Pesticides in the typical agricultural groundwater in Songnen plain, northeast China: occurrence, spatial distribution and health risks

Huang, Fuyang; Li, Zeyan; Zhang, Chong; Habumugisha, Théogène; Liu, Fei; Luo, Ximing

doi:10.1007/s10653-019-00331-5

Original Paper
Published: 25 May 2019

Pesticides in the typical agricultural groundwater in Songnen plain, northeast China: occurrence, spatial distribution and health risks

Fuyang Huang^1,2,
Zeyan Li^1,2,
Chong Zhang^1,2,
Théogène Habumugisha^1,2,
Fei Liu^1,2 &
Ximing Luo³

Environmental Geochemistry and Health volume 41, pages 2681–2695 (2019)Cite this article

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Abstract

Songnen plain is an important commodity grain base of China, and this is the first study on the comprehensive detection of multiple pesticides in groundwater. Based on an analytical method of 56 pesticides, 30 groundwater samples were collected and analyzed. At least 4 pesticides were detected in each sample and 32 out of 56 pesticides were detected. The average detected levels of individual pesticides were approximately 10–100 ng/L. Organophosphorus pesticides and carbamate pesticides were the dominant pesticides, and their percentage of total pesticide concentrations were 35.9% and 55.5%, respectively. Based on the spatial distribution, the characteristic of nonpoint source pollution was indicated in the whole study area except for a point source pollution with the influence of a sewage oxidation pond. Nine core pesticides and three distinct clusters of the core pesticides with various concentration patterns were revealed by cluster analysis. Linear regression identified a significant relationship between the cumulative detections and the cumulative concentrations, providing access to identify the outlying contaminant events that deviate substantially from the linear trend. A new insight for prediction of pesticide occurrence was provided by the Pearson correlation between some individual pesticide concentrations and the cumulative detections or the cumulative concentrations. According to health risk assessment, the residual pesticides posed medium risks for children and infants and approximately 90% of risks were composed of β-HCH, dimethoate, ethyl-p-nitrophenyl phenylphosphonothioate and methyl parathion. These findings contributed to establishing a database for future monitoring and control of pesticides in agricultural areas.

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References

Affum, A. O., Acquaah, S. O., Osae, S. D., & Kwaansa-Ansah, E. E. (2018). Distribution and risk assessment of banned and other current-use pesticides in surface and groundwaters consumed in an agricultural catchment dominated by cocoa crops in the Ankobra Basin, Ghana. Science of the Total Environment,633, 630–640. https://doi.org/10.1016/j.scitotenv.2018.03.129.
CAS Article Google Scholar
Alam, M. J., Yuan, D., Yong Jun, J., Sun, Y., Li, Y., & Xu, X. (2014). Sources and transports of organochlorine pesticides in the Nanshan underground river, China. Environmental Earth Sciences,71(4), 1977–1987. https://doi.org/10.1007/s12665-013-2919-5.
CAS Article Google Scholar
Bai, Y., Ruan, X., & van der Hoek, J. P. (2018). Residues of organochlorine pesticides (OCPs) in aquatic environment and risk assessment along Shaying River, China. Environmental Geochemistry and Health,40(6), 2525–2538. https://doi.org/10.1007/s10653-018-0117-9.
CAS Article Google Scholar
Bi, E., Liu, Y., He, J., Wang, Z., & Liu, F. (2012). Screening of emerging volatile organic contaminants in shallow groundwater in east China. Ground Water Monitoring and Remediation,32(1), 53–58. https://doi.org/10.1111/j.1745-6592.2011.01362.x.
CAS Article Google Scholar
Bradley, P. M., Journey, C. A., Romanok, K. M., Barber, L. B., Buxton, H. T., Foreman, W. T., et al. (2017). Expanded target-chemical analysis reveals extensive mixed organic-contaminant exposure in US streams. Environmental Science and Technology,51(9), 4792–4802. https://doi.org/10.1021/acs.est.7b00012.
CAS Article Google Scholar
Carpenter, C. M. G., & Helbling, D. E. (2018). Widespread micropollutant monitoring in the hudson river estuary reveals spatiotemporal micropollutant clusters and their sources. Environmental Science and Technology,52(11), 6187–6196. https://doi.org/10.1021/acs.est.8b00945.
CAS Article Google Scholar
Castro-Gutierrez, V., Masis-Mora, M., Diez, M. C., Tortella, G. R., & Rodriguez-Rodriguez, C. E. (2017). Aging of biomixtures: Effects on carbofuran removal and microbial community structure. Chemosphere,168, 418–425. https://doi.org/10.1016/j.chemosphere.2016.10.065.
CAS Article Google Scholar
Chen, L., Jin, S., Liu, Y., & Liu, F. (2014). Presence of Semi-Volatile Organic Contaminants in Shallow Groundwater of Selected Regions in China. Ground Water Monitoring and Remediation,34(4), 33–43. https://doi.org/10.1111/gwmr.12078.
CAS Article Google Scholar
Chen, L., Lang, H., Liu, F., Jin, S., & Yan, T. (2018). Presence of antibiotics in shallow groundwater in the Northern and Southwestern Regions of China. Groundwater,56(3), 451–457. https://doi.org/10.1111/gwat.12596.
CAS Article Google Scholar
China Geological Survey (CGS). (2008). Guideline for Geological Survey and Assessment on Groundwater Contamination. Beijing: China Geological Survey.
Google Scholar
Chowdhury, A. Z., Jahan, S. A., Islam, M. N., Moniruzzaman, M., Alam, M. K., Zaman, M. A., et al. (2012). Occurrence of organophosphorus and carbamate pesticide residues in surface water samples from the Rangpur District of Bangladesh. Bulletin of Environmental Contamination and Toxicology,89(1), 202–207. https://doi.org/10.1007/s00128-012-0641-8.
CAS Article Google Scholar
Close, M. E., & Skinner, A. (2012). Sixth national survey of pesticides in groundwater in New Zealand. New Zealand Journal of Marine and Freshwater Research,46(4), 443–457. https://doi.org/10.1080/00288330.2012.707131.
CAS Article Google Scholar
ECCAY (Editorial Committee of China Agriculture Yearbook). (2011). China agriculture year book. Beijing: Agriculture Press of China.
Google Scholar
El Alfy, M., & Faraj, T. (2017). Spatial distribution and health risk assessment for groundwater contamination from intensive pesticide use in arid areas. Environmental Geochemistry and Health,39(1), 231–253. https://doi.org/10.1007/s10653-016-9825-1.
CAS Article Google Scholar
Grung, M., Lin, Y., Zhang, H., Steen, A. O., Huang, J., Zhang, G., et al. (2015). Pesticide levels and environmental risk in aquatic environments in China—A review. Environment International,81, 87–97. https://doi.org/10.1016/j.envint.2015.04.013.
CAS Article Google Scholar
Hao, F., Chen, S., Ouyang, W., Shan, Y., & Qi, S. (2013). Temporal rainfall patterns with water partitioning impacts on maize yield in a freezee–thaw zone. Journal of Hydrology,486(12), 412–419. https://doi.org/10.1016/j.jhydrol.2013.02.008.
Article Google Scholar
Hu, Y., Qi, S., Yuan, L., Liu, H., & Xing, X. (2018). Assessment of organochlorine pesticide contamination in waterbirds from an agricultural region, Central China. Environmental Geochemistry and Health,40(1), 175–187. https://doi.org/10.1007/s10653-016-9891-4.
CAS Article Google Scholar
Hu, Y., Qi, S., Zhang, J., Tan, L., Zhang, J., Wang, Y., et al. (2011). Assessment of organochlorine pesticides contamination in underground rivers in Chongqing, Southwest China. Journal of Geochemical Exploration,111(1–2), 47–55. https://doi.org/10.1016/j.gexplo.2011.07.006.
CAS Article Google Scholar
Hu, L., Zhang, G., Zheng, B., Qin, Y., Lin, T., & Guo, Z. (2009). Occurrence and distribution of organochlorine pesticides (OCPs) in surface sediments of the Bohai Sea. China. Chemosphere,77(5), 663–672. https://doi.org/10.1016/j.chemosphere.2009.07.070.
CAS Article Google Scholar
Hu, J., Zhu, T., & Li, Q. (2007). Chapter 3 organochlorine pesticides in China. Developments in Environmental Science,7, 159–211. https://doi.org/10.1016/S1474-8177(07)07003-9.
CAS Article Google Scholar
Huang, F., Zou, S., Deng, D., Lang, H., & Liu, F. (2019). Antibiotics in a typical karst river system in China: Spatiotemporal variation and environmental risks. Science of the Total Environment,650, 1348–1355. https://doi.org/10.1016/j.scitotenv.2018.09.131.
CAS Article Google Scholar
Jacobsen-Pereira, C. H., dos Santos, C. R., Maraslis, F. T., Pimentel, L., Lobo Feijo, A. J., Silva, C. I., et al. (2018). Markers of genotoxicity and oxidative stress in farmers exposed to pesticides. Ecotoxicology and Environmental Safety,148, 177–183. https://doi.org/10.1016/j.ecoenv.2017.10.004.
CAS Article Google Scholar
Köck-Schulmeyer, M., Villagrasa, M., Lopez de Alda, M., Cespedes-Sanchez, R., Ventura, F., & Barcelo, D. (2013). Occurrence and behavior of pesticides in wastewater treatment plants and their environmental impact. Science of the Total Environment,458, 466–476. https://doi.org/10.1016/j.scitotenv.2013.04.010.
CAS Article Google Scholar
Li, J., Zhang, G., Guo, L., Xu, W., Li, X., Lee, C. S. L., et al. (2007). Organochlorine pesticides in the atmosphere of Guangzhou and Hong Kong: Regional sources and long-range atmospheric transport. Atmospheric Environment,41(18), 3889–3903. https://doi.org/10.1016/j.atmosenv.2006.12.052.
CAS Article Google Scholar
Lin, Y., Yang, J., & Ye, Y. (2018). Spatial-temporal analysis of the relationships between agricultural production and use of agrochemicals in Eastern China and related environmental and political implications (Based on Decoupling Approach and LMDI Decomposition Analysis). Sustainability,10(4), 917. https://doi.org/10.3390/su10040917.
Article Google Scholar
Liu, B., Chen, L., Huang, L., Wang, Y., & Li, Y. (2015). Distribution of volatile organic compounds (VOCs) in surface water, soil, and groundwater within a chemical industry park in Eastern China. Water Science and Technology,71(2), 259–267. https://doi.org/10.2166/wst.2014.499.
CAS Article Google Scholar
Liu, B., Li, Y., Ma, J., Huang, L., & Chen, L. (2016). Detection of semi-volatile organic compounds (SVOCs) in surface water, soil, and groundwater in a chemical industrial park in Eastern China. Water Science and Technology,73(5), 1175–1189. https://doi.org/10.2166/wst.2015.586.
CAS Article Google Scholar
Liu, X., Zhang, G., Li, J., Yu, L., Xu, Y., Li, X., et al. (2009). Seasonal Patterns and Current Sources of DDTs, Chlordanes, Hexachlorobenzene, and Endosulfan in the Atmosphere of 37 Chinese Cities. Environmental Science and Technology,43(5), 1316–1321. https://doi.org/10.1021/es802371n.
CAS Article Google Scholar
Margot, J., Kienle, C., Magnet, A., Weil, M., Rossi, L., de Alencastro, L. F., et al. (2013). Treatment of micropollutants in municipal wastewater: Ozone or powdered activated carbon? Science of the Total Environment,461, 480–498. https://doi.org/10.1016/j.scitotenv.2013.05.034.
CAS Article Google Scholar
Massei, R., Busch, W., Wolschke, H., Schinkel, L., Bitsch, M., Schulze, T., et al. (2018). Screening of pesticide and biocide patterns as risk drivers in sediments of major european river mouths: Ubiquitous or river basin-specific contamination? Environmental Science and Technology,52(4), 2251–2260. https://doi.org/10.1021/acs.est.7b04355.
CAS Article Google Scholar
Münze, R., Hannemann, C., Orlinskiy, P., Gunold, R., Paschke, A., Foit, K., et al. (2017). Pesticides from wastewater treatment plant effluents affect invertebrate communities. Science of the Total Environment,599, 387–399. https://doi.org/10.1016/j.scitotenv.2017.03.008.
CAS Article Google Scholar
NBSC (National Bureau of Statistics of China). (2015). China Statistical Yearbook. China Statistical Press, Beijing, http://www.stats.gov.cn/tjsj/ndsj/2015/indexeh.htm.
Ouyang, W., Cai, G., Huang, W., & Hao, F. (2016). Temporal-spatial loss of diffuse pesticide and potential risks for water quality in China. Science of the Total Environment,541, 551–558. https://doi.org/10.1016/j.scitotenv.2015.09.120.
CAS Article Google Scholar
Ouyang, W., Cai, G., Tysklind, M., Yang, W., Hao, F., & Liu, H. (2017). Temporal-spatial patterns of three types of pesticide loadings in a middle-high latitude agricultural watershed. Water Research,122, 377–386. https://doi.org/10.1016/j.watres.2017.06.023.
CAS Article Google Scholar
Palma, P., Köck-Schulmeyer, M., Alvarenga, P., Ledo, L., Barbosa, I. R., López de Alda, M., et al. (2014). Risk assessment of pesticides detected in surface water of the Alqueva reservoir (Guadiana basin, southern of Portugal). Science of the Total Environment,488, 208–219. https://doi.org/10.1016/j.scitotenv.2014.04.088.
CAS Article Google Scholar
Pan, H., Lei, H., He, X., Xi, B., Han, Y., & Xu, Q. (2017a). Levels and distributions of organochlorine pesticides in the soil-groundwater system of vegetable planting area in Tianjin City, Northern China. Environmental Geochemistry and Health,39(2), 417–429. https://doi.org/10.1007/s10653-016-9899-9.
CAS Article Google Scholar
Pan, H., Lei, H., He, X., Xi, B., & Xu, Q. (2017b). Spatial distribution of organochlorine and organophosphorus pesticides in soil-groundwater systems and their associated risks in the middle reaches of the Yangtze River Basin. Environmental Geochemistry and Health. https://doi.org/10.1007/s10653-017-9970-1.
Article Google Scholar
Rani, M., Shanker, U., & Jassal, V. (2017). Recent strategies for removal and degradation of persistent & toxic organochlorine pesticides using nanoparticles: A review. Journal of Environmental Management,190, 208–222. https://doi.org/10.1016/j.jenvman.2016.12.068.
CAS Article Google Scholar
Singh, S., Kumar, V., Thakur, S., Banerjee, B. D., Chandna, S., Rautela, R. S., et al. (2011). DNA damage and cholinesterase activity in occupational workers exposed to pesticides. Environmental Toxicology and Pharmacology,31(2), 278–285. https://doi.org/10.1016/j.etap.2010.11.005.
CAS Article Google Scholar
Steingrímsdóttir, M. M., Petersen, A., & Fantke, P. (2018). A screening framework for pesticide substitution in agriculture. Journal of Cleaner Production,192, 306–315. https://doi.org/10.1016/j.jclepro.2018.04.266.
CAS Article Google Scholar
Sun, S., Chen, Y., Lin, Y., & An, D. (2018). Occurrence, spatial distribution, and seasonal variation of emerging trace organic pollutants in source water for Shanghai, China. Science of the Total Environment,639, 1–7. https://doi.org/10.1016/j.scitotenv.2018.05.089.
CAS Article Google Scholar
Thomatou, A.-A., Zacharias, I., Hela, D., & Konstantinou, I. (2013). Determination and risk assessment of pesticide residues in lake Amvrakia (W. Greece) after agricultural land use changes in the lake’s drainage basin. International Journal of Environmental Analytical Chemistry,93(7), 780–799. https://doi.org/10.1080/03067319.2012.656099.
CAS Article Google Scholar
Toccalino, P. L., Gilliom, R. J., Lindsey, B. D., & Rupert, M. G. (2014). Pesticides in groundwater of the United States: Decadal-scale changes, 1993–2011. Groundwater,52, 112–125. https://doi.org/10.1111/gwat.12176.
CAS Article Google Scholar
U.S. EPA. (2017). U.S. Environmental Protection Agency: Human Health Benchmarks for Pesticides: Updated 2017 Technical Document. https://www.epa.gov/dwstandardsregulations/human-health-benchmarks-pesticides-drinking-water.
Wang, Y., Guo, S., Xu, Y., Wang, W., Qi, S., Xing, X., et al. (2012). The concentration and distribution of organochlorine pesticides in the air from the karst cave, South China. Environmental Geochemistry and Health,34(4), 493–502. https://doi.org/10.1007/s10653-011-9441-z.
CAS Article Google Scholar
Wang, Y., Xu, Y., Qi, S., Li, X., Kong, X., Yuan, D., et al. (2013). Distribution and potential sources of organochlorine pesticides in the karst soils of a tiankeng in southwest China. Environmental Earth Sciences,70(6), 2873–2881. https://doi.org/10.1007/s12665-013-2349-4.
CAS Article Google Scholar
WHO. (2008). Guidelines for drinking water quality (Health Criteria and Other Supporting Information 4th ed., Vol. 2). World Health Organization, Geneva, WHO Library Cataloguing-in-Publication Data.
Wu, C., Luo, Y., Gui, T., & Huang, Y. (2014). Concentrations and potential health hazards of organochlorine pesticides in (shallow) groundwater of Taihu Lake region, China. Science of the Total Environment,470, 1047–1055. https://doi.org/10.1016/j.scitotenv.2013.10.056.
CAS Article Google Scholar
Xu, Y., Guo, C., Luo, Y., Lv, J., Zhang, Y., Lin, H., et al. (2016). Occurrence and distribution of antibiotics, antibiotic resistance genes in the urban rivers in Beijing, China. Environmental Pollution,213, 833–840. https://doi.org/10.1016/j.envpol.2016.03.054.
CAS Article Google Scholar
Yan, C., Yang, Y., Zhou, J., Liu, M., Nie, M., Shi, H., et al. (2013). Antibiotics in the surface water of the Yangtze Estuary: Occurrence, distribution and risk assessment. Environmental Pollution,175, 22–29. https://doi.org/10.1016/j.envpol.2012.12.008.
CAS Article Google Scholar
Zhang, G., Deng, W., Yang, Y. S., & Salama, R. B. (2007). Evolution study of a regional groundwater system using hydrochemistry and stable isotopes in Songnen Plain, northeast China. Hydrological Processes,21(8), 1055–1065. https://doi.org/10.1002/hyp.6286.
CAS Article Google Scholar
Zhang, C., Liao, X., Li, J., Xu, L., Liu, M., Du, B., et al. (2013). Influence of long-term sewage irrigation on the distribution of organochlorine pesticides in soil-groundwater systems. Chemosphere,92(4), 337–343. https://doi.org/10.1016/j.chemosphere.2013.01.020.
CAS Article Google Scholar
Zhang, B., Song, X., Zhang, Y., Han, D., Tang, C., Yang, L., et al. (2015). The relationship between and evolution of surface water and groundwater in Songnen Plain, Northeast China. Environmental Earth Sciences,73(12), 8333–8343. https://doi.org/10.1007/s12665-014-3995-x.
CAS Article Google Scholar
Zhang, B., Song, X., Zhang, Y., Han, D., Tang, C., Yu, Y., et al. (2012). Hydrochemical characteristics and water quality assessment of surface water and groundwater in Songnen plain, Northeast China. Water Research,46(8), 2737–2748. https://doi.org/10.1016/j.watres.2012.02.033.
CAS Article Google Scholar
Zhang, D., Wang, Y., Yu, K., Li, P., Zhang, R., & Xu, Y. (2014). Occurrence, Distribution and Sources of organochlorine pesticides (OCPs) in surface sediments from the Lijiang River, a Typical Karst River of Southwestern China. Bulletin of Environmental Contamination and Toxicology,93(5), 580–585. https://doi.org/10.1007/s00128-014-1387-2.
CAS Article Google Scholar
Zheng, S., Chen, B., Qiu, X., Chen, M., Ma, Z., & Yu, X. (2016). Distribution and risk assessment of 82 pesticides in Jiulong River and estuary in South China. Chemosphere,144, 1177–1192. https://doi.org/10.1016/j.chemosphere.2015.09.050.
CAS Article Google Scholar
Zou, S., Huang, F., Chen, L., & Liu, F. (2018). The occurrence and distribution of antibiotics in the Karst River System in Kaiyang, Southwest China. Water Science and Technology: Water Supply,18, 2044–2052. https://doi.org/10.2166/ws.2018.026.
CAS Article Google Scholar

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Acknowledgements

This work is supported by the National Natural Science Foundation of China (No. 41572229) and the China Geological Survey (DD20160312).

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MOE Key Laboratory of Groundwater Circulation and Environmental Evolution, China University of Geosciences (Beijing), Beijing, 100083, People’s Republic of China
Fuyang Huang, Zeyan Li, Chong Zhang, Théogène Habumugisha & Fei Liu
Beijing Key Laboratory of Water Resources and Environmental Engineering, China University of Geosciences (Beijing), Beijing, 100083, People’s Republic of China
Fuyang Huang, Zeyan Li, Chong Zhang, Théogène Habumugisha & Fei Liu
School of Ocean Sciences, China University of Geosciences (Beijing), Beijing, 100083, People’s Republic of China
Ximing Luo

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Fuyang Huang
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Zeyan Li
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Chong Zhang
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Théogène Habumugisha
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Fei Liu
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Ximing Luo
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Huang, F., Li, Z., Zhang, C. et al. Pesticides in the typical agricultural groundwater in Songnen plain, northeast China: occurrence, spatial distribution and health risks. Environ Geochem Health 41, 2681–2695 (2019). https://doi.org/10.1007/s10653-019-00331-5

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Received: 02 March 2019
Accepted: 18 May 2019
Published: 25 May 2019
Issue Date: December 2019
DOI: https://doi.org/10.1007/s10653-019-00331-5

Keywords

Organochlorine pesticides
Organophosphorus pesticides
Carbamate pesticides
Groundwater
Songnen plain
Risk assessment