KENTSEL BİR BÖLGEDE ATMOSFERİK PCDD/F KONSANTRASYONLARI KULLANILARAK TOPRAK VE SUCUL ORTAMLARDAKİ SEVİYELERİNİN TAHMİN EDİLMESİ

Öz

Poliklorlu dibenzo-p-dioksinler ve dibenzofuranlar (PCDD/F’ler) Stokholm Sözleşmesi’nin EK-C kısmında listelenmiş, insan ve çevre sağlığı açısından önemli risk teşkil eden kalıcı organik kirleticilerdendir. PCDD/F’ler kaynaktan salındıktan sonra atmosferik çökelme ve dağılım mekanizmaları ile toprak ve su ortamına karışabilmektedirler. Biyolojik olarak zor bozunabilme özellikleri sayesinde bu ortamlarda yaygın olarak bulunabilmekte ve farklı canlı ve ortamlara taşınabilmektedirler. PCDD/F’lerin farklı ortamlardaki konsantrasyon seviyelerinin belirlenmesi bu kirleticilerin davranış mekanizmalarının anlaşılması açısından önem taşımaktadır. Türkiye’de toprak ortamı için oldukça az sayıda ölçüm verisi bildirilmiş olup sucul ortam için bildirilen herhangi bir veri bulunmamaktadır. Bu çalışmada Bursa şehrinin kentsel bir bölgesinde dört mevsimi kapsayacak şekilde ölçümü yapılmış olan atmosferik PCDD/F konsantrasyonları kullanılarak çeşitli denge durumu eşitlikleri yardımı ile toprak ve sucul ortamlardaki PCDD/F konsantrasyon seviyelerinin araştırılması amaçlanmıştır. Buna göre toprak ve sucul ortam için hesaplanan ortalama PCDD/F konsantrasyonlarının sırasıyla 702,74±553,74 pg/g (21,14±13,41 pg TEQ/g) ve 0,8±0,61 pg/L (0,12±0,08 pg TEQ/L) olduğu belirlenmiştir. Bu değerlerin literatürde bildirilen çeşitli çalışmalar ile uyum içinde olduğu görülmüştür. En yüksek konsantrasyon değerleri iki ortam için de kış ayları için hesaplanmış, mevsimsel etkinin konsantrasyon seviyeleri üzerindeki etkisi açıkça gözlemlenmiştir.

Anahtar Kelimeler

• Dioksin
• dağılım katsayısı
• denge durumu
• Henry yasası
• su
• toprak

Destekleyen Kurum

Türkiye Bilimsel ve Teknolojik Araştırma Kurumu (TÜBİTAK)

Proje Numarası

TÜBİTAK 121Y473

Etik Beyan

Etik Onayına ihtiyaç yoktur.

Teşekkür

TÜBİTAK'a finansal desteğinden dolayı teşekkür ederiz.

Estimation of PCDD/F Levels in Soil and Aquatic Environments Using the Atmospheric Concentrations in an Urban Site

Öz

Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) are persistent organic pollutants listed in Annex C of the Stockholm Convention, which pose a significant risk to public and environmental health. PCDD/Fs, after being released from the source, can enter the soil and water environment through atmospheric deposition and partition mechanisms. Due to their characteristic of difficult biodegradability, they can be widely found in these environments and can be transported to different living organisms and environments. Determination of the concentration levels of PCDD/Fs in different environments is important for understanding the behavioural mechanisms of these pollutants. In Türkiye, few measurement data have been reported for the soil environment, and currently, there is no data reported for the aquatic environment. In this study, it was aimed to investigate the PCDD/F concentration levels in soil and aquatic environments by using atmospheric PCDD/F concentrations measured over four seasons in an urban area of Bursa city by means of various equilibrium equations. Accordingly, the mean total PCDD/F concentrations estimated for soil and aquatic environment were 702.74±553.74 pg/g (21.14±13.41 pg TEQ/g) and 0.8±0.61 pg/L (0.12±0.08 pg TEQ/L), respectively. These values were found to be in agreement with various studies reported in the literature. The highest concentration values were estimated in winter months for both environments, and the effect of seasonal effect on concentration levels was clearly observed.

Anahtar Kelimeler

• Dioxin
• partition coefficient
• equilibrium state
• Henry
• water
• soil

Proje Numarası

TÜBİTAK 121Y473

Kaynakça

1. Alimohammadi, M., & Lake, C. (2022). Fate and transport of particle matter during GEOTextile tube dewatering of a dioxin and furan (PCDD/F) contaminated sediment. Geotextiles and Geomembranes, 50(2), 203–215. https://doi.org/10.1016/j.geotexmem.2021.09.006
2. Bakoglu, M., Karademir, A., & Durmusoglu, E. (2005). Evaluation of PCDD/F levels in ambient air and soils and estimation of deposition rates in Kocaeli, Turkey. Chemosphere, 59(10), 1373–1385. https://doi.org/10.1016/j.chemosphere.2004.12.029
3. Bei, J., Xu, X., Zhan, M., Li, X., Jiao, W., Khachatryan, L., & Wu, A. (2022). Revealing the Mechanism of Dioxin Formation from Municipal Solid Waste Gasification in a Reducing Atmosphere. Environmental Science & Technology, 56(20), 14539–14549. https://doi.org/10.1021/acs.est.2c05830
4. Caliskan, B., Celik, S., Sakin, A. E., & Tasdemir, Y. (2025). Atmospheric polycyclic aromatic hydrocarbon concentrations in a semi-urban site: temporal variation, risk assessment, source identification, and estimation of levels in diverse environments. Environmental Toxicology and Chemistry, 44(3), 683–697. https://doi.org/10.1093/etojnl/vgaf025
5. Chakraborty, P., Selvaraj, S., Nakamura, M., Prithiviraj, B., Cincinelli, A., & Bang, J. J. (2018). PCBs and PCDD/Fs in soil from informal e-waste recycling sites and open dumpsites in India: Levels, congener profiles and health risk assessment. Science of The Total Environment, 621, 930–938. https://doi.org/10.1016/j.scitotenv.2017.11.083
6. Chi, K. H., Luo, S., Kao, S. J., Hsu, W.-T., & Lee, T. Y. (2015). Sources and Deposition Fluxes of PCDD/Fs in the Largest Reservoir System in Taiwan before and after Typhoon Morakot. Aerosol and Air Quality Research, 15(4), 1227–1239. https://doi.org/10.4209/aaqr.2014.10.0235
7. Cho, H.-K., Khuman, S. N., Cho, I.-G., Park, M.-K., & Choi, S.-D. (2024). Spatial distributions and source identification of PCDD/Fs and PCBs in soils and pine needles in the multi-industrial city of Ulsan, South Korea. Chemosphere, 369, 143821. https://doi.org/10.1016/j.chemosphere.2024.143821
8. Cortés, J., González, C. M., Morales, L., Abalos, M., Abad, E., & Aristizábal, B. H. (2014). PCDD/PCDF and dl-PCB in the ambient air of a tropical Andean city: Passive and active sampling measurements near industrial and vehicular pollution sources. Science of The Total Environment, 491–492, 67–74. https://doi.org/10.1016/j.scitotenv.2014.01.113

9. Demircioglu, E., Sofuoglu, A., & Odabasi, M. (2011). Particle-phase dry deposition and air–soil gas exchange of polycyclic aromatic hydrocarbons (PAHs) in Izmir, Turkey. Journal of Hazardous Materials, 186(1), 328–335. https://doi.org/10.1016/j.jhazmat.2010.11.005
10. Deng, Y., Peng, P., Ren, M., Song, J., & Huang, W. (2011). The winter effect on formation of PCDD/Fs in Guangzhou by vehicles: A tunnel study. Atmospheric Environment, 45(15), 2541–2548. https://doi.org/10.1016/j.atmosenv.2011.02.022
11. DeVito, M., Bokkers, B., van Duursen, M. B. M., van Ede, K., Feeley, M., Antunes Fernandes Gáspár, E., Haws, L., Kennedy, S., Peterson, R. E., Hoogenboom, R., Nohara, K., Petersen, K., Rider, C., Rose, M., Safe, S., Schrenk, D., Wheeler, M. W., Wikoff, D. S., Zhao, B., & van den Berg, M. (2024). The 2022 world health organization reevaluation of human and mammalian toxic equivalency factors for polychlorinated dioxins, dibenzofurans and biphenyls. Regulatory Toxicology and Pharmacology, 146, 105525. https://doi.org/10.1016/j.yrtph.2023.105525
12. Ding, L., Li, Y., Wang, P., Li, X., Zhao, Z., Zhang, Q., Tuan, T., & Jiang, G. (2012). Seasonal trend of ambient PCDD/Fs in Tianjin City, northern China using active sampling strategy. Journal of Environmental Sciences, 24(11), 1966–1971. https://doi.org/10.1016/S1001-0742(11)61058-9
13. Gao, L., Zhang, Q., Zhang, B., Liu, W., & Xiao, K. (2014). Polychlorinated dibenzo-p-dioxins and dibenzofurans in water and six fish species from Dongting Lake, China. Chemosphere, 114, 150–157. https://doi.org/10.1016/j.chemosphere.2014.04.015
14. Gülegen, B., Noori, A. A., & Tasdemir, Y. (2024). Urban air PCDD/Fs: Atmospheric concentrations, temporal changes, gas/particle partitioning, possible sources and cancer risks. Science of The Total Environment, 934, 173231. https://doi.org/10.1016/j.scitotenv.2024.173231
15. Güzel, B., Çetintürk, K., Canlı, O., & Karademir, A. (2024). Spatial distribution, source identification, and risk assessment of polychlorinated organic pollutants (PCDD/Fs and DL-PCBs) in the sediments of the largest urban water supply area (Iznik lake) in the Marmara region, Bursa, Türkiye. CATENA, 234, 107566. https://doi.org/10.1016/j.catena.2023.107566
16. Harner, T., Green, N. J. L., & Jones, K. C. (2000). Measurements of Octanol−Air Partition Coefficients for PCDD/Fs: A Tool in Assessing Air−Soil Equilibrium Status. Environmental Science & Technology, 34(15), 3109–3114. https://doi.org/10.1021/es000970m
17. Hippelein, M., & McLachlan, M. S. (1998). Soil/Air Partitioning of Semivolatile Organic Compounds. 1. Method Development and Influence of Physical−Chemical Properties. Environmental Science & Technology, 32(2), 310–316. https://doi.org/10.1021/es9705699
18. Hsu, Y.-C., Que, D. E., Gou, Y.-Y., Tsou, T.-C., Liu, C.-K., Wang, Y.-L., Hou, W.-C., Lin, Y.-H., Liu, W.-Y., Chao, H.-R., & Lee, W.-J. (2018). National surveillance of 2,3,7,8-substituted polychlorinated dibenzo-p-dioxins/furans in soil in Taiwan. Chemosphere, 203, 239–252. https://doi.org/10.1016/j.chemosphere.2018.03.191
19. Japan Government, (2012). Dioxins, Japan.
20. Khairy, M., Barrett, K., & Lohmann, R. (2015). Changing sources of polychlorinated dibenzo- p -dioxins and furans in sediments and ecological risk for nekton in the lower Passaic River and Newark Bay, New Jersey, USA. Environmental Toxicology and Chemistry, 35(3), 550–562. https://doi.org/10.1002/etc.3223
21. Khoury, N., Martínez, M. Á., Paz-Graniel, I., Martínez-González, M. Á., Corella, D., Castañer, O., Martínez, J. A., Alonso-Gómez, Á. M., Wärnberg, J., Vioque, J., Romaguera, D., López-Miranda, J., Estruch, R., Tinahones, F. J., Lapetra, J., Serra-Majem, J. L., Bueno-Cavanillas, A., Tur, J. A., Sanjurjo, S. C., … Salas-Salvadó, J. (2023). Dietary intake of polychlorinated dibenzo-p-dioxins and furans, adiposity and obesity status. Environmental Research, 227, 115697. https://doi.org/10.1016/j.envres.2023.115697
22. Le, L. T. H., Dat, N. D., Minh, N. H., & Nguyen, K.-A. (2019). Characteristics of PCDD/Fs in soil and sediment samples collected from A-So former airbase in Central Vietnam. Science of The Total Environment, 661, 27–34. https://doi.org/10.1016/j.scitotenv.2019.01.163
23. Lei, R., Liu, W., He, Y., Jia, T., Li, C., Su, W., & Xing, Y. (2024). Spatial distributions, behaviors, and sources of PCDD/Fs in surface water and sediment from the Yangtze River Delta. Environmental Research, 251, 118540. https://doi.org/10.1016/j.envres.2024.118540
24. Li, W., Li, C., Chen, Z., Ding, N., & Cai, Z. (2014). Levels of polychlorinated dibenzo-p-dioxins and dibenzofurans in mountainous and park soils in Beijing, China. International Journal of Environmental Analytical Chemistry, 94(7), 691–711. https://doi.org/10.1080/03067319.2014.891106
25. Liang, M., Gao, Y., Shen, Y., Zhang, X., Gu, J., & Ji, G. (2024). Serum metabolism distribution in individuals exposed to dioxins: A case study of residents near the municipal solid waste incinerators in China. Science of The Total Environment, 947, 174431. https://doi.org/10.1016/j.scitotenv.2024.174431
26. Liang, Y., Liu, H., Wang, L., Zhao, J., Li, S., Yi, L., Jiang, S., Lu, Z., & Zhang, G. (2025). A new yeast-based bioreporter for simple, sensitive, and cost-effective detection of dioxin-like compounds. Sensors and Actuators B: Chemical, 423, 136730. https://doi.org/10.1016/j.snb.2024.136730
27. Liu, C., Yu, S., Song, W., & Peng, S. (2024). Investigation and risk assessment of dioxins and dioxin-like PCBs in main aquatic products in market from Shanghai. Microchemical Journal, 207, 111925. https://doi.org/10.1016/j.microc.2024.111925
28. Liu, Y., Peng, P., Li, X., Zhang, S., & Ren, M. (2008). Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in water and suspended particulate matter from the Xijiang River, China. Journal of Hazardous Materials, 152(1), 40–47. https://doi.org/10.1016/j.jhazmat.2007.06.071
29. Lohmann, R., Vrana, B., Muir, D., Smedes, F., Sobotka, J., Zeng, E. Y., Bao, L.-J., Allan, I. J., Astrahan, P., Barra, R. O., Bidleman, T., Dykyi, E., Estoppey, N., Fillmann, G., Greenwood, N., Helm, P. A., Jantunen, L., Kaserzon, S., Macías, J. V., … Wong, C. S. (2023). Passive-Sampler-Derived PCB and OCP Concentrations in the Waters of the World─First Results from the AQUA-GAPS/MONET Network. Environmental Science & Technology, 57(25), 9342–9352. https://doi.org/10.1021/acs.est.3c01866
30. Lu, F., Jiang, Y., Wu, D., Zhou, J., Li, S., & Zhang, J. (2016). Levels and profiles of polychlorinated dibenzo-p-dioxin and dibenzofurans in raw and treated water from water treatment plants in Shenzhen, China. Environmental Pollution, 211, 233–240. https://doi.org/10.1016/j.envpol.2015.12.062
31. Muñoz-Arnanz, J., Roscales, J. L., Vicente, A., Ros, M., Barrios, L., Morales, L., Abad, E., & Jiménez, B. (2018). Assessment of POPs in air from Spain using passive sampling from 2008 to 2015. Part II: Spatial and temporal observations of PCDD/Fs and dl-PCBs. Science of The Total Environment, 634, 1669–1679. https://doi.org/10.1016/j.scitotenv.2018.04.164
32. Ngo, T. H., Tsou, H. H., Chen, Y. F., Chen, Y. W., & Chi, K. H. (2018). Sources identification of PCDD/Fs in soil and atmospheric deposition in Taiwan. Chemosphere, 208, 374–381. https://doi.org/10.1016/j.chemosphere.2018.05.195
33. Ngo, T. H., Yang, Y.-H., Chen, Y.-C., Pan, W. C., & Chi, K. H. (2020). Continuous nationwide atmospheric PCDD/F monitoring network in Taiwan (2006–2016): Variation in concentrations and apportionment of emission sources. Chemosphere, 255, 126979. https://doi.org/10.1016/j.chemosphere.2020.126979
34. Nieuwoudt, C., Quinn, L. P., Pieters, R., Jordaan, I., Visser, M., Kylin, H., Borgen, A. R., Giesy, J. P., & Bouwman, H. (2009). Dioxin-like chemicals in soil and sediment from residential and industrial areas in central South Africa. Chemosphere, 76(6), 774–783. https://doi.org/10.1016/j.chemosphere.2009.04.064
35. Rao, Q., Wang, X., Zhang, Q., Hoogenboom, R., Li, H., Deng, Z., Song, W., Cheng, L., Liu, X., Guan, S., Song, W., Yao, C., Chen, S., & Zhou, J. (2022). New insights into the transfer and accumulation of dioxins and dioxin-like PCBs in the food web of farmed Chinese mitten crabs: A typical case from the Yangtze River area. Journal of Hazardous Materials, 436, 129178. https://doi.org/10.1016/j.jhazmat.2022.129178
36. Song, S., Chen, K., Huang, T., Ma, J., Wang, J., Mao, X., Gao, H., Zhao, Y., & Zhou, Z. (2023). New emission inventory reveals termination of global dioxin declining trend. Journal of Hazardous Materials, 443, 130357. https://doi.org/10.1016/j.jhazmat.2022.130357
37. Taiwan EPA, (2013). Environmental Policy Monthly XVI:12
38. Tang, X., Zeng, B., Hashmi, M. Z., Long, D., Yu, B., Ullah, N., Shen, C., & Chen, Y. (2014). PBDEs and PCDD/Fs in surface soil taken from the Taizhou e-waste recycling area, China. Chemistry and Ecology, 30(3), 245–251. https://doi.org/10.1080/02757540.2013.844798
39. Thuan, N. T., Tsai, C. L., Weng, Y. M., Lee, T. Y., & Chang, M. B. (2011). Analysis of polychlorinated dibenzo-p-dioxins and furans in various aqueous samples in Taiwan. Chemosphere, 83(6), 760–766. https://doi.org/10.1016/j.chemosphere.2011.02.065
40. Tran, H. T., Lin, C., Hoang, H. G., Bui, X. T., Le, V. G., & Vu, C. T. (2022). Soil washing for the remediation of dioxin-contaminated soil: A review. Journal of Hazardous Materials, 421, 126767. https://doi.org/10.1016/j.jhazmat.2021.126767
41. Tran, H.-T., Hoang, H. G., Chacha, W. E., Mukherjee, S., Duong, T. V. H., Nguyen, N. S. H., Nguyen, K. N., & Naidu, R. (2024). A review of advanced bioremediation technologies for dioxin-contaminated soil treatment: Current and future outlook. Chemosphere, 366, 143400. https://doi.org/10.1016/j.chemosphere.2024.143400
42. USEPA, (2001a). Correcting the Henry’s Law Constant for Soil Temperature.
43. USEPA, (2001b). National Primary Drinking Water Standards.
44. van Drooge, B. L., Abalos, M., Abad, E., Adrados, M. A., Gomez, A., Gallés, P., & Grimalt, J. O. (2021). Qualitative and quantitative changes in traffic and waste incineration PCDD/Fs in urban air and soils under different seasonal conditions (Metropolitan Area of Barcelona). Science of The Total Environment, 753, 142149. https://doi.org/10.1016/j.scitotenv.2020.142149
45. Van den Berg, M., Birnbaum, L. S., Denison, M., De Vito, M., Farland, W., Feeley, M., Fiedler, H., Hakansson, H., Hanberg, A., Haws, L., Rose, M., Safe, S., Schrenk, D., Tohyama, C., Tritscher, A., Tuomisto, J., Tysklind, M., Walker, N., & Peterson, R. E. (2006). The 2005 World Health Organization Reevaluation of Human and Mammalian Toxic Equivalency Factors for Dioxins and Dioxin-Like Compounds. Toxicological Sciences, 93(2), 223–241. https://doi.org/10.1093/toxsci/kfl055
46. Vassura, I., Passarini, F., Ferroni, L., Bernardi, E., & Morselli, L. (2011). PCDD/Fs atmospheric deposition fluxes and soil contamination close to a municipal solid waste incinerator. Chemosphere, 83(10), 1366–1373. https://doi.org/10.1016/j.chemosphere.2011.02.072
47. Vernez, D., Oltramare, C., Sauvaget, B., Demougeot-Renard, H., Aicher, L., Roth, N., Rossi, I., Radaelli, A., Lerch, S., Marolf, V., & Berthet, A. (2023). Polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) soil contamination in Lausanne, Switzerland: Combining pollution mapping and human exposure assessment for targeted risk management. Environmental Pollution, 316, 120441. https://doi.org/10.1016/j.envpol.2022.120441
48. Wang, X., Rao, Q., Zhang, Q., Liu, C., Li, Y., Wang, D., Huang, D., Li, Y., Yao, C., & Song, W. (2024). Tissue distribution and exposure risk assessment of dioxins, dioxin-like polychlorinated biphenyls and perfluoroalkyl substances in red swamp crayfish. Food Control, 166, 110747. https://doi.org/10.1016/j.foodcont.2024.110747
49. Wu, J., Hu, J., Wang, S., Jin, J., Wang, R., Wang, Y., & Jin, J. (2018). Levels, sources, and potential human health risks of PCNs, PCDD/Fs, and PCBs in an industrial area of Shandong Province, China. Chemosphere, 199, 382–389. https://doi.org/10.1016/j.chemosphere.2018.02.039
50. Yu, J., Li, H., Liu, Y., & Wang, C. (2023). PCDD/Fs in indoor environments of residential communities around a municipal solid waste incineration plant in East China: Occurrence, sources, and cancer risks. Environment International, 174, 107902. https://doi.org/10.1016/j.envint.2023.107902
51. Yukhimets, A., Kuzu, S. L., Akyüz, E., & Saral, A. (2020). Investigation of geospatial distribution of PAH compounds in soil phase and determination of soil–air exchange direction in a megacity. Environmental Geochemistry and Health, 42(8), 2471–2484. https://doi.org/10.1007/s10653-019-00369-5
52. Zhang, Q., Gao, L., Zheng, M., Liu, L., & Li, C. (2014). Polychlorinated Dibenzo-p-dioxins (PCDDs) and Dibenzofurans (PCDFs) and Polychlorinated Biphenyls (PCBs) in Water Samples from the Middle Reaches of the Yangtze River, China. Bulletin of Environmental Contamination and Toxicology, 92(5), 585–589. https://doi.org/10.1007/s00128-013-1189-y