECHNICAL TASK: CHALLENGES AND BENEFITS STRUCTURES AVAILABLE AND POTENTIAL CO-OPERATION FIELDS JOINT PROJECTS AND COLLABORATION INITIATIVES LINKAGE ONGOING PROGRAMMES AND DATABASES POTENTIAL LINKS AND RELATIONS BETWEEN THE ENVINET TECHNICAL TASKS CONCLUSIONS AND PERSPECTIVES ACKNOWLEDGEMENT...25 REFERENCES ENCLOSURE 1: QUESTIONNAIRE

4 Objectives and goals The final goal for the technical task on long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions is to provide an effective joint scientific platform for fostering interdiscipilinary discussions as well as creating relevant ideas for comprehensive and harmonised research initiatives within the research topic Long-range transport processes and exchange processes. All participating institutions and research stations agreed to joint and actively contribute in inter-institutional discussions and co-operations on data evaluation, method adaptation, quantification methods, harmonisation of sample treatment, choice of priority contaminants and parameters and harmonised sample protocols and quality assurance/ control (e.g. first intercalibration exercises, data as well as method exchange and harmonisation efforts) which are intended to continue independently after the initial ENVINET project is finalised. Three prioritised sub-goals has been pursued by the TT group as integrated parts of the technical task: 1.) A database on available methods and data related to determination and evaluation methods for parameters related to LRT will be established. A questionnaire has been developed and circulated between all ENVINET stations (DATABASE). 2.) A co-operation network focussing on the role of particles/aerosols for long-range transport in both the marine and the atmospheric environment was established and will be maintained in the future. (PARTICLES) 3.) Method development for the investigation of ocean-surface/atmosphere exchange processes has been started and will be subject for further developments. Information on methods for the elucidation of particle transfer between atmosphere and sea surface will be investigated. (TRANSBOUNDARY EXCHANGE). 4.) A first study on bioturbation and redistribution of antropogenic contaminants has been performed from the Scottish Association for Marine Science (SAMS) with the support from the Ny-Ålesund Large Scale Facility and ENVINET (BIOTURBATION AND REDISTRIBUTION). 5.) Structural necessities and method harmonisation for a medium-scale study for the transport of persistent pollutants from known sources into Alpine and Arctic deposition regions are prepared and will be implemented in the preparation work for future international large scale project initiatives. (HARMONISATION). Background and strategies During the past century, the global phenomenon of atmospheric long-range transport into remote regions like Arctic and high alpine regions was investigated as one of the most complex research topics in modern sciences. Sulphate particles transported via the atmosphere from industrial source regions towards Scandinavia were identified as the major causes for the substantial acidification of freshwater lakes in the 1970s. In the course of the scientific follow-ups, long-range transported particulate material was also identified as important parameters for regional and global climate change processes. Long-range transport Today, atmosphere, sea currents, the transpolar pack ice and the large Arctic rivers are considered as the most important transport vehicles in the complicated process of long-range transport for 4

5 anthropogenic pollutants into the Arctic ecosystem (figure 1). The atmosphere is today recognised as the major pathway for contaminants into the high Alpine pristine regions of our globe. Which way a respective pollutant is transported into the Arctic and high alpine regions depends on the chemical and physical properties of the substance transported. Figure 1: Different entrance routes for pollutants into the Arctic. Anthropogenic pollutants can be transported into the Arctic via ambient air, ocean currents, and transpolar ice drift. Particles and aerosols The particulate phase in ambient air is still a major research object in the recent scientific efforts to understand fully atmospheric long-range transport and global climate change processes. Comprehensive investigations on the haze plume from the United States indicated that aerosol organics are spread as light sulphate compounds (Hegg et al. 1997). Thus, an accurate and comprehensive characterisation is needed for the estimation of the role of particles and aerosols to the overall phenomenon of global climate changes. Recent estimates have shown that 30 40% of the mass concentrations of particles smaller than one or two micrometers (mm) in diameter consist of organic material collected from air in urban or rural areas (Cass, 2000). However, usually only the total organic carbon (TOC) or black carbon (BC) concentration is documented in the literature, no information about compound specific composition is available yet even from comprehensively investigated regions. The lack of information about the distribution of the organic fraction in the atmospheric particulate phase makes it impossible to create a complete inventory of chemical compounds that make up the fine-particle fraction in the atmosphere from any site on the globe. This is important since organic compounds in the fine particulate fraction must be considered as the second most abundant contributor to the fine aerosols after sulphate. This is especially true for remote regions. Unlike the inorganic fraction, the organic partition covers an extremely wide range of 5

6 molecular structures, solubility, and physico-chemical properties. This mixture makes a complete chemical characterisation very difficult although urgently needed. Elemental carbon distribution (EC) has been studied but influence of non-elemental carbonaceous material on the EC fraction is not sufficiently investigated (Jakobson et al. 2000). On the other hand, organic carbon (OC) is a complex mixture of thousands of different organic compounds and only a very small portion of its molecular composition (~10%)has been characterised. Organic compounds that have been characterised include among others n-alkanes, n-alkanoic acids and polycyclic aromatic compounds. Due to difficulty in measuring organic compounds our current knowledge about organic matter is limited and incomplete. Primary emission sources for organic carbon include combustion processes, geological (fossil fuels) and biogenic sources. Elemental carbon (EC) has a chemical structure similar to impure graphite and is emitted as primary particles mainly during combustion processes from wood-burning, diesel engines etc. In Western Europe the contribution of diesel emissions to EC concentrations is estimated to be between 70 and 90% (Hamilton and Mansfield, 1991). Elemental carbon both absorbs and scatters light and contributes significantly to the total light extinction. In general, effects and consequences of particulate matter in the atmosphere are well documented. The significant influence of high particulate content in urban air during smog events on back scattering of light is obvious and has been known for a long time. Consequences such as reduced visibility, human health effects (e.g., disease of the respiratory organs, allergic reactions) and direct influences on the surrounding vegetation are well known direct effects of high particulate content in urban air. In addition, aerosols and particles have a documented direct radiative forcing because they scatter and adsorb solar and infrared radiation back in the atmosphere, and lead to a reduction of actual radiation reaching the troposphere and the ground. Aerosols are also known to change warm, ice and mixed-phase cloud formation processes and precipitation efficiency. Climate Change The newly released report on climate changes 2001 (IPCC 2001) stated that anthropogenic emissions influence the recently observed global climate change processes significantly. It is expected, that human influences will continue to alter atmospheric composition and the delicate climate equilibrium throughout the 21 st century. Thus, complex international efforts are needed to control and change this expected development. In the past, the sensitive environments of the Polar Regions have proven to be important indicator regions for early alarm signals of global climate changes. An important example, the stratospheric ozone depletion over the Antarctic caused by CFC (chlorofluorocarbons) must be mentioned (Molina 1992). Considerable changes of the Arctic climate were also reported. Since the 1980s, sea-level pressure (SLP) in the central Arctic oceans has decreased significantly (Wallace and Thompson 2002). These changes have been correlated with the Arctic Oscillation, describing the leading component of variance in the Northern hemisphere (SLP time series) as a manifestation of the strength of the polar vortex. For most contaminants, concentration levels tend to decrease from the point of release due to dispersion, transformation/degradation and dilution. However, scenarios have been described where concentrations have been higher in remote regions than in source regions. Examples are the elevated concentrations of selected persistent organic pollutants in Arctic and high mountain regions (e.g. Pacyna, 1995; Wania and Mackay, 1996; Wania and Mackay, 1999). One of the explanations for this enrichment may be attributed to prolonged persistence of such compounds in cold climates. Another explanation to the observed enrichment in cold regions of the globe that may act in parallel is the 6

7 increasing capacity of sorbing phases, such as soils and sediments, as temperature decreases (e.g. Wania, 1999). Both phenomena may, thus, result in elevated concentrations for selected POPs and other contaminants in cold regions compared to warmer middle latitude regions. As a consequence of the increase in temperature, a more rapid degradation of these compounds may occur in the Arctic. However, considerable changes in fluxes of contaminants and nutrients from phases where they have been initially trapped, such as sea- and fresh-water ice, sediment- and water-particles (i.e. remobilisation processes) might also be a direct consequence of temperature changes. Similar mechanisms are already assumed and documented for HCH pesticides in the Arctic environment (Li et al. 1998). Thus, an increase in temperatures of various environmental compartments (sea- and fresh water, soils and sediments) may result in specific alterations in the environmental distribution of persistent contaminants within the Arctic ecosystem as a direct result of the Arctic climate change. Ultimately, scenarios enhanced bioavailability in the water column with subsequent enhanced uptake of contaminants by aquatic biota and further accumulation in Arctic food chains can be envisaged in the future. Activities and status The above priority goals (see objectives and goals) were pursued during the technical tasks in order to provide an excellent scientific basis for a future co-operative network between the stations based on ENVINET. Database As a first initial step towards a joint database on methods and instrumentation for the elucidation of long-range transport and sea surface/atmosphere exchange processes a questionnaire has been developed in order to collect a first data set describing the state-of-the-science at the ENVINET stations participating in the technical task. The final version of the questionnaire is enclosed to the document (Enclosure 1). After sending the short questionnaire to all 17 ENVINET stations, 12 stations completed the questions. In addition to the completed questionnaires, information about relevant instrumentation, measuring campaigns and data available at the stations was extracted from already available ENVINET database on site specific information (www.amap.no/envinet). A first general survey revealed the comprehensive competence of all stations with regard to various disciplines relevant for research in long-range transport and trans-boundary exchange processes (figure 2). 13 major scientific topics and disciplines have been identified as relevant for the research work performed at the various stations. This broad spectrum of disciplines reflects the multi-disciplinary co-operation within the working group on the ENVINET technical task Long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions. Atmospheric physics and chemistry (11 stations), Environmental technology (11 stations) as well as Ecology and Ecotoxicology (11 stations) are the major disciplines within the group of 17 background research stations involved. Supporting research areas in environmental chemistry (10 stations), general botany (9 stations) as well as microbiology/ physiology (8 stations) reflects a certain overlap between the research areas, which cannot be excluded. Therefore, the overview presented must be considered as a first qualitative approach to describe the scientific potential of the working group. However, many of the minor research areas like Geology and environmental monitoring as well as oceanography and hydrology must be seen as important supporting disciplines for the major areas mentioned. However, based on the above, the major focus of future joint research initiatives should 7

8 be laid upon the multidisciplinary linkage between the 4 major research disciplines identified (Atmospheric physics and chemistry, Environmental Chemistry, Environmental Technology and Ecology/ Ecotoxicolgy). All stations cover a broad spectrum of scientific knowledge essential to cope with the future challenge of interdisciplinary research on long-range transport and dynamic exchange processes. The broad scientific competence of the scientific stations and their researchers involved must be considered as unique in an international scale. Thus, we conclude that the presented working group, representing 17 research stations in high altitude and high latitude regions, is well equipped and well suited for the demands for the highly complex scientific efforts requested for scientific investigation of global processes determining long-range transport and exchange processes in high-arctic and high latitude regions. No of institutions Atmopsheric physics and chemistry Environmental Chemistry Zoology Botany Microbiology/physiology Environmental Technology Ecology/ Ecotoxicology Geology GIS Modelling Glaciology Oceanography Hydrology Figure 2: Scientific topics covered by the 17 ENVINET stations with relevance for studies on longrange transport and exchange processes In addition to the scientific competence, the comprehensive coverage of all relevant environmental research areas crucial for a broad and interdisciplinary scientific elucidation of all aspects related to Long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions has been confirmed for all participating stations (figure 3). However, based on the present information database, more emphasis must be placed upon the needs for method harmonisation, co-ordination of monitoring and screening events, method comparisons etc. Thus, based on this information the stations will continue to co-ordinate their efforts to harmonise their work towards a future European network of excellence on studies for long-range transport and trans-boundary exchange processes in high Arctic and Alpine regions. 8

9 No of institutions Aerosol/ atmospheric particles Gas phase Studies on higher organisms Lower organisms Fresh water Sediment Soil Atmospheric radiation Contaminants (POPs, metals) Population studies Meteorological data Cloud studies Nutrients Precipitation Snow Ice Seawater Underwater radiation Cosmic ray studies Wind waves Aurora borealis Ligh conditions Total Ozone Greenhouse gases Geomagnetism Primary production Research topics Glaciology Figure 3: Research priorities covered by the 17 ENVINET stations relevant for research on longrange transport and trans-boundary exchange processes. The questionnaire used for the inquiries is appended to the report. Additional information about instruments and campaigns has been extracted form the ENVINET database on site specific information (http://www.amap.no/envinet). Most of the stations reported collection of data on atmospheric radiation (11), contaminant monitoring or campaigns (10) as well as meteorological information (12 stations collecting data on eg, temperature, humidity, wind speed). Thus, future harmonisation efforts should therefore focus on co-operation in data collection on the 6 major scientific topics presented in figure 3: 1.) Meteorological data collection (12 stations) 2.) Atmospheric radiation measurements (11 stations) 3.) Contaminant monitoring (10 stations) 4.) Studies on higher organisms (8 stations) 5.) Investigation of aerosols in the atmosphere (6 stations) 6.) Total ozone measurements 9

10 Several other minor topics should be implemented, since they obviously contribute to the major cooperation efforts with additional information. Examples: 1.) The investigation of greenhouse gases and cloud characterisation is an essential parameter for the evaluation of total ozone levels in the atmosphere. 2.) Population studies will directly contribute to ecological investigation on higher organisms. 3.) The linkage of aerosols and gas phase is obvious and cannot be investigated separately without loosing essential scientific information. However, these topics should not be considered as major research focus but more as supplementary efforts contribute to the 6 major research fields. At many stations, similar parameters are determined with different instrumentation. Based on information extracted from the site specific information database and the questionnaire (see attachment), a variety of methods for the determination of ozone profiles (ECC balloon sondes, LIDAR etc.), total ozone (Brewer, SAOZ etc.), meteorological parameters (radio sondes, stationary instrumentation etc.), aerosols (EC/OC, aethalometer etc.) have been identified Therefore, as a next step, the stations are expected to perform method validations and intercalibration exercises within the network in order to ensure comparability of the data in those cases were co-ordinated surveys or monitoring programmes are planned involving different types of instrumentation. The primary data set collected through the questionnaires is available from the author of this report or the ENVINET secretariat (Excel-sheet, 28 pages). Environmental compartments covered within relevance for studies on long-range transport and exchange processes No of institutions Boundary layer Troposphere/ Stratosphere Higher Atmopshere Marine Environment Terrestrial Environment 10

11 Figure 4: Interdisciplinary research areas covered by the participating stations. Concluding remarks Based on the information provided by the questionnaire as well as the site specific information database, a first general conclusions with regard to priority research with the field of Long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions can be drawn. Scientific co-operation and research initiative within the group should focus on the combination of the major disciplines such as atmospheric physics and chemistry, environmental chemistry, environmental technology as well as covering ecology and ecotoxicological aspects. The research frame should include meteorological data and be based on atmospheric radiation, contaminant research, as well as effects on higher organisms. The investigation of aerosols and total ozone should be implemented. The exchange processes in the marine/ atmosphere boundary layer should be in the focus of the research initiatives in future co-operations. Particles Regionally restricted but also global climate change processes are often related to the presence of aerosols/ particles in the atmosphere as relevant contaminants as well as parameters important for Albedo effects and, thus, large scale temperature regulations of the climate. Therefore, international agreements such as the Intergovernmental Panel on Climate Change (IPCC) include studies about particles in their considerations as high priority topics. However, a comprehensive elucidation of the organic particulate proportion in pristine air from Arctic and high alpine regions is still overdue. The investigation of partitioning of gas-particle organic compounds in the atmosphere is an important task in determining their association with the fine particulate matter. Understanding the mechanisms that control the conversion of organic matter from the vapour to particulate matter will provide valuable information for determining future control strategies for reducing the partition of organic matter in the particulate phase. However, there is a great number of different complex chemical forms of organic matter and an absence of direct chemical analysis. (Pandis et al., 1992). Black carbon (BC) aerosols formed during combustion processes cause positive climate forcing by absorbing sunlight and heating the lower atmosphere. IPCC estimates the BC forcing as W/m 2 (IPCC report) Aerosol yield is defined as the fraction of a reactive organic gas that is transformed to aerosol. There have been several methods for modelling the partition of organic matter into the aerosol phase. As the most promising method, the quantification of elementary- and organic carbon (EC/OC) in aerosol particles is of considerable scientific value for determining their primary sources. EC is usually present in the form of chain aggregates of small soot globules, and is responsible for the light absorption of the material collected on filters. Unfortunately this light absorption depends on the size distribution of the soot particles and on the association of the soot particles with other substances in the aerosol particles and on sample filters. Optical methods to determine EC are therefore only semiquantitative, and calibration factors may vary from one situation to another (e.g. Liousse et al., 1993). EC/OC determination For a first characterisation of organic particulate matter in the atmosphere, the ratio between elementary carbon (EC) and organic carbon (OC) is often used as a valuable tool for the elucidation 11

12 of the origin of the air masses investigated. Three established techniques are available for EC/OC characterisation at the four groups participating in the intercalibration exercise: 1.) Particle samples are collected using 37 mm quartz fiber filter. Thermal/optical EC/OC analyses are performed using an instrument from Sunset Laboratory Inc. (NIOSH method 5040). A standard sized punch is made from the exposed filters and placed in a quartz oven. The oven is purged with helium, and a stepped temperature ramp increases the oven temperature to 870º C, thermally desorbing organic compounds and pyrolysis products into an oxidizing oven. The organic carbon is quantitatively oxidized to carbon dioxide gas. The carbon dioxide gas is mixed with hydrogen and the mixture subsequently flows through a heated nickel catalyst where it is quantitatively converted to methane. The methane is quantified using a flame ionization detector (FID). After cooling the oven to 600º C a second temperature ramp is initiated and the elemental carbon is oxidized off the filter by introducing a mixture of helium and oxygen into the oxidizing oven. The elemental carbon is detected in the same manner as the organic carbon. 2. EC/OC measurements are carried out using the ACPM technique (Ambient Carbon Particulate Monitor, Series 5400: Rupprecht & Patashnick). Ambient particles are collected on impactors, which are used instead of filters in order to minimise unwanted artefacts during sample collection. After sampling, the impactor is heated to 340º C for 780 s, during which time organic carbon (OC) is oxidised, and then to 750ºC for 480 s, which oxidises the remaining elementary carbon (EC). The CO 2 is usually measured with a non-disperse infrared (NDIR) spectrophotometer. 3. However, high temperature thermal determination methods have clear limitations in terms of thermal degradation and composition changes of the organic particulate content (Huebert and Charlson, 2000). Therefore, the established techniques will be carefully evaluated and modified. Thus, a third method using optical techniques will be used for the determination and evaluation of EC/OC composition. Elemental carbon is monitored at the Zeppelin atmospheric research station (Ny-Alesund, Svalbard) and other stations (Mace Head) by means of optical transmission techniques (namely the Aethalometer (Maggee Sci)). The Aethalometer is an analytical instrument that uses a differentialradiometric optical transmission technique to determine the concentration of aerosol 'Black Carbon' particles suspended in the sampled air stream. The absorption is determined simultaneously at many wavelengths to yield the absorption spectrum. The calculation of EC or BC mass concentration is performed as follows: BC mass/filter unit area: BC m = ATN/ α API α API specific absorption cross section of BC aerosol on filter (m 2 g -1 ) α API = m 2 g -1 (depending on wavelength) ATN = -100ln(I/I 0 ) I 0 : transmitted light intensity through a blank portion of filter material I: transmitted light intensity through a portion of filter material with deposited aerosol sample From each sample (and blank) two circular specimen of ø=47mm were cut out to suit the Aethalometer filter holder. White light was transmitted through the centre of the specimen, and the 12

13 output current of the receptor photocell was measured.the Attenuation was calculated by the negative log of the ratio between the photocell output for the sample I1 and the photocell output for the respective blank I0. A = -ln(i 1 /I 0 ) (1) Assuming that the aerosol light absorption is the same in air as within the filter matrix, the absorption coefficient of the aerosol in ambient air σ was calculated by multiplying the Attenuation with the surface area a of the filter and dividing by the sampled air volume V. σ = A*a/V (2) Theoretical carbon mass on the filter MBC was calculated by dividing the Attenuation by the attenuation cross section for BC on the filter σaeth, specified by the Aethalometer manufacturer to σaeth = 19m²/g. M BC = A/σ Aeth (3) Assuming that the thermal analysis gives an estimate of the true BC concentration on the filters, the specific attenuation cross section for the sampled aerosols on the filter σa was calculated by σ a = A/M BC (4) Sample collection and preparation An independent sampling device for the intercomparison was installed at the Zeppelin Research staion (Ny-Ålesund, Svalbard). A high volume air sampler collection PM>2.1 µm and PM<2.1 µm aerosol on glass fiber filters was used for the purpose. The sampling periods of 1 week (January 2003) were chosen and two samples were collected and divided in sub-samples at NILU (Kjeller, Norway). The following research groups participated in the exercise: 1.) Dr. Konstantinos Eleftheriadis (Demokritos, Arthens, Greece) 2.) Prof. Dr. S. Gerald Jennings and Dr. Carsten Junker (University of Galway, Ireland) 3.) Prof. Dr. Hans Puxbaum (Technical University of Vienna, Austria) 4.) Dr. Roland Kallenborn (Norwegian Institute for Air research) The samples were divided in sub-samples and send to the respective institutions for analysis. The results of the exercise are summarized. Instrumentation and methods available at the participating institutes: National University of Ireland, Galway: The light absorption measurements of the Quartz fibre filters from Zeppelin mountain were performed using an Aethalometer for manual filter change, model AE-8. Demokritos, Athens (Greece): Continuous Black Carbon concentrations are monitored by means of a multi wavelength version of an Aethalometer (e.g. Model AE31, 7 channels from 450 to 950 nm). The AE-10 instrument operates with a broadband visible light source yielding a single BC output per measurement (see details above). 13

14 Norwegian Institute for Air Research (NILU): Particle samples are collected using 37 mm quartz fiber filter. Thermal/optical EC/OC analysis is performed using an instrument from Sunset Laboratory Inc. (NIOSH method 5040). For more details see above. Technical University Vienna (Austria): EC/OC measurements are done with the ACPM technique (Ambient Carbon Particulate Monitor, Series 5400: Rupprecht and Patashnick). The abbreviation TC means Total Carbon and gives a value for the amount total carbon measured. Table 1: Comparison of the results for elemental carbon (EC), Black carbon (BC)/ organic carbon (OC) and total carbon (TC) produced by three different analytical methods (see above). Aethaolometer measurements were performed both at Galway University and NCSR. Technical University of Vienna Norwegian Institute for Air Research NCSR Demokritos Galway University EC OC TC EC OC TC EC/BC 1 EC/BC 2 Samples µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 ug/m3 Zeppelin 1 0,133 0,353 0,353 0, ,232 0,232 0,005 0,008 Zeppelin 2 0,039 0,262 0,262 0,000 0,192 0,192 0,006 0,006 Zeppelin 3 0,035 0,272 0,272 0,039 0,192 0,232 0,009 0,011 Zeppelin 4 0,019 0,175 0,175 0,000 0,139 0,139 0,006 0,007 Zeppelin 5 0,000 0,064 0,064 0,000 0,148 0,148 Zeppelin 11 0,023 0,102 0,102 0,000 0,111 0,111 0,008 0,013 Zeppelin 12 0,122 0,346 0,346 0,102 0,132 0,235 0,070 0,109 Zeppelin 13 0,169 0,544 0,544 0,157 0,289 0,446 0,134 0,196 Zeppelin 14 0,267 0,764 0,764 0,249 0,425 0,674 0,183 0,284 Zeppelin 15 Blank 0,007 0,043 0,043 0,000 0,029 0,029 Zeppelin FBL 1 * 0,023 0,077 0,077 0,000 0,054 0,054 Zeppelin FBL 3 0,036 0,039 0,039 0,000 0,022 0,022 * FBL = Field Blank = not detected 1 NCSR performed parallel measurements, thus, the results reported are from separate aethalometer measurements 2 It is assumed that BC (black carbon) and EC are representing the same type of carbon All four laboratories reported results back to the secretariat. It should be noted that the data reported from NSCR Demokritos (K. Eleftheriadis) are measured in an independent sample set by Aethalometer measurements (instrument AE-31). It was not possible to perform thermo-optical analysis like the other groups did. NCSR Both institutes, NCSR Demokritos and Galway University performed thermal measurements/ transmission measurements with Aethalometer instruments. All results obtained are reported in table 1. In general, a large variation of the reported data is indicated (Standard deviations larger then median values). The method dependent variation of the results is statistically presented in table 2. Large sample to sample variations are observed for all groups indicating that aerosol composition (size, 14

15 characterisation etc.) is crucial for of high importance for the accurate determination of EC, OC and TC. The largest deviation from the average values has been found for EC, where for sample Zeppelin 1 the reported results spread over 1016 % related to the median (n=4, table 3). However, it should be noted that the Aethalometer measurements for the determination of EC/BC (Black carbon) corresponded well and, thus, indicate a good instrument related comparability for EC/BS measurements. For EC relative deviations ranging from 1016% (Zeppelin 1) to 16% (Zeppelin 13; see table 3) have been found illustrating the high sample and instrument depended variability. Also for the EC determination in of the field blank values (FLB) the strongest variation was found for EC measurements indicating a significant influence of the method and instrumentation used for determination of EC. The variability for OC (5 145%) and TC (5-56%) was not as pronounced as for EC (Table 3). However, only two participants reported OC and corresponding TC values. Thus, only two data points are assumed to be too few for a good estimation. The Aethalometer methods used for EC determination seems to deliver results comparable with the NIOSH method Deviations from the NIOSH method 5040 of around 20-40% are found for all sampling periods (1-4, 11-14) compared to both aethalometer measurments. Table 2: Average distribution, standard deviation and min/ max values for the reported EC/BC, OC and TC values. EC/BC OC TC n Median STD* min max n Median STD min max n Median STD min max Sample µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 µg/m 3 Zeppelin 1 4 0,006 0,064 0,000 0, ,125 0,151 0,017 0, ,292 0,086 0,232 0,353 Zeppelin 2 4 0,006 0,017 0,000 0, ,114 0,111 0,035 0, ,227 0,049 0,192 0,262 Zeppelin 3 4 0,023 0,016 0,009 0, ,108 0,119 0,024 0, ,252 0,029 0,232 0,272 Zeppelin 4 4 0,006 0,008 0,000 0, ,082 0,082 0,024 0, ,157 0,025 0,139 0,175 Zeppelin 5 4 0,000 0,000 0,000 0, ,084 0,090 0,021 0, ,106 0,059 0,064 0,148 Zeppelin ,010 0,010 0,000 0, ,082 0,040 0,054 0, ,106 0,006 0,102 0,111 Zeppelin ,105 0,022 0,070 0, ,165 0,046 0,132 0, ,290 0,078 0,235 0,346 Zeppelin ,163 0,026 0,134 0, ,279 0,015 0,268 0, ,495 0,069 0,446 0,544 Zeppelin ,258 0,044 0,183 0, ,410 0,021 0,395 0, ,719 0,064 0,674 0,764 Zeppelin 15 Blank 4 0,003 0,005 0,000 0, ,032 0,005 0,029 0, ,036 0,010 0,029 0,043 Zeppelin FBL 1 * 4 0,011 0,016 0,000 0, ,049 0,006 0,045 0, ,065 0,016 0,054 0,077 * STD = standard deviation However, these first results should be rated as just indications and not to be considered as evidence for as advantage and/or weakness of a particular method for EC/OC determination. Such a limited intercalibrated as performed here cannot deliver decisive information about quality, and accuracy for specific determination methods. Much more emphasis must be laid upon a comprehensive comparison and method adaptation to meat the quantitative requirements for EC/OC determination in pristine/, background aerosol samples. 15

16 Thus, based on the here presented results, a Joint Research Activity dedicated to the development and optimisation of sampling techniques for aerosol in the atmosphere is sought to be funded within the a subsequent ENVINET II application. Table 3: Relative deviation in percent of the EC, OC and TC results reported (Median = 100 %). EC OC TC Sample rel. Deviation [%] rel. Deviation [%] rel. Deviation [%] Zeppelin Zeppelin Zeppelin Zeppelin Zeppelin Zeppelin Zeppelin Zeppelin Zeppelin Zeppelin 15 Blank Zeppelin FBL 1* Zeppelin FBL FBL = Field blank sample Trans-boundary exchange Transport of contaminants is usually described as a combination of different transport media and the respective exchange processes through the boundary layers. The importance of the different transport routes depends on a set of parameters such as water solubility, volatility and ability to adsorb to particles. However, recent models (e.g., fugacity model, multi compartment box models) are based on a combination of different transport routes where the physical properties of the transported compound define the significance of the respective medium during the transport process. Thus, metals will be transported mainly in the water column as ions, particle bound salts and minerals, or by air, whereas, in the gaseous state the metals are often particle bound. Radionuclides are mostly transported by air and water, depending on contaminant characteristics. Transport of persistent organic pollutants (POPs) includes both the atmosphere and the water column. For several semivolatile POPs a repeated deposition from the atmosphere into the water column and a subsequent remobilisation of the compounds into the atmosphere is postulated (Wania and Mackay 1993; Wania and Mackay 1996). This process is commonly named as grasshopper effect. In general, input via the atmosphere is considered the main source of semi-volatile POPs to the Arctic environment. However, only a smaller fraction of the total amount of pollutants is present in the atmosphere. Oceans, fresh water bodies and the terrestrial environment are important storage media, which are in continuous exchange with the atmosphere. The oceans are a large reservoir of POPs with equilibrium concentrations in seawater, which are several magnitudes higher than in air. Depending on ambient temperature differences, semi-volatile POPs are deposited at different latitudes resulting in a global 16

17 distillation or fractionation. As a first conclusion, it can be assumed that oceans, fresh water bodies and the terrestrial environment as well as the atmosphere are important storage and transport media that are in continuous exchange with each other. However, experimental studies on the mechanisms ruling trans-boundary exchange processes are still sparse although highly needed. Therefore, an interdisciplinary initiative was inaugurated within the technical task Long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions in order to design an experimental approach for the elucidation of atmosphere/ sea surface exchange processes for selected persistent contaminants. Several project initiatives are planned for 2003 to apply for national and international funding. All project experiments will be interlinked. A combination of active and passive sampling devices will be employed at different sampling sites. One new technique with passive air sampling of pollutants developed during last 10 years is expected to open new possibilities for an time integrated knowledge of longe-range transportation of xenobiotics. There have also been different efforts to compare this technique with traditional measurement methods (Ockenden et al., 1998) reporting excellent comparability, but other experiences show that more knowledge of the influence of different environmental factors such as wind speed, temperature and precipitation is necessary. The method using semi-permeable membrane devices (SPMD) for sampling of persistent contaminant in the atmosphere has shown to be valid for monitoring programmes (Meijer et al. 2003). There are at present a range of different methods used and thus there may be need for comparisons for future applications. In the recent US-SETAC-conference (November 2002) reports were presented considering urbanrural transects and the use of diffusive samplers in the US, and also passive air sampling surveys for POPs in a cross transect of the North Americas. First investigations in co-operation with the University of Lancaster has shown that exchange processes between snow/ ice surface and the atmosphere contribute significant to the remobilization of persistent organic pollutants in Arctic regions (Halsall et al. 2002, Fizpatrick et al. 2002). This study has been performed as a joint experiment funded as an ARI within the LSF Ny-Ålesund. The following joint research activities have already started in the research field Exchange processes in the interphase atmosphere / seawater and atmosphere/ snow surface as a direct out come of the Technical task on Long- range transport of pollutants and boundary layer exchange in Arctic and Alpine regions. 1.) Method adaptation for the application of SPMDs for boundary layer exchange processes in the seawater / atmosphere interface. Activities: Project application to national Research programmes in progress Participants: NILU, Kristineberg marine station, IVL Swedish Environmental Research Institute 2.) Optimisation and evaluation of polyurethane foam plug passive sampling devices for longterm investigation of contaminant transport and cycling processes in remote regions. Activities: Project application to national Research programmes in progress Participants: NILU, Lancaster University. 17

18 3.) The influence of climate change parameters on long-range transport and boundary layer exchange processes in remote Arctic and alpine regions. Activities: Project application to national Research programmes and EU in progress Participants: Norwegian Polar Institute, NILU, Lancaster University, UNIS. Expected results The joint research activities are expected to provide 1. Harmonised information on basic parameters ruling the dynamics of exchange processes between the different compartments. 2. Quality controlled empirical data and information on exchange rates for indicator compounds as important input in validation and evaluation of models 3. Reliable information on temperature and wind-dependence and other physical, oceanographic, geographic and meteorological parameters crucial for exchange processes 4. Scientific information on seasonal variations influencing exchange rates and contaminant levels 5. Scientific estimates of climate dependence for exchange processes 6. Reliable data input to already existing models and important scientific input for new concepts within modelling and scenario assessments Bioturbation and redistribution The Scottish Association for Marine Science (SAMS) has performed a pilot study on bioturbation and redistribution of long-range transported contaminants in the Arctic Environment. First experiments were performed at Ny-Ålesund research facilities as an ARI contract in The following preliminary results and activities were reported from the study: 1.) Samples from the Ny-Ålesund water reservoir were collected for the study of atmospheric pollutants 2.) Sediment samples were taken in the outer ice-free part of the Kongsfjord from the research vessel Lance from two stations. The samples will be analysed with regard to primary production input to sediments in the spring. 3.) A mooring was deployed in the Kongsfjord area with a sediment trap implemented. The equipment was successfully recovered in September Unique data are expected with regard to sedimentation rate and sediment composition (figure 5). 18

19 Figure 5: Mooring deployed in Kongsfjord (Svalbard) The scientific data gathered form the various experiments will be published in peer-reviewed international scientific journals. 19

20 Harmonisation Today, for all inter-institutional scientific co-operations, all major international and national monitoring and surveillance programmes agree that a firm harmonisation of sampling periods and sampling procedures as well as instrumentation is essential in order to obtain the best possible scientific basis for the comparison of results and scientific information. Thus, for future co-operation joint protocols for the harmonisation of the sampling periods for all stations will be developed and refined. Sampling procedures and important common criteria for aerosol, particle collection as well as contaminant analysis etc. will be summarised in a protocol for all stations involved and will include appropriate description of the experimental set-up. National regulatory institutions also recognise the need for harmonisation of monitoring initiatives. Thus, already in 1991, the Danish Environmental Research institute (NERI), department for atmospheric research has launched an initiative on "Harmonisation within Atmospheric Dispersion Modelling for Regulatory Purposes". This initiatives serves as a national tool for increased cooperation and standardisation of atmospheric dispersion models for regulatory purposes. Based on the outcome of large international monitoring programmes, it can be stated that international studies on distribution and fate of persistent organic pollutants (POP) are still important to assess the pollution magnitude of harmful substances across borders. Especially in pristine and fragile ecosystems like arctic and sub-arctic as well as high alpine regions, evaluations of the degree of pollution are essential for the assessment of ecotoxicological risks. In 1995 the Arctic Monitoring and Assessment Programme (AMAP) developed a collection of method performance criteria and quality control measures for Arctic environmental samples (AMAP 1995). The quality control criteria developed includes standardisation of the sampling procedures as well, as major factors to be considered in the fieldwork, which have influence on the determination of contaminants (particles, pollutants etc.). In order to both standardize existing analytical methods and develop new procedures, a tight cooperation between the laboratories is needed and required. The general need for harmonisation and quality assurance of the collected data within large monitoring and surveillance programmes is recognised by all major international environmental monitoring programmes like the European Monitoring and Evaluation programme (EMEP), Arctic Monitoring and Assessment Programme (AMAP) and others. EMEP has recently documented needs and requirements for comprehensive international monitoring programmes (EMEP 2001). In order to meet the requirements of scientific based quality assurance (QA) and harmonisation between the stations, EMEP recommends: Appointment of a QA Manager in each of the participating units (countries, laboratories). These persons will be responsible for implementing harmonized quality assurance systems within the units, including documentation of standards and reference materials. Development of standardized operating procedures based on recognised QA recommendations (e.g., AMAP 1994, EMEP 2001). Co-location experiments and instrument comparisons in the various units to document precision and quantify internal network differences. Continuation of efforts towards site characterization. 20

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