持久性有機污染物藉由海氣界面之傳輸作用對此類化合物在全球環境中分佈而言是相當重要的，而探討此種機制需要準確量測的濃度及經適當方式推估而得的物理化學參數來計算求得。本研究旨在分析高雄港區大氣及水中之多環芳香烴、多氯聯苯及六氯苯化合物的濃度，以計算出各化合物的海-氣交換通量。研究期間由2003 年12 月到2005 年1 月之間分別採樣並分析了二十二個水及空氣樣品。海氣通量計算係利用實測氣態及水中溶解態濃度及經鹽度與溫度校正之亨利常數代入Whitman’s thin-film 模式計算得出前述各化合物的通量。此外，本研究亦利用空氣及水樣中各化合物在顆粒相之濃度來推估多環芳香烴可能來源分布與多環芳香烴、多氯聯苯及六氯苯化合物的乾沈降通量。
研究結果顯示在多環芳香烴部份，揮發(volatile)及吸收(absorptive)的海氣通量以三環的phenanthrene 在2004 年4 月7 日及1 月27 日所測得之通量值最高，分別為+3560 ng m-2 day-1 及-1230 ng m-2 day-1 。同時，乾季(十月至三月)及雨季(四月至九月)分別所測得之多環芳香烴通量大小與方向均明顯不同。至於多氯聯苯同源物及六氯苯的通量則均為由水中進入空氣中(揮發)，最高的揮發通量為2003 年12 月在較高風速及水中濃度狀況下所測得，其測值為+172 ng m-2 day-1 (二氯聯苯)，而唯一的吸收通量則是2004 年1 月所測得，測值為-0.03 ng m-2 day-1 (二氯聯苯)。整體來說，乾季所測得的平均日通量為-727 ng m-2 day-1 ，而在雨季則測得+808 ng m-2 day -1 ，因此可以推估得出本研究中多環芳香烴化合物藉海氣交換在乾季揮發及雨季吸收之數量分別為4.0 及3.6 公斤。至於多氯聯苯及六氯苯每年總通量分別為57.4 及28.3 ×103 ng m-2 yr-1 ，而累計每年約有1.5 公斤的多氯聯苯及0.76 公斤的六氯苯由高雄港區藉由海氣交換方式進入大氣中。
利用同分異構物的比例判別方式，可以看出大氣中多環芳香烴的來源主要來自草、木柴及煤燃燒與部份來自石油燃燒來源。而水中的來源可能來自汽機車或船舶等運輸工具內燃機的不完全燃燒。至於大氣及水中多環芳香烴的主成份分析結果各分別得出三個有意義的主成份，在大氣方面，由主成份結果得出的可能來源分為內燃機排放，土壤或水中多環芳香烴的揮發及燃煤等，而在水中的來源則以內燃機排放，洩油及燃煤為主。若由多環芳香烴、多氯聯苯及六氯苯在空氣顆粒所測得的濃度來計算乾沈降通量，可以求出在本研究期間全年的多環芳香烴乾沈降通量與其海氣交換通量相近。相反的，多氯聯苯及六氯苯的乾沈降通量則遠低於其海氣交換通量。整體而言，高雄港區多環芳香烴海氣交換通量在乾季時呈現較強的吸收或較弱的揮發通量，而雨季則相反，至於多氯聯苯及六氯苯方面，則是全年海氣交換通量均以揮發通量為主。

Estimation of the transport of persistent organic pollutants via air-water exchange
requires precise field concentrations from advanced experimental techniques and
adequate physic-chemical parameters generated from proper methods. In this study,
concentrations of polycyclic aromatic hydrocarbons (PAHs), polychlorinated
biphenyls (PCBs) and hexachlorobenzene (HCB) in the ambient air and water column
of Kaohsiung Harbor lagoon were measured and used to determine the air-water
exchange fluxes of these compounds from December, 2003 to January, 2005. The
Whitman’s thin-film model was used by taking temperature and salinity corrected
Henry’s law constants into the model to calculate the fluxes. In addition, particulate
concentrations and composition in the ambient air and water column were used to
apportion PAH sources and dry particle deposition of PAHs, PCBs and HCB.
Instantaneous air-water exchange fluxes of PAHs, PCBs and HCB were calculated
from twenty-two pairs of air and water samples. The highest net volatile (+3560 ng
m-2 day-1) and absorptive (-1230 ng m-2 day-1) PAH fluxes in this study were both
obtained from the three-ring PAH, phenanthrene on April 7 and January 27 in 2004,
respectively. Differences of flux magnitude and direction between dry and rain season
were obvious for PAHs in this study. Most net fluxes of PCB homologues and HCB in
this study are from water to air (net volatilization). The highest net volatile flux
observed was +172 ng m-2 day-1 (dichlorobiphenyl) in December, 2003 due to
elevated wind speed and dissolved concentration, while the only net absorptive flux
observed in this study was -0.03 ng m-2 day-1 (dichlorobiphenyl) in January, 2004.
Mean daily PAH diffusive fluxes were -727 ng m-2 day-1 influx in dry season but +808
ng m-2 day -1 efflux in rain season and integrated 3.6 kg and 4.0 kg of PAHs were
absorbed into and emitted from harbor lagoon surface waters in dry and rain seasons,
respectively. The net PCBs and HCB fluxes suggest that the annual sum of 69 PCBs
and HCB measured in this study were mainly volatile (57.4 and 28.3 ×103 ng m-2 yr-1,
respectively) and integrated 1.5 kg and 0.76 kg of PCBs and HCB emitted from
harbor lagoon surface waters to ambient atmosphere in the year.
Sources apportionment by the isomer ratios, PAHs in the air phase were mainly
from grass, wood and coal combustion and some from liquid fuel combustion. Unlike
that in air phase, fluoranthene / fluoranthene + pyrene ratios of water phase suggest
PAHs were from incomplete-combusted fuel particles emitted from vehicle exhaust.
Principal component analysis (PCA) extracted three meaningful PCs for air and water
samples, respectively. For the air samples, the three major sources suggested by three
sources are vehicular emissions, volatilization to the air from contaminated soil or
waters and the coal-burning emission. Among the water samples, the three major
sources suggested by three sources are vehicular emissions, oil spill source and
coal-burning emission. Air particulate concentrations of PAHs, PCBs and HCB were
also used to calculate their dry particle deposition. Throughout our sampling
campaigns, PAH dry particle fluxes were quite comparable to fluxes of air-water
exchange. On the contrary, PCB and HCB dry particle deposition flux were negligible
comparing to their air-water exchange fluxes. Our results suggest PAHs exhibits
strong absorptive or weaker volatile fluxes in the dry season but the opposite in the
rain season. However, for PCBs and HCB, Kaohsiung Harbor water is potentially an
important source to ambient air.

中文摘要…………………………………………………………………………………………………………..….………II
ABSTRACT………………………………………………………………………………………………………………IV
TABLE OF CONTENTS……………………………………………………………………………….……..…VI
LIST OF TABLES…………………………………………………………………………………………………VIII
LIST OF FIGURES…………………………………………………………………………………………………IX

CHAPTER 1 INTRODUCTION…………………………………………………………………….…………1
1.1 NATURES OF PAHS, PCBS AND HCB………………………………………………………….……………….……………1
1.2 LONG-RANGE ATMOSPHERIC TRANSPORT OF PAHS, PCBS AND HCB………….……….….…..3
1.3 AIR-WATER EXCHANGE FLUXES…………………………………………………………………….………….……………3
1.4 BACKGROUND OF KAOHSIUNG HARBOR LAGOON………………………………………………….………5
1.5 OBJECTIVES……………………………………………………………………………………………….……………………..……………5
CHAPTER 2 METHODOLOGY……………………………………………………………………………11
2.1 SAMPLING SITES………………………………………………………………………………………………………….…….….…. 11
2.2 METEOROLOGICAL CONDITIONS AND ANCILLARY MEASUREMENTS…….………..……..11
2.3 AIR SAMPLING PROCEDURES…………………………………………………………..…………………….………..….…12
2.4 WATER SAMPLING PROCEDURES………………………………………………………………………….……..….……12
2.5 ANALYTICAL PROCEDURES………………………………………………………………………………….……….….……13
2.5.1 CHEMICALS…………………………………………………………………………………………………………………………13
2.5.2 WATER SAMPLES……………………………………………………………..………………………………………..….……13
2.5.3 AIR SAMPLES…………………………………………………...............................…………………………....….....….….….….14
2.5.4 QUANTIFICATION……………………………………..........................................………………………....………….………15
2.5.5 QA-QC………………………………………………….....................................................................…………………...………………16
2.6 AIR-WATER EXCHANGE MODEL…………………………………………………………………………….……………..17
2.6.1 MODELS FOR AIR-WATER EXCHANGE…………………………………………………………...……………17
2.6.2 COEFFICIENTS OF WHITMAN’S THIN FILM MODEL…………………………..………………….. 18
2.6.3 HENRY’S LAW CONSTANT………………………………………………..………………………..……………………21
2.7 PROPAGATION OF ERRORS FOR AIR-WATER EXCHANGE……………...………………………………25
2.8 SENSITIVITY ANALYSIS FOR DIFFUSIVE FLUX CALCULATIONS…………………………..……26
CHAPTER 3 DIFFUSIVE EXCHANGE OF PAHS ACROSS THE AIR-WATER INTERFACE OF KAOHSIUNG HARBOR LAGOON, TAIWAN………...……………33
3.1 DISSOLVED AND GAS PHASE CONCENTRATIONS………………………………….…………..……………33
3.2 INSTANTANEOUS GAS EXCHANGE FLUXES……………………………………………..………….……………34
3.3 ANNUAL FLUXES AND SEASONAL VARIATION………………………………………………….…………..…35
3.4 COMPARISON OF PAH DIFFUSIVE FLUXES IN KHH TO GLOBAL RESULTS……..………. 37
CHAPTER 4 DIFFUSIVE EXCHANGE OF PCBS AND HCB ACROSS THE AIR-WATER INTERFACE OF KAOHSIUNG HARBOR LAGOON, TAIWAN……………………………………………………………………………………………………….……………47
4.1 DISSOLVED AND GAS PHASE CONCENTRATIONS…………………………………………..……….………47
4.2 INSTANTANEOUS GAS EXCHANGE FLUXES…………………………………………….……..…………………48
4.3 ANNUAL FLUXES…………………………………………………..……………………………………..…………….………………50
4.4 COMPARISON OF TOTAL PCB DIFFUSIVE FLUXES IN KHH TO GLOBAL RESULTS………………………………………………………………..…………………………………………………….…...…………………51
CHAPTER 5 PAH AND PCB CONCENTRATIONS IN THE ATMOSPHERE AND WATER COLUMN OF KAOHSIUNG HARBOR LAGOON, TAIWAN…………………………………………………………………………………………….………………………61
5.1 PAH CONCENTRATIONS…………………………...........................................………………….......……................................... 61
5.2 PCB CONCENTRATIONS…………………………………………………………………...................................................………63
5.3 PAH COMPOSITION IN THE WATER COLUMN AND ATMOSPHERE…………...…………….……65
5.3.1 PAH SOURCES IDENTIFICATION BY ISOMER RATIOS…………………………………………..………65
5.3.2 MULTIVARIATE ANALYSIS……………………………...............................……………………..………..…………………66
5.4 DRY DEPOSITION OF PARTICLE BOUND PAHS, PCBS, AND HCB…………………...………..……68
CHAPTER 6 CONCLUSIONS AND SUGGESTIONS……………………………...…………82
6.1 CONCLUSIONS……………………………………………………………………………………………………………………………82
6.2 SUGGESTIONS FOR FUTURE WORKS…………………………………………………………………..………………86
REFERENCES…………………………………………………..…………………………….………..………………88

Achman, D. R., Brownawell, B. J., Zhang, L. C., 1996. Exchange of polychlorinated biphenyls between sediment and water in the Hudson River Estuary. Estuaries 19, 950-965.
Achman, D. R., Hornbuckle, K. C., Eisenreich, S. J., 1993. Volatilization of polychlorinated-biphenyls from Green Bay, Lake-Michigan. Environ. Sci. Technol. 27, 75-87.
Ahrens, M., Depree, C., 2004. Inhomogeneous distribution of polycyclic aromatic hydrocarbons in different size and density fractions of contaminated sediment from Auckland Harbour, New Zealand: an opportunity for mitigation. Mar. Pollut. Bull. 48, 341-350.
Alaee, M., Whittal, R. M., Strachan, W. M. J., 1996. The effect of water temperature and composition on Henry's Law constant for various PAH's. Chemosphere 32, 1153-1164.
Bailey, R. E., 2001. Global hexachlorobenzene emissions. Chemosphere 43, 167-182.
Bamford, H. A., Ko, F. C., Baker, J. E., 2002a. Seasonal and annual air-water exchange of polychlorinated biphenyls across Baltimore Harbor and the northern Chesapeake Bay. Environ. Sci. Technol. 36, 4245-4252.
Bamford, H. A., Offenberg, J. H., Larsen, R. K., Ko, F. C., Baker, J. E., 1999a. Diffusive exchange of polycyclic aromatic hydrocarbons across the air-water interface of the Patapsco River, an urbanized subestuary of the Chesapeake Bay. Environ. Sci. Technol. 33, 2138-2144.
Bamford, H. A., Poster, D. L., Baker, J. E., 1999b. Method for measuring the temperature dependence of the Henry's Law Constant of selected polycyclic aromatic hydrocarbons. Polycyclic Aromatic Compounds 14, 11-22.
Bamford, H. A., Poster, D. L., Baker, J. E., 1999c. Temperature dependence of Henry's law constants of thirteen polycyclic aromatic hydrocarbons between 4 degrees C and 31 degrees C. Environ. Toxicol. Chem. 18, 1905-1912.
Bamford, H. A., Poster, D. L., Huie, R. E., Baker, J. E., 2002b. Using extrathermodynamic relationships to model the temperature dependence of Henry's law constants of 209 PCB congeners. Environ. Sci. Technol. 36, 4395-4402.
Baumard, P., Budzinski, H., Garrigues, P., Dizer, H., Hansen, P. D., 1999. Polycyclic aromatic hydrocarbons in recent sediments and mussels (Mytilus edulis) from the Western Baltic Sea: occurrence, bioavailability and seasonal variations. Mar. Environ. Res. 47, 17-47.
Bidleman, T. F., McConnell, L. L., 1995. A review of field experiments to determine air-water gas-exchange of persistent organic pollutants. Sci. Total Environ. 159, 101-117.
Boehm, P. D., Page, D. S., Burns, W. A., Bence, A. E., Mankiewicz, P. J., Brown, J. S., 2001. Resolving the origin of the petrogenic hydrocarbon background in Prince William Sound, Alaska. Environ. Sci. Technol. 35, 471-479.
Boehm, P. D., Page, D. S., Gilfillan, E. S., Bence, A. E., Burns, W. A., Mankiewicz, P. J., 1998. Study of the fates and effects of the Exxon Valdez oil spill on benthic sediments in two bays in Prince William Sound, Alaska. 1. Study design, chemistry, and source fingerprinting. Environ. Sci. Technol. 32, 567-576.
Breivik, K., Sweetman, A., Pacyna, J., Jones, K., 2002. Towards a global historical emission inventory for selected PCB congeners - a mass balance approach 1. Global production and consumption.,. Sci. Total Environ. 290, 181-198.
Bremle, G., Larsson, P., 1998. PCB in the air during landfilling of a contaminated lake sediment. Atmos. Environ. 32, 1011-1019.
Broecker, W., Peng, T. H., 1984. Gas exchange measurements in natural systems. Gas transfer at water surfaces. Brutsaert, W., Jirka, G. Boston, MA, USA, D. Reidel: 479-493.
Brunner, S., Hornung, E., Santl, H., Wolff, E., Piringer, O. G., Altschuh, J., Bruggemann, R., 1990. Henry Law constants for polychlorinated-biphenyls - experimental-determination and structure property relationships. Environ. Sci. Technol. 24, 1751-1754.
Budzinski, H., Jones, I., Bellocq, J., Pierard, C., Garrigues, P., 1997. Evaluation of sediment contamination by polycyclic aromatic hydrocarbons in the Gironde estuary. Mar. Chem. 58, 85-97.
Burgess, R. M., Ahrens, M. J., Hickey, C. W., 2003. Geochemistry of PAHs in aquatic environments: source, persistence and distribution. PAHs: An Ecotoxicological Perspective. Douben, P. E. T. New York, John Wiley & Sons Ltd: 35-45.
Burns, W. A., Mankiewicz, P. J., Bence, A. E., Page, D. S., Parker, K. R., 1997. A principal-component and least-squares method for allocating polycyclic aromatic hydrocarbons in sediment to multiple sources. Environ. Toxicol. Chem. 16, 1119-1131.
Chao, W., Hsu, C., Guo, Y., 1997. Middle-ear disease in children exposed prenatally to polychlorinated-biphenyls and polychlorinated dibenzofurans. Arch. Environ. Health 52, 257-262.
Coleman, P. J., Lee, R. G. M., Alcock, R. E., Jones, K. C., 1997. Observations on PAH, PCB, and PCDD/F trends in UK urban air, 1991-1995. Environ. Sci. Technol. 31, 2120-2124.
Dachs, J., Bayona, J. M., Fowler, S. W., Miquel, J. C., Albaiges, J., 1996. Vertical fluxes of polycyclic aromatic hydrocarbons and organochlorine compounds in the western Alboran Sea (southwestern Mediterranean). Mar. Chem. 52, 75-86.
Dachs, J., Eisenreich, S. J., Baker, J. E., Ko, F. C., Jeremiason, J. D., 1999. Coupling of phytoplankton uptake and air-water exchange of persistent organic pollutants. Environ. Sci. Technol. 33, 3653-3660.
Dewulf, J., Drijvers, D., Vanlangenhove, H., 1995. Measurement of Henrys Law constant as function of temperature and salinity for the low-temperature range. Atmos. Environ. 29, 323-331.
Ding, X., Wang, X. M., Xie, Z. Q., Xiang, C. H., Mai, B. X., Sun, L. G., Zheng, M., Sheng, G. Y., Fu, J. M., Poschl, U., 2007. Atmospheric polycyclic aromatic hydrocarbons observed over the North Pacific Ocean and the Arctic area: Spatial distribution and source identification. Atmos. Environ. 41, 2061-2072.
Erickson, M. D., 1986. Analytical chemistry of PCBs. Boston, Ann Arbor Science, Pages.
Fang, G. C., Chang, K. F., Lu, C. S., Bai, H. L., 2004a. Estimation of PAHs dry deposition and BaP toxic equivalency factors (TEFs) study at Urban, Industry Park and rural sampling sites in central Taiwan, Taichung. Chemosphere 55, 787-796.
Fang, G. C., Wu, Y. S., Chen, M. H., Ho, T. T., Huang, S. H., Rau, J. Y., 2004b. Polycyclic aromatic hydrocarbons study in Taichung, Taiwan, during 2002-2003. Atmos. Environ. 38, 3385-3391.
Fang, M.-D., Hsieh, P.-C., Ko, F.-C., Baker, J. E., Lee, C.-L., 2007. Sources and distribution of polycyclic aromatic hydrocarbons in the sediments of Kaoping River and Submarine Canyon system. Marine Pollution Bulletin (in press).
Fang, M. D., Lee, C. L., Nung, W. C. (2004c). Distribution and sources recognition of PAHs and PCBs in the sediment of Kaohsiung Harbour, Taiwan. Coastal Environment. Alicante, Spain.
Fang, M. D., Lee, C. L., Yu, C. S., 2003. Distribution and source recognition of polycyclic aromatic hydrocarbons in the sediments of Hsin-ta Harbour and adjacent coastal areas, Taiwan. Mar. Pollut. Bull. 46, 941-953.
Fraser, M. P., Cass, G. R., Simoneit, B. R. T., Rasmussen, R. A., 1998. Air quality model evaluation data for organics. 5. C-6-C-22 nonpolar and semipolar aromatic compounds. Environ. Sci. Technol. 32, 1760-1770.
Fuller, E. N., Schettler, P. D., Giddings, J. C., 1966. A new method for prediction of binary gas-phase diffusion coefficient. Ind. Eng. Chem. 58, 19-27.
Garcia-Flor, N., Guitart, C., Abalos, M., Dachs, J., Bayona, J. M., Albaiges, J., 2005. Enrichment of organochlorine contaminants in the sea surface microlayer: An organic carbon-driven process. Mar. Chem. 96, 331-345.
Garcia, A., Den Boer, A., De Jong, A., 1996. Determination of non- and mono-ortho-polychlorinated biphenyls in background ambient air. Environ. Sci. Technol. 30, 1032-1037.
Gigliotti, C. L., Brunciak, P. A., Dachs, J., Glenn, T. R., Nelson, E. D., Totten, L. A., Eisenreich, S. J., 2002. Air-water exchange of polycyclic aromatic hydrocarbons in the New York-New Jersey, Usa, Harbor Estuary. Environ. Toxicol. Chem. 21, 235-244.
Gigliotti, C. L., Totten, L. A., Offenberg, J. H., Dachs, J., Reinfelder, J. R., Nelson, E. D., Glenn, T. R., Eisenreich, S. J., 2005. Atmospheric concentrations and deposition of polycyclic aromatic hydrocarbons to the Mid-Atlantic East Coast Region. Environ. Sci. Technol. 39, 5550-5559.
Gordon, J. E., Thorne, R. L., 1967a. Salt effects on activity coefficients of naphthalene in mixed aqueous electrolyte solutions. I. Mixtures of two salts. J. Phys. Chem. 71, 4390-4399.
Gordon, J. E., Thorne, R. L., 1967b. Salt effects on non-electrolyte activity coefficients in mixed aqueous electrolyte solutions. II. Artificial and natural sea waters. Geochim. Cosmochim. Acta 31, 2433-2443.
Guo, Y., Ryan, J., Lau, B., Yu, M., Hsu, C., 1997. Blood-serum levels of pcbs and pcdfs in yucheng women 14 years after exposure to a toxic rice oil. Arch. Environ. Con. Tox. 33, 104-108.
Gustafson, K. E., Dickhut, R. M., 1997. Gaseous exchange of polycyclic aromatic hydrocarbons across the air-water interface of southern Chesapeake Bay. Environ. Sci. Technol. 31, 1623-1629.
Gustafsson, K. E., Dickhut, R. M., 1997. Particle/gas concentrations and distributions of PAHs in the atmosphere of southern Chesapeake Bay. Environ. Sci. Technol. 31, 140-147.
Hargrave, B. T., Barrie, L. A., Bidleman, T. F., Welch, H. E., 1997. Seasonality in exchange of organochlorines between Arctic air and seawater. Environ. Sci. Technol. 31, 3258-3266.
Harrison, R. M., Smith, D. J. T., Luhana, L., 1996. Source apportionment of atmospheric polycyclic aromatic hydrocarbons collected from an urban location in Birmingham, U.K. Environ. Sci. Technol. 30, 825-832.
Hartmann, P. C., Quinn, J. G., Cairns, R. W., King, J. W., 2004. The distribution and sources of polycyclic aromatic hydrocarbons in Narragansett Bay surface sediments. Mar. Pollut. Bull. 48, 351-358.
Hileman, B., 1992. Ban on persistent toxic compounds urged. Chem. Eng. News 6, 6.
Hornbuckle, K. C., Sweet, C. W., Pearson, R. F., Swackhamer, D. L., Eisenreich, S. J., 1995. Assessing annual water-air fluxes of polychlorinated-biphenyls in Lake-Michigan. Environ. Sci. Technol. 29, 869-877.
Iwata, H., Tanabe, S., Sakal, N., Tatsukawa, R., 1993. Distribution of persistent organochlorines in the oceanic air and surface seawater and the role of ocean on their global transport and fate. Environ. Sci. Technol. 27, 1080-1098.
Jantunen, L. M., Bidleman, T. F., 2006. Henry's law constants for hexachlorobenzene, p,p'-DDE and components of technical chlordane and estimates of gas exchange for Lake Ontario. Chemosphere 62, 1689-1696.
Jeremiason, J. D., Hornbuckle, K. C., Eisenreich, S. J., 1994. PCBs in Lake-Superior, 1978-1992 - decreases in water concentrations reflect Loss by volatilization. Environ. Sci. Technol. 28, 903-914.
Jurado, E., Jaward, F., Lohmann, R., Jones, K. C., Simo, R., Dachs, J., 2005. Wet deposition of persistent organic pollutants to the global oceans. Environ. Sci. Technol. 39, 2426-2435.
Jurado, E., Jaward, F. M., Lohmann, R., Jones, K. C., Simo, R., Dachs, J., 2004a. Atmospheric dry deposition of persistent organic pollutants to the Atlantic and inferences for the global oceans. Environ. Sci. Technol. 38, 5505-5513.
Jurado, E., Lohmann, R., Meijer, S., Jones, K. C., Dachs, J., 2004b. Latitudinal and seasonal capacity of the surface oceans as a reservoir of polychlorinated biphenyls. Environ. Pollut. 128, 149-162.
Kimbrough, R., Doemland, M., Krouskas, C., 2001. Analysis of research studying the effects of polychlorinated-biphenyls and related chemicals on neurobehavioral development in children. Vet. Hum. Tox. 43, 220-228.
Ko, F. C., Baker, J. E., 2004. Seasonal and annual loads of hydrophobic organic contaminants from the Susquehanna River basin to the Chesapeake Bay. Mar. Pollut. Bull. 48, 840-851.
Kucklick, J. R., Hinckley, D. A., Bidleman, T. F., 1991. Determination of Henry Law constants for hexachlorocyclohexanes in distilled water and artificial seawater as a function of temperature. Mar. Chem. 34, 197-209.
Larsen, R. K., Baker, J. E., 2003. Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere: A comparison of three methods. Environ. Sci. Technol. 37, 1873-1881.
Latimer, j. S., Zheng, J., 2003. The sources, transport, and fate of PAHs in the marine environment. PAHs: An Ecotoxicological Perspective. Douben, P. E. T. New York, John Wiley & Sons Ltd: 9-33.
Lee, B. K., Lee, C. B., 2004. Development of an improved dry and wet deposition collector and the atmospheric deposition of PAHs onto Ulsan Bay, Korea. Atmos. Environ. 38, 863-871.
Lee, W. J., Lin, S. J., Chen, Y. Y., Wang, Y. F., Sheu, H. L., Su, C. C., Fan, Y. C., 1996. Polychlorinated Biphenyls in the ambient air of petroleum refinery, urban and rural areas. Atmos. Environ. 30, 2371-2378.
Li, C. K., Kamens, R. M., 1993. The use of polycyclic armomatic hydrocarbons as source signatures in receptor modeling. Atmos. Environ. 27, 523-532.
Li, J., Zhang, G., Li, X. D., Qi, S. H., Liu, G. Q., Peng, X. Z., 2006. Source seasonality of polycyclic aromatic hydrocarbons (PAHs) in a subtropical city, Guangzhou, South China. Sci. Total Environ. 355, 145-155.
Liss, P. S., 1973. Processes of gas exchange across an air-water interface. Deep-Sea Research 20, 221-238.
Livingstone, D. M., Imboden, D. M., 1993. The nonlinear influence of wind-speed variability on gas transfer in lakes. Tellus Series B-Chemical and Physical Meteorology 45, 275-295.
Lohmann, R., Nelson, E., Eisenreich, S. J., Jones, K. C., 2000. Evidence for dynamic air-water exchange of PCDD/Fs: A study in the Raritan Bay/Hudson River Estuary. Environ. Sci. Technol. 34, 3086-3093.
Luo, X. J., Mai, B. X., Yang, Q. S., Fu, J. M., Sheng, G. Y., Wang, Z. S., 2004. Polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides in water columns from the Pearl River and the Macao harbor in the Pearl River Delta in South China. Mar. Pollut. Bull. 48, 1102-1115.
Mackay, D., Yeun, A. T. K., 1983. Mass-transfer coefficient correlations for volatilization of organic solutes from water. Environ. Sci. Technol. 17, 211-217.
May, W. E., Wise, S. A., 1984. Liquid-chromatographic determination of polycyclic aromatic-hydrocarbons in air particulate extracts. Anal. Chem. 56, 225-232.
Mullin, M. D., Pochini, C. M., McCrindle, S., Romkes, M., Safe, S. H., Safe, L. M., 1984. High-resolution PCB analysis - synthesis and chromatographic properties of all 209-PCB congeners. Environ. Sci. Technol. 18, 468-476.
Neff, J. M., 1979. Polycyclic aromatic hydrocarbons in the aquatic environment. London, Applied Science Publishers Ltd., Pages.
Nelson, E. D., McConnell, L. L., Baker, J. E., 1998. Diffusive exchange of gaseous polycyclic aromatic hydrocarbons and polychlorinated biphenyls across the air-water interlace of the Chesapeake Bay. Environ. Sci. Technol. 32, 912-919.
Offenberg, J. H., Baker, J. E., 1999. Influence of Baltimore's urban atmosphere on organic contaminants over the northern Chesapeake Bay. Journal of the Air & Waste Management Association 49, 959-965.
Offenberg, J. H., Baker, J. E., 2000. PCBs and PAHs in southern Lake Michigan in 1994 and 1995: Urban atmospheric influences and long-term declines. Journal of Great Lakes Research 26, 196-208.
Offenberg, J. H., Baker, J. E., 2002. The influence of aerosol size and organic carbon content on gas/particle partitioning of polycyclic aromatic hydrocarbons (PAHs). Atmos. Environ. 36, 1205-1220.
Othmer, D. F., Thakar, M. S., 1953. Correlating diffusion coefficients in liquids. Ind. Eng. Chem. 45, 589-593.
Page, D. S., Boehm, P. D., Douglas, G. S., Bence, A. E., Burns, W. A., Mankiewicz, P. J., 1999. Pyrogenic polycyclic aromatic hydrocarbons in sediments record past human activity: A case study in Prince William Sound, Alaska. Mar. Pollut. Bull. 38, 247-260.
Pandit, G. G., Sahu, S. K., 2001. Gas exchange of OCPs across the air-water interface at the creek adjoining Mumbai harbour, India. Journal of Environmental Monitoring 3, 635-638.
Park, J. S., Wade, T. L., Sweet, S., 2001. Atmospheric deposition of organochlorine contaminants to Galveston Bay, Texas. Atmos. Environ. 35, 3315-3324.
Park, J. S., Wade, T. L., Sweet, S. T., 2002a. Atmospheric deposition of PAHs, PCBs, and organochlorine pesticides to Corpus Christi Bay, Texas. Atmos. Environ. 36, 1707-1720.
Park, S. S., Kim, Y. J., Kang, C. H., 2002b. Atmospheric polycyclic aromatic hydrocarbons in Seoul, Korea. Atmos. Environ. 36, 2917-2924.
Perez, S., Dachs, J., Barcelo, D., 2003. Sea breeze modulated volatilization of polycyclic aromatic hydrocarbons from the Masnou Harbor (NW Mediterranean sea). Environ. Sci. Technol. 37, 3794-3802.
Perlinger, J. A., Tobias, D. E., Morrow, P. S., Doskey, P. V., 2005. Evaluation of novel techniques for measurement of air-water exchange of persistent bioaccumulative toxicants in Lake Superior. Environ. Sci. Technol. 39, 8411-8419.
Poor, N., Tremblay, R., Kay, H., Bhethanabotla, V., Swartz, E., Luther, M., Campbell, S., 2004. Atmospheric concentrations and dry deposition rates of polycyclic aromatic hydrocarbons (PAHs) for Tampa Bay, Florida, USA. Atmos. Environ. 38, 6005-6015.
Rice, C. P., Chernyak, S. M., McConnell, L. L., 1997. Henry's law constants for pesticides measured as a function of temperature and salinity. J. Agric. Food Chem. 45, 2291-2298.
Rowe, A. A., Totten, L. A., Xie, M. G., Fikslin, T. J., Eisenreich, S. J., 2007. Air-water exchange of polychlorinated biphenyls in the delaware river. Environ. Sci. Technol. 41, 1152-1158.
Salau, J. S. I., Tauler, R., Bayona, J. M., Tolosa, I., 1997. Input characterization of sedimentary organic contaminants and molecular markers in the Northwestern Mediterranean Sea by exploratory data analysis. Environ. Sci. Technol. 31, 3482-3490.
Schwarzenbach, R. P., Gschwend, P. M., Imboden, D. M., 2003. Environmental organic chemistry. New Jersey, John Wiley & sons, Pages.
Shannigrahi, A. S., Fukushima, T., Ozaki, N., 2005. Comparison of different methods for measuring dry deposition fluxes of particulate matter and polycyclic aromatic hydrocarbons (PAHs) in the ambient air. Atmos. Environ. 39, 653-662.
Sheu, H. L., Lee, W. J., Lin, S. J., Fang, G. C., Chang, H. C., You, W. C., 1997. Particle-bound PAH content in ambient air. Environ. Pollut. 96, 369-382.
Shoemaker, D. P., Garland, G. W., Steinfeld, J. I., 1974. Propagation of errors. Experiments in physical chemistry. New York, NY, USA, McGraw-Hill: 51-58.
Silliman, J. E., Meyers, P. A., Ostrom, P. H., Ostrom, N. E., Eadie, B. J., 2000. Insights into the origin of perylene from isotopic analyses of sediments from Saanich Inlet, British Columbia. Org. Geochem. 31, 1133-1142.
Sinkkonen, S., Kamarainen, N., Paasivirta, J., Lahtipera, M., Lammi, R., 1998. Alkylated dibenzothiophenes in pine needles from pulp and paper mill environment. Chemosphere 36, 2475-2482.
Soclo, H. H., Affokpon, A., Sagbo, A., Thomson, S., Budzinski, H., Garrigues, P., Matsuzawa, S., Rababah, A., 2002. Urban runoff contribution to surface sediment accumulation for polycyclic aromatic hydrocarbons in the Cotonou lagoon, Benin. Polycyclic Aromatic Compounds 22, 111-128.
Strand, A., Hov, F., 1996. A model strategy fro the simulation of chlorinated hydrocarbon distribution in the global environment. Water, Air, Soil Pollut. 86, 283-316.
Tasdemir, Y., Odabasi, M., Vardar, N., Sofuoglu, A., Murphy, T. J., Holsen, T. M., 2004. Dry deposition fluxes and velocities of polychlorinated biphenyls (PCBs) associated with particles. Atmos. Environ. 38, 2447-2456.
Tateya, S., Tanabe, S., Tatsukawa, R., 1988. PCBs on the globe. Toxic contamination in large lakes. Schmidtke, N. W. Chelsa, Michigan, USA, Lewis Publishers. III: 237-281.
ten Hulscher, T. E. M., Vandervelde, L. E., Bruggeman, W. A., 1992. Temperature-dependence of Henry Law constants for selected chlorobenzenes, polychlorinated-biphenyls and polycyclic aromatic-hydrocarbons. Environ. Toxicol. Chem. 11, 1595-1603.
Tenhulscher, T. E. M., Vandervelde, L. E., Bruggeman, W. A., 1992. Temperature-Dependence of Henry Law Constants for Selected Chlorobenzenes, Polychlorinated-Biphenyls and Polycyclic Aromatic-Hydrocarbons. Environ. Toxicol. Chem. 11, 1595-1603.
Totten, L. A., Brunciak, P. A., Gigliotti, C. L., Dachs, J., Glenn, T. R., Nelson, E. D., Eisenreich, S. J., 2001. Dynamic air-water exchange of polychlorinated biphenyls in the New York - New Jersey Harbor Estuary. Environ. Sci. Technol. 35, 3834-3840.
Totten, L. A., Gigliotti, C. L., Offenberg, J. H., Baker, J. E., Eisenreich, S. J., 2003. Reevaluation of air-water exchange fluxes of PCBs in Green Bay and southern Lake Michigan. Environ. Sci. Technol. 37, 1739-1743.
Totten, L. A., Gigliotti, C. L., Vanry, D. A., Offenberg, J. H., Nelson, E. D., Dachs, J., Reinfelder, J. R., Eisenreich, S. J., 2004. Atmospheric concentrations and deposition of polychorinated biphenyls to the Hudson River Estuary. Environ. Sci. Technol. 38, 2568-2573.
Tsai, P., Hoenicke, R., Yee, D., 2002. Atmospheric concentrations and fluxes of organic compounds in the northern San Francisco estuary. Environ. Sci. Technol. 36, 4741-4747.
Tsapakis, M., Apostolaki, M., Eisenreich, S., Stephanou, E. G., 2006. Atmospheric deposition and marine sedimentation fluxes of polycyclic aromatic hydrocarbons in the eastern Mediterranean basin. Environ. Sci. Technol. 40, 4922-4927.
van Birgelen, A., 1998. Hexachlorobenzene as a possible major contributor to the dioxin activity of human milk. Environ. Health Perspect. 106, 683-688.
Venkataraman, C., Lyons, J. M., Friedlander, S. K., 1994. Size distributions of polycyclic aromatic-hydrocarbons and elemental carbon .1. Sampling, measurement methods, and source characterization. Environ. Sci. Technol. 28, 555-562.
Venkatesan, M. I., 1988. Occurrence and possible sources of perylene in marine-sediments - a review. Mar. Chem. 25, 1-27.
Wang, Z. D., Fingas, M., Shu, Y. Y., Sigouin, L., Landriault, M., Lambert, P., Turpin, R., Campagna, P., Mullin, J., 1999. Quantitative characterization of PAHs in burn residue and soot samples and differentiation of pyrogenic PAHs from petrogenic PAHs - The 1994 Mobile Burn Study. Environ. Sci. Technol. 33, 3100-3109.
Wania, F., Axelman, J., Broman, D., 1998. A review of processes involved in the exchange of persistent organic pollutants across the air-sea interface. Environ. Pollut. 102, 3-23.
Wanninkhof, R., Ledwell, J., Crusius, J., 1990. Gas transfer velocities on lakes measured with sulfur hexafluoride. Air-water mass transfer. Wilhelms, S., Gulliver, J. New York, NY, USA, American Society of Civil Engineers,: 441-458.
Whitman, W. G., 1923. The two-film theory of gas absorption. Chem. Met. Eng. 29, 146-148.
Wu, W. Z., Schramm, K. W., Henkelmann, B., Xu, Y., Yediler, A., Kettrup, A., 1997. PCDD/F-s, PCBs, HCHs and HCB in sediments and soils of Ya-Er lake area in China: Results on residual levels and correlation to the organic carbon and particle size. Chemosphere 34, 191-202.
Xie, W. H., Shiu, W. Y., Mackay, D., 1997. A review of the effect of salts on the solubility of organic compounds in seawater. Mar. Environ. Res. 44, 429-444.
Yu, M., Hsu, C., Guo, Y., Lai, T., Chen, S., Luo, J., 1994. Disordered behavior in the early-born Taiwan Yucheng Children. Chemosphere. 29, 2413-2422.
Yunker, M. B., Macdonald, R. W., Vingarzan, R., Mitchell, R. H., Goyette, D., Sylvestre, S., 2002. PAHs in the Fraser River basin: a critical appraisal of PAH ratios as indicators of PAH source and composition. Org. Geochem. 33, 489-515.
Zhang, H. X., Eisenreich, S. J., Franz, T. R., Baker, J. E., Offenberg, J. H., 1999. Evidence for increased gaseous PCB fluxes to Lake Michigan from Chicago. Environ. Sci. Technol. 33, 2129-2137.