Assessing pollution and risk of polycyclic aromatic hydrocarbons in sewage sludge from wastewater treatment plants in China’s top coal-producing region
- 49 Downloads
Abstract
Managing and disposing of sewage sludge have been a severe environmental challenge around the world. China produces hundreds of million tons of sewage sludge annually, and a better understanding of the extent and risk of the associated pollution is of critical importance for implementing environmentally safe regulations and practices. The present study examined the quantity, composition, source, and risk of polycyclic aromatic hydrocarbons (PAHs) in sewage sludge from 18 wastewater treatment plants (WWTPs) in Shaanxi, one of China’s top coal-producing provinces. The total concentrations of 16 PAHs varied from 778 to 3264 ng/g dry weight, which is below the upper safety limit (5000 ng/g dry weight) set for the disposal of sludge from municipal wastewater treatment plants for agricultural use in China. However, the concentration of individual PAH compound exceeded the acceptable level prescribed by the Netherland Soil Standard. Three-ring PAHs were the most abundant constituent (50% of total PAHs on average), followed by four-ring PAHs averaging 25%. Relative to sludge PAHs in the same region a decade ago, the total concentrations decreased by more than 27% and the composition shifted to a more pronounced dominance by low molecular weight compounds. This compositional shift suggests higher contributions of petrogenic sources, which may reflect China’s increasing consumption of petroleum products over the past decade. The flux of sludge PAHs from each WWTP was positively correlated with the corresponding city’s GDP and population, and the total flux amounted to over 100 kg each year for WWTPs in the Xi’an city. The mean toxicity equivalent quantity (TEQ) value was more than twice higher than the value recommended by the Netherlands Soil Standard, and seven carcinogenic PAHs were the primary contributor (i.e., 89–99%) of the TEQ. Collectively, our findings demonstrate that sewage sludge PAHs in Shaanxi constitute a significant source of environmental pollution and toxicity, which cautions against the direct discharge and reuse of sewage sludge and further highlights challenges in managing and disposing of the vast quantities of sewage sludge in China.
Keywords
Polycyclic aromatic hydrocarbons Sewage sludge Wastewater treatment plant Toxic equivalent quantity Risk assessment Shaanxi Coal production Coal consumptionNotes
Funding information
The project was funded by Guangzhou University’s 2017 training program for young top-notch personnel (BJ201713), National Natural Science Foundation of China (Project No. 21477100), Strategic Research Grant (Grant No. 7004184), CityU Startup Grant (Grant No. 7200384), MFPRC Grant (Grant No. 9680132). Y. Lu acknowledges the support from Center for Freshwater Studies Faculty Research Grant from the University of Alabama, the Alabama Water Resources Research Institute Grant (2016–2017), and the 2018 Sabbatical Fellowship Program from the South University of Science and Technology in China.
Supplementary material
References
- Bai, Y., Zuo, W., Shao, H., Mei, L., Tang, B., Gu, C., Wang, X., & Guan, Y. (2018). Eastern China coastal mudflats: Salt-soil amendment with sewage slude. Land Degradation & Development, 29 (10) https://doi.org/10.1002/ldr.3092
- Balcioglu, E. B., Aksu, A., Balkis, N., & Ozturk, B. (2014). T-PAH contamination in Mediterranean mussels (Mytilus galloprovincialis, Lamarck, 1819) at various stations of the Turkish Straits System. Marine Pollution Bulletin, 88(1–2), 344–346. https://doi.org/10.1016/j.marpolbul.2014.08.034.CrossRefGoogle Scholar
- Bhuiyan, M. A. H., Parvez, L., Islam, M. A., Dampare, S. B., Suzuki, S. (2010) Heavy metal pollution of coalmine-affected agriculutral soils in the northern part of Bangladesh. Journal of Hazardous Materials, 173 (1–3), 384–392. Google Scholar
- Blanchard, M., Teil, M. J., Ollivon, D., Legenti, L., & Chevreuil, M. (2004). Polycyclic aromatic hydrocarbons and polychlorobiphenyls in wastewaters and sewage sludges from the Paris area (France). Environmental Research, 95(2), 184–197. https://doi.org/10.1016/j.envres.2003.07.003.CrossRefGoogle Scholar
- Bortey-Sam, N., Ikenaka, Y., Nakayama, S. M., Akoto, O., Yohannes, Y. B., Baidoo, E., et al. (2014). Occurrence, distribution, sources and toxic potential of polycyclic aromatic hydrocarbons (PAHs) in surface soils from the Kumasi Metropolis, Ghana. Science of the Total Environment, 496, 471–478. https://doi.org/10.1016/j.scitotenv.2014.07.071.CrossRefGoogle Scholar
- Cai, Q.-Y., Mo, C.-H., Wu, Q.-T., Zeng, Q.-Y., & Katsoyiannis, A. (2007). Occurrence of organic contaminants in sewage sludges from eleven wastewater treatment plants, China. Chemosphere, 68(9), 1751–1762. https://doi.org/10.1016/j.chemosphere.2007.03.041.CrossRefGoogle Scholar
- European Union Commission (2013). Directive 2013/39/EU of the European Parliament and of the Council amending Directives 2000/60/EC and 2008/105/EC as regards priority substances in the field of water policy. Official Journal of the European Union https://eur-lex.europa.eu/LexUriServ/LexUriServ.do?uri=OJ:L:2013:226:0001:0017:EN:PDF. Accessed 15 Oct 2017.
- Dai, J., Xu, M., Chen, J., Yang, X., & Ke, Z. (2007). PCDD/F, PAH and heavy metals in the sewage sludge from six wastewater treatment plants in Beijing, China. Chemosphere, 66(2), 353–361. https://doi.org/10.1016/j.chemosphere.2006.04.072.CrossRefGoogle Scholar
- Feng, Y., Zhang, Y., Quan, X., & Chen, S. (2014). Enhanced anaerobic digestion of waste activated sludge digestion by the addition of zero valent iron. Water Research, 52(Supplement C), 242–250. https://doi.org/10.1016/j.watres.2013.10.072.CrossRefGoogle Scholar
- Feng, L., Luo, J., & Chen, Y. (2015). Dilemma of sewage sludge treatment and disposal in China. Environmental Science & Technology, 49(8), 4781–4782. https://doi.org/10.1021/acs.est.5b01455.CrossRefGoogle Scholar
- He, Q.-S., Zhang, L., Cui, Y., Cheng, M.-c., Guo, L.-l., Liu, M., & Chen, L.-g. C. (2017). Particle dry deposition of polycyclic aromatic hydrocarbons and its risk assessment in a typical coal-polluted and basin city, northern China. Atmospheric Pollution Research, 8, 1081–1089. https://doi.org/10.1016/j.apr.2017.04.008.CrossRefGoogle Scholar
- Hu, Y., Li, G., Yan, M., Ping, C., & Ren, J. (2014). Investigation into the distribution of polycyclic aromatic hydrocarbons (PAHs) in wastewater sewage sludge and its resulting pyrolysis bio-oils. The Science of the Total Environment, 473, 459–464. https://doi.org/10.1016/j.scitotenv.2013.12.051. CrossRefGoogle Scholar
- Katsoyiannis, A., Terzi, E., & Cai, Q. Y. (2007). On the use of PAH molecular diagnostic ratios in sewage sludge for the understanding of the PAH sources. Is this use appropriate? Chemosphere, 69(8), 1337–1339. https://doi.org/10.1016/j.chemosphere.2007.05.084.CrossRefGoogle Scholar
- Khadhar, S., Higashi, T., Hamdi, H., Matsuyama, S., & Charef, A. (2010). Distribution of 16 EPA-priority polycyclic aromatic hydrocarbons (PAHs) in sludges collected from nine Tunisian wastewater treatment plants. Journal of Hazardous Materials, 183(1–3), 98–102. https://doi.org/10.1016/j.jhazmat.2010.06.112.CrossRefGoogle Scholar
- Li, J., Dong, H., Zhang, D., Han, B., Zhu, C., Liu, S., Liu, X., Ma, Q., & Li, X. (2015). Sources and ecological risk assessment of pahs in surface sediments from bohai sea and northern part of the yellow sea, China. Marine Pollution Bulletin, 96(1–2), 485–490. https://doi.org/10.1016/j.marpolbul.2015.05.002.CrossRefGoogle Scholar
- Lin, M., Ning, X.-A., An, T., Zhang, J., Chen, C., Ke, Y., et al. (2016). Degradation of polycyclic aromatic hydrocarbons (PAHs) in textile dyeing sludge with ultrasound and Fenton processes: effect of system parameters and synergistic effect study. Journal of Hazardous Materials, 307, 7–16. https://doi.org/10.1016/j.jhazmat.2015.12.047.CrossRefGoogle Scholar
- Man, Y. B., Chow, K. L., Cheng, Z., Mo, W. Y., Chan, Y. H., Lam, J. C. W., Lau, F. T. K., Fung, W. C., & Wong, M. H. (2016). Profiles and removal efficiency of polycyclic aromatic hydrocarbons by two different types of sewage treatment plants in Hong Kong. Jounral of Environmental Sciences, 53, 196–206. https://doi.org/10.1016/j.jes.2016.04.020.
- Manoli, E., & Samara, C. (1999). Occurrence and mass balance of polycyclic aromatic hydrocarbons in the Thessaloniki sewage treatment plant. Journal of Environmental Quality, 28, 176–187. https://doi.org/10.2134/jeq1999.00472425002800010021x.CrossRefGoogle Scholar
- Melnyk, A., Dettlaff, A., Kuklinska, K., Namiesnik, J., & Wolska, L. (2015). Concentration and sources of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) in surface soil near a municipal solid waste (MSW) landfill. Sci Total Environ, 530-531, 18–27. https://doi.org/10.1016/j.scitotenv.2015.05.092.CrossRefGoogle Scholar
- Meng, X. Z., Venkatesan, A. K., Ni, Y. L., Steele, J. C., Wu, L. L., Bignert, A., Bergman, Å., & Halden, R. U. (2016). Organic contaminants in Chinese sewage sludge: a meta-analysis of the literature of the past 30 years. Environmental Science & Technology, 50(11), 5454–5466. https://doi.org/10.1021/acs.est.5b05583.CrossRefGoogle Scholar
- Ministry of Housing and Urban-Rural Development. (2009). Disposal of sludge from municipal wastewater treatment plant—control standards for agricultural use (CJ/T 309-2009). Beijing: Standards Press of China.Google Scholar
- Ministry of Housing Spatial Planning and Environment. (1994). Environmental quality objectives in the Netherlands: a review of environmental quality objectives and their policy framework in the Netherlands. Hague, Netherlands: Ministry of Housing, Spatial Planning and Environment.Google Scholar
- Mori, J., Sæbø, A., Hanslin, H. M., Teani, A., Ferrini, F., Fini, A., & Burchi, G. (2015). Deposition of traffic-related air pollutants on leaves of six evergreen shrub species during a Mediterranean summer season. Urban Forestry & Urban Greening, 14(2), 264–273. https://doi.org/10.1016/j.ufug.2015.02.008.CrossRefGoogle Scholar
- National Bureau of Statistics of China. (2017). Energy Production in 2016. http://www.stats.gov.cn/tjsj/zxfb/201702/t20170228_1467575.html. Accessed 15 Oct 2017.
- Nguyen, T. C., Loganathan, P., Nguyen, T. V., Vigneswaran, S., Kandasamy, J., Slee, D., Stevenson, G., & Naidu, R. (2014). Polycyclic aromatic hydrocarbons in road-deposited sediments, water sediments, and soils in Sydney, Australia: comparisons of concentration distribution, sources and potential toxicity. Ecotoxicology and Environmental Safety, 104, 339–348. https://doi.org/10.1016/j.ecoenv.2014.03.010.CrossRefGoogle Scholar
- Ning, X.-A., Lin, M.-Q., Shen, L.-Z., Zhang, J.-H., Wang, J.-Y., Wang, Y.-J., Yang, Z. Y., & Liu, J. Y. (2014). Levels, composition profiles and risk assessment of polycyclic aromatic hydrocarbons (PAHs) in sludge from ten textile dyeing plants. Environmental Research, 132, 112–118. https://doi.org/10.1016/j.envres.2014.03.041.CrossRefGoogle Scholar
- Oh, J.-Y., Choi, S.-D., Kwon, H.-O., & Lee, S.-E. (2016). Leaching of polycyclic aromatic hydrocarbons (PAHs) from industrial wastewater sludge by ultrasonic treatment. Ultrasonics Sonochemistry, 33, 61–66. https://doi.org/10.1016/j.ultsonch.2016.04.027.CrossRefGoogle Scholar
- Ouyang, Z.-Z., Gao, L.-M., & Yang, C. (2018). Distribution, sources and influence factors of polycyclic aromatic hydrocarbon at different depths of the soil and sediments of two typical coal mining subsidence areas in Huainan, China. Ecotoxicology and Environmental Safety, 163, 255–265. https://doi.org/10.1016/j.ecoenv.2018.07.024.CrossRefGoogle Scholar
- Ozaki, N., Takamura, Y., Kojima, K., & Kindaichi, T. (2015). Loading and removal of PAHs in a wastewater treatment plant in a separated sewer system. Water Research, 80, 337–345. https://doi.org/10.1016/j.watres.2015.05.002.CrossRefGoogle Scholar
- Ozcan, S., Tor, A., & Aydin, M. E. (2013). Investigation on the levels of heavy metals, polycyclic aromatic hydrocarbons, and polychlorinated biphenyls in sewage sludge samples and ecotoxicological testing. Clean- Soil Air Water, 41(4), 411–418. https://doi.org/10.1002/clen.201100187.
- Pérez, S., Farré, M. L., Garcia, M. J., & Barceló, D. (2001a). Occurrence of polycyclic aromatic hydrocarbons in sewage sludge and their contribution to its toxicity in the ToxAlert® 100 bioassay. Chemosphere, 45(6), 705–712. https://doi.org/10.1016/S0045-6535(01)00152-7.
- Pérez, S., Guillamón, M., Barceló, D., Pérez, S., Farré, M. L., Garcia, M. J., et al. (2001b). Quantitative analysis of polycyclic aromatic hydrocarbons in sewage sludge from wastewater treatment plants. Journal of Chromatography A, 938(1), 57–65. https://doi.org/10.1016/S0021-9673(01)01338-3.CrossRefGoogle Scholar
- Poluszyńska, J., Jarosz-Krzemińska, E., & Helios-Rybicka, E. (2017). Studying the effects of two various methods of composting on the degradation levels of polycyclic aromatic hydrocarbons (PAHs) in sewage sludge. Water, Air, and Soil Pollution, 228(8), 305. https://doi.org/10.1007/s11270-017-3481-7. CrossRefGoogle Scholar
- Qiao, M., Wang, C., Huang, S., Wang, D., & Wang, Z. (2006). Composition, sources, and potential toxicological significance of pahs in the surface sediments of the meiliang bay, Taihu lake, China. Environment International, 32(1), 28–33. https://doi.org/10.1016/j.envint.2005.04.005.CrossRefGoogle Scholar
- Schwarzenbach, R. P., Gschwend, P. M., & Imboden, D. M. (2003). Environmental organic chemistry (2nd ed.). Hoboken, NJ, USA: John Wiley & Sons.Google Scholar
- Talalaj, I. A. (2014). Assessment of groundwater quality near the landfill site using the modified water quality index. Environmental Monitoring and Assessment, 186(6), 3673–3683. https://doi.org/10.1007/s10661-014-3649-1.CrossRefGoogle Scholar
- Tao, Y., Yu, J., Xue, B., Yao, S., & Wang, S. (2017). Precipitation and temperature drive seasonal variation in bioaccumulation of polycyclic aromatic hydrocarbons in the planktonic food webs of a subtropical shallow eutrophic lake in China. Sci Total Environ, 583, 447–457. https://doi.org/10.1016/j.scitotenv.2017.01.100.CrossRefGoogle Scholar
- Tiwary, R. K. (2001). Environmental impact of coal mining on water regime and its management. Water Air and Soil pollution, 132(1–2), 185–199. https://doi.org/10.1023/A:1012083519667.CrossRefGoogle Scholar
- Torretta, V., & Katsoyiannis, A. (2013). Occurrence of polycyclic aromatic hydrocarbons in sludges from different stages of a wastewater treatment plant in Italy. Environmental Technology, 34(7), 937–943. https://doi.org/10.1080/09593330.2012.722693/Taylor&Francis. CrossRefGoogle Scholar
- Tsai, P.-J., Shih, T.-S., Chen, H.-L., Lee, W.-J., Lai, C.-H., & Liou, S.-H. (2004). Assessing and predicting the exposures of polycyclic aromatic hydrocarbons (PAHs) and their carcinogenic potencies from vehicle engine exhausts to highway toll station workers. Atmospheric Environment, 38(2), 333–343. https://doi.org/10.1016/j.atmosenv.2003.08.038.CrossRefGoogle Scholar
- US Environmental Protection Agency (2016). Regional Screening Levels (Formerly HHMSSL - Human Health Medium-Specific Screening Levels). https://www.epa.gov/risk/regional-screening-levels-rsls-generic-tables-may-2016. Accessed March 20, 2017.
- Wang, X.-T., Hu, B.-P., Cheng, H.-X., Jia, H.-H., & Zhou, Y. (2017). Spatial variations, source apportionment and potential ecological risks of polycyclic aromatic hydrocarbons and synthetic musks in river sediments in Shanghai, China. Chemosphere, 193, 108–117. https://doi.org/10.1016/j.chemosphere.2017.10.145.CrossRefGoogle Scholar
- Wlodarczyk-Makula, M. (2005). The loads of pahs in wastewater and sewage sludge of municipal treatment plant. Polycyclic Aromatic Compounds, 25(2), 183–194. https://doi.org/10.1080/10406630590930743.CrossRefGoogle Scholar
- Wu, Y., Luo, Y., Zou, D., Ni, J., Liu, W., Teng, Y., & Li, Z. (2008). Bioremediation of polycyclic aromatic hydrocarbons contaminated soil with Monilinia sp.: degradation and microbial community analysis. Biodegradation, 19(2), 247–257. https://doi.org/10.1007/s10532-007-9131-9.CrossRefGoogle Scholar
- Wu, Q., Leung, J. Y., Tam, N. F., Chen, S., Mai, B., Zhou, X., et al. (2014). Biological risk and pollution history of polycyclic aromatic hydrocarbons (PAHs) in Nansha mangrove, South China. Marine Pollution Bulletin, 85(1), 92–98. https://doi.org/10.1016/j.marpolbul.2014.06.014.CrossRefGoogle Scholar
- Wu, S., Liu, X., Liu, M., Chen, X., Liu, S., et al. (2018). Sources, influencing factors and environmental indications of PAH pollution in urban soil columns of Shanghai, China. Ecological Indicators, 85, 1170–1180. https://doi.org/10.1016/j.ecolind.2017.11.067.CrossRefGoogle Scholar
- Xu, S., Liu, W., & Tao, S. (2006). Emission of polycyclic aromatic hydrocarbons in China. Environmental Science & Technology, 40(3), 702–708. https://doi.org/10.1021/es0517062.CrossRefGoogle Scholar
- 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. Organic Geochemistry, 33(4), 489–515. https://doi.org/10.1016/s0146-6380(02)00002-5.CrossRefGoogle Scholar
- Zakaria, M., Hiaw Geik, K., Yoon Lee, W., & Hayet, R. (2005). Landfill leachate as a source of polycyclic aromatic hydrocarbons (PAHs) to Malaysian waters (Vol. 29(2)).Google Scholar
- Zeng, X., Lin, Z., Gui, H., Shao, W., Sheng, G., Fu, J., & Yu, Z. (2010). Occurrence and distribution of polycyclic aromatic carbons in sludges from wastewater treatment plants in Guangdong, China. Environmental Monitoring and Assessment, 169(1–4), 89–100. https://doi.org/10.1007/s10661-009-1153-9.CrossRefGoogle Scholar
- Zhang, L., Dong, L., Ren, L., Shi, S., Zhou, L., Zhang, T., & Huang, Y. (2012a). Concentration and source identification of polycyclic aromatic hydrocarbons and phthalic acid esters in the surface water of the Yangtze River Delta, China. [Journal Article; Research Support, Non-U.S. Gov't]. J Environ Sci (China), 24(2), 335–342. https://doi.org/10.1016/s1001-0742(11)60782-1.CrossRefGoogle Scholar
- Zhang, W., Wei, C., Chai, X., He, J., Cai, Y., Ren, M., Yan, B., Peng, P., & Fu, J. (2012b). The behaviors and fate of polycyclic aromatic hydrocarbons (PAHs) in a coking wastewater treatment plant. Chemosphere, 88(2), 174–182. https://doi.org/10.1016/j.chemosphere.2012.02.076.CrossRefGoogle Scholar
- Zhang, W., Wei, C., Feng, C., Yan, B., Li, N., Peng, P., & Fu, J. (2012c). Coking wastewater treatment plant as a source of polycyclic aromatic hydrocarbons (PAHs) to the atmosphere and health-risk assessment for workers. Science of the Total Environment, 432, 396–403. https://doi.org/10.1016/j.scitotenv.2012.06.010.CrossRefGoogle Scholar
- Zhang, Y., Nie, R., Shi, R., & Zhang, M. (2016). Measuring the capacity utilization of the coal sector and its decoupling with economic growth in China’s supply-side reform. Resources, Conservation and Recycling, 129, 314–325. https://doi.org/10.1016/j.resconrec.2016.09.022.CrossRefGoogle Scholar
- Zheng, B., Wang, L., Lei, K., & Nan, B. (2016). Distribution and ecological risk assessment of polycyclic aromatic hydrocarbons in water, suspended particulate matter and sediment from Daliao River estuary and the adjacent area, China. Chemosphere, 149, 91–100. https://doi.org/10.1016/j.chemosphere.2016.01.039.CrossRefGoogle Scholar
- Zhou, W., Fu, D., & Sun, Z. (1991). Determination of black list of China’s priority pollutants in water. Research of Environmental Sciences, 4(6), 9–12. https://doi.org/10.13198/j.res.1991.06.11.zhouwm.002. CrossRefGoogle Scholar
- Zhu, Y., Tao, S., Sun, J. T., Wang, X. L., Li, X. D., Tsang, D. C. W., Zhu, L. Z., Shen, G. F., Huang, H. J., Cai, C. Y., & Liu, W. X. (2019). Multimedia modeling of the PAH concentration and distribution in the Yangtze River Delta and human health risk assessment. Science of the Total Environment, 647, 962–972. https://doi.org/10.1016/j.scitotenv.2018.08.075.CrossRefGoogle Scholar