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Interfaces in Aquatic Ecosystems: Implications for Transport and Impact of I Anthropogenic Compounds Luhbds-«6KE---C)I‘> Interfaces in aquatic ecosystems: Implications for transport and impact of I anthropogenic compounds luhbDS-«6KE---c)I‘> "rol° STER DISTfiStihON OF THIS DOCUMENT iS UNUMITED % In memory of Fetter, victim of human negligence and To my family andfriends Organization Document name LUND UNIVERSITY DOCTORAL DISSERTATION Department of Ecology Date of issue November 19, 1996 Chemical Ecology and Ecotoxicology Ecology Building CODEN: SE- LUNBDS/NBKE-96/1010+136 S-223 62 Lund, Sweden Authors) Sponsoring organization Swedish Environ­ JOHANNES KNULST mental Research Institute (IVL) Title and subtitle Interfaces in aquatic ecosystems : Implications for transport and impact of anthropogenic compounds Abstract Mechanisms that govern transport, accumulation and toxicity of persistent pollutants at interfaces in aquatic ecosystems were the foci of this thesis . Specific attention was paid to humic substances, their occurrence, composition, and role in exchange processes across interfaces. It was concluded that: The composition of humic substances in aquatic surface microlavers is different from that of the subsurface water and terrestrial humic mat­ ter. Levels of dissolved organic carbon (DOC)in the aquatic surface micro ­ layer reflect the DOC levels in the subsurface water. While the levels and enrichment of DOC in the microlaver generally show small variations, the levels and enrichment of particulate organic car­ bon (POC) vary to a great extent. Similarities exist between aquatic surface films, artificial semi-per­ meable and biological membranes regarding their structure and function ­ ing. Acidification and liming of freshwater ecosystems affect DOC:POC ratio and humic composition of the surface film, thus influencing the parti­ tioning of pollutants across aquatic interfaces. 21 Properties of lake catchment areas extensively govern DOC:POC ratio both 41 in the surface film and subsurface water. Increased UV-B irradiation changes the DOC:POC ratio in the surface 61 film and thus affect transfer of matter across the interface. SIS Transport of lipophilic, persistent organic pollutants across semi-per­ DOKUMENTDATABLAD enl meable membranes is influenced by the solutes organic composition. aquatic surface film, surface microlayer, humic substances, interface, transport, particles, acidification, liming, UV-B Classification system and/or index terms (if any) Supplementary bibliographical information Language English ISSN and key title ^^105-082-5 Recipient's notes Number of pages ^35 Price Security classification Distribution by (name and address) Johan. Knulst, Swedish Environmental Res. Instit., S-360 30 Lammhult , Sweden I, the undersigned, being the copyright owner of the abstract of the above-mentioned dissertation, hereby grant to all reference sources permission to publish and disseminate the abstract of the above-mentioned dissertation. Signature n„e Interfaces in aquatic ecosystems: Implications for transportand impact of anthropogenic compounds Johannes Knulst FK, Sm Akademisk avhandling, som for avlaggande av filosofie doktorsexamen vid matematisk- naturvetenskapliga fakulteten vid Lunds Universitet, kommer att offentligen forsvaras i Bla Hallen, Ekologihuset, Solvegatan 37, Lund, ffedagen den 13 december 1996, kl. 1300. DISCLAIMER Portions of this document may be illegible in electronic image products. Images are produced from the best available original document Interfaces in aquatic ecosystems: Implications for transport and impact of anthropogenic compounds Johannes Knulst FK,Sm Dissertation Lund 1996 A doctoral thesis at a university in Sweden is produced either as a monograph or as a collection of papers. In the latter case, the introductory part constitutes the formal thesis, which summarizes the accompanying papers. These have either already been published or are manuscripts at various stages (in press, submitted or in ms). ISBN 91-7105-082-5 SE-LUNBDS/NBKE-96/1010+136 Contents Introduction 7 Materials and Methods 20 Conclusions 26 Summary 35 A cknowledgements 37 References 37 D ankwoord 44 List of used abbreviations 46 List of Papers This thesis is based on the following papers which are referred to by Roman numerals. Papers I-III, V and VII are reprinted with permission from the publishers. I. Espedal, H. A., O. M. Johannessen and J. Knulst. Satellite detection of natural films on the ocean surface. Geophysical Research Letters (in press). II. Sodergren, A., P. Larsson, J. Knulst and C. Bergqvist. (1990) Transport of incinerated organochlorine compounds to air, water, microlayer, and organisms. Marine Pollution Bulletin 21:18-24. III. Knulst, J. and A. Sodergren. (1994) Occurrence and toxicity of persistent pollutants in surface microlayers near an incineration plant. Chemosphere 29(6): 1339-1347. IV. Knulst, J., P. Backlund, D. O. Hessen, G. Riise, and A. Sodergren. Response of surface microlayers to artificial acid precipitation in a meso-humic lake in Norway. Water Research (submitted). V. Knulst, J. C. C. (1992) Effects of pH and humus on the availability of 2,2',4,4',5,5'- hexachlorobiphenyl- C in lake water. Environmental Toxicology and Chemistry 11(9): 1209-1216. VI. Knulst, J. C., R. C. Boerschke and S. Loemo. Differences in organic surface microlayers from an artificially acidified and control lake, elucidated by XAD- 8ZXAD-4 tandem separation and solid state 13C NMR spectroscopy. Environmental Science &Technology (submitted). VII. Hessen, D. O., E. T. Gjessing, J. Knulst and E. Fjeld. TOC fluctuations in a humic lake as related to catchment acidification, season and climate. Biogeochemistry, (in press). i ’’For out of the oldfieldes, as men saithe, Cometh al this new come fro yere to yere; And out of old bookes, in goodfaithe, Cometh al this new science that men lere. ” —Geoffrey Chaucer (1328-1400) From Tyrwhitt Introduction Mechanismsthat govern transport, accumulation and toxicity of persistent pollutants at interfaces in aquatic ecosystems are the foci of this thesis. Specific attention is paid to humic substances, their occurrence, composition, and role in exchange processes across interfaces. The interface between air and water of lakes and oceans is covered with a thin layer of chemical substances. This thin layer (the surface film or microlayer) reveals properties distinct from subsurface water, and may therefore be treated as a separate ecosystem. Langmuir (1917) stated that anthropogenic effects occurring at physical boundaries of systems are of key importance for biological, physical, and chemical processes. Therefore, the properties of the surface film that presumably covers all bodies of water on Earth, are of particular interest. The presence of an unique environment at the air-water interface has interested man for a long time. As early as 1500 B.c. Babylonian seafarers experienced that oil calmed angry seas when poured on the waves. A number of review articles (Liss 1975, Norkrans 1980, Hunter and Liss 1981, Hardy 1982, Maki 1993) assimilated findings on the chemistry, physics and biology of this environmental interface. Surface films are defined as a relativelythin (0.001 to 200 pm), organic substance-rich layer at the water surface (Norkrans 1980). They maintain specific chemical and biological features (Daumas et al. 1976, Kjelleberg et al. 1979, Hardy 1982, Nageli et al. 1993). The upper portion of this film is referred to as the surface microlayer. In this thesis, an arbitrary difference between surface film and microlayer is that: • The film contains a number of strata with concentrated biota, chemicals, and distinct physical characteristics compared to subsurfacewater, • while the microlayer constitutes the portion of the surface film sampled by the collector. 7 ATMOSPHERE Gas exchange ^ Dry deposition wind generated aerosols wet depostion bursting bubbles animal defecation evaporation gas exchange biotic uptake ^ biotic uptake run-off ^Wind and SURFACE FILM currents Upwelling j L Biotic uptake convection = wave action diffusion % emulsion bubbles •| dissolution floatation E sedimentation _ re-fluxing r downwelling run-off a y ^wmd and Figure 1. Sources and pathways of chemical substances to aquatic surface films. (After Hardy and Word 1986). Natural surface film is exposed to many environmental factors such as rain, winds, temperature gradients, and cosmic irradiance. Understanding the effects of man-made environmental changes on the properties of the surface film improves our ability to describe and explain the influence of surface films on transport of pollutants from air to water and vice versa. Studies of this kind are complicated, and the environmental circumstances must be considered carefully. 8 In spite of frequent sources of disturbance surface films are resistant to disruption, suggesting that a surface film is present on almost all surface waters. After physical disruption, the film is rapidly restored (Jarvis 1967, Williams et al. 1980, Dragcevic and Pravdic 1981). Sources of the materials building surface films are, among others: Aquatic biota releasing by-products (Dietz and Lafond 1950), leaching of allochtonous matter from land (Goldacre 1949), compounds of anthropogenic origin (Baier et al. 1974, Cross et al. 1987, Papers II and III), and atmospheric deposition (Hatcher and Parker 1974, Elzerman et al. 1979). Transport of energy and matter from the atmosphere to aquatic ecosystems follows several processes (Fig. 1). Air-water interface The structure of the surface film has been described with several models (Fig. 2). Figure 2. Surface film models proposed by
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