Abstract
Benzophenone (BP) and diethyl phthalate (DEP)—chemical substances of environmental concern due to potential toxicity—have been quantified in considerable concentrations in different environmental matrices worldwide. Wastewater treatment plants (WWTPs) with multi-stage hybrid biological systems have been considered a potential strategy to improve the removal of different micropollutants in wastewater from biological systems. On the other hand, investigations on the efficiency of these systems to treat real wastewater with focus on the removal of DEP are scarce, and there is no information on the removal of BP. The aim of this study was to evaluate the performance of a pilot-scale multi-stage hybrid bioreactor (MSHR) on the efficiency of BP and DEP removal from a real wastewater, whose composition varies over short periods of time, thus causing impacts on biological processes. The efficiency of the biological treatment was assessed in two different phases: (I) predominantly suspended biomass and (II) predominantly fixed biomass, both in the aerobic tank. Besides, this study presents and discusses the correlation between BP and DEP removal and different physical–chemical parameters and operating conditions. The highly variable composition of the influent illustrated by the variation in the organic load resulted in oscillation in the treatment performance. Despite this variation, the pilot-scale multi-stage hybrid bioreactor was able to remove up to 69.6% of BP and 74.5% of DEP, both in the phase of predominantly fixed biomass.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data availability
All data generated or analyzed during this study are included in this manuscript and its supplementary information file.
References
Abdel daiem, M. M., Rivera-Utrilla, J., Ocampo-Pérez, R., Méndez-Díaz, J. D., & Sánchez-Polo, M. (2012). Environmental impact of phthalic acid esters and their removal from water and sediments by different technologies - A review. Journal of Environmental Management, 109, 164–178. https://doi.org/10.1016/j.jenvman.2012.05.014
Ahmadi, E., Gholami, M., Farzadkia, M., Nabizadeh, R., & Azari, A. (2015). Study of moving bed biofilm reactor in diethyl phthalate and diallyl phthalate removal from synthetic wastewater. Bioresource Technology, 183, 129–135. https://doi.org/10.1016/j.biortech.2015.01.122
Alvarino, T., Lema, J., Omil, F., & Suárez, S. (2018a). Trends in organic micropollutants removal in secondary treatment of sewage. Reviews in Environmental Science and Biotechnology, 17(3), 447–469. https://doi.org/10.1007/s11157-018-9472-3
Alvarino, T., Suarez, S., Lema, J., & Omil, F. (2018b). Science of the total environment understanding the sorption and biotransformation of organic micropollutants in innovative biological wastewater treatment technologies. Science of the Total Environment, 615, 297–306. https://doi.org/10.1016/j.scitotenv.2017.09.278
APHA, AWWA, WEF. (2017). Standard methods for the examination of water and wastewater (23rd Editi.). Washington, DC.
Araujo, F. G., Bauerfeldt, G. F., Marques, M., & Martins, E. M. (2020). Development and validation of an analytical method for detection and quantification of benzophenone, bisphenol A, diethyl phthalate and 4-nonylphenol by UPLC-MS/MS in surface water. PeerJ Analytical Chemistry, 2, e7. https://doi.org/10.7717/peerj-achem.7
Archana, G., Dhodapkar, R., & Kumar, A. (2017). Ecotoxicological risk assessment and seasonal variation of some pharmaceuticals and personal care products in the sewage treatment plant and surface water bodies (lakes). Environmental Monitoring and Assessment, 189(9). https://doi.org/10.1007/s10661-017-6148-3
Arias, A., Alvarino, T., Allegue, T., Suárez, S., Garrido, J. M., & Omil, F. (2018). An innovative wastewater treatment technology based on UASB and IFAS for cost-efficient macro and micropollutant removal. Journal of Hazardous Materials, 359(July), 113–120. https://doi.org/10.1016/j.jhazmat.2018.07.042
Ashfaq, M., Li, Y., Wang, Y., Qin, D., Rehman, M. S. U., Rashid, A., et al. (2018). Monitoring and mass balance analysis of endocrine disrupting compounds and their transformation products in an anaerobic-anoxic-oxic wastewater treatment system in Xiamen, China. Chemosphere, 204, 170–177. https://doi.org/10.1016/j.chemosphere.2018.04.028
Banayan Esfahani, E., Asadi Zeidabadi, F., Bazargan, A., & McKay, G. (2019). The Modified Bardenpho Process. Handbook of Environmental Materials Management (1st ed.). Springer. https://doi.org/10.1007/978-3-319-73645-7_87
Bolívar-Subirats, G., Rivetti, C., Cortina-Puig, M., Barata, C., & Lacorte, S. (2021). Occurrence, toxicity and risk assessment of plastic additives in Besos river. Spain. Chemosphere, 263, 128022. https://doi.org/10.1016/j.chemosphere.2020.128022
Butler, C. S., & Boltz, J. P. (2014). Biofilm processes and control in water and wastewater treatment. Comprehensive Water Quality and Purification (Vol. 3). Elsevier Ltd. https://doi.org/10.1016/B978-0-12-382182-9.00083-9
Casas, M. E., Chhetri, R. K., Ooi, G., Hansen, K. M. S., Litty, K., Christensson, M., et al. (2015). Biodegradation of pharmaceuticals in hospital wastewater by staged moving bed biofilm reactors (MBBR). Water Research, 83, 293–302. https://doi.org/10.1016/j.watres.2015.06.042
Cetesb. (2011). Guia Nacional de Coleta e Preservação de Amostras - Água, Sedimento, Comunidades Aquáticas e Efluentes Líquidos. Companhia Ambiental do Estado de São Paulo. C737g
Chiang, Y., & Ismail, W. (2020). Anaerobic utilization of hydrocarbons, oils, and lipids. In Anaerobic Utilization of Hydrocarbons, Oils, and Lipids (1st ed., pp. 1–32). Cham: Springer. https://doi.org/10.1007/978-3-319-33598-8
Cunha, D. L., Araujo, F. G., & Marques, M. (2017). Psychoactive drugs: Occurrence in aquatic environment, analytical methods, and ecotoxicity—A review. Environmental Science and Pollution Research, 24, 24076–24091. https://doi.org/10.1007/s11356-017-0170-4
Cunha, D. L., Mendes, M. P., & Marques, M. (2019). Environmental risk assessment of psychoactive drugs in the aquatic environment. Environmental Science and Pollution Research, 26(1), 78–90. https://doi.org/10.1007/s11356-018-3556-z
Dargnat, C., Teil, M. J., Chevreuil, M., & Blanchard, M. (2009). Phthalate removal throughout wastewater treatment plant. Case study of Marne Aval station (France). Science of the Total Environment, 407(4), 1235–1244. https://doi.org/10.1016/j.scitotenv.2008.10.027
Dezotti, M., Lippel, G., & Bassin, J. P. (2018). Advanced biological processes for wastewater treatment: Emerging, consolidated technologies and introduction to molecular techniques. Advanced Biological Processes for Wastewater Treatment: Emerging, Consolidated Technologies and Introduction to Molecular Techniques (1st ed.). Springer International Publishing. https://doi.org/10.1007/978-3-319-58835-3
Falås, P., Wick, A., Castronovo, S., Habermacher, J., Ternes, T. A., & Joss, A. (2016). Tracing the limits of organic micropollutant removal in biological wastewater treatment. Water Research, 95, 240–249. https://doi.org/10.1016/j.watres.2016.03.009
Farajzadeh, M. A., & Mogaddam, M. R. A. (2012). Air-assisted liquid-liquid microextraction method as a novel microextraction technique: Application in extraction and preconcentration of phthalate esters in aqueous sample followed by gas chromatography-flame ionization detection. Analytica Chimica Acta, 728, 31–38. https://doi.org/10.1016/j.aca.2012.03.031
Fischer, K., & Majewsky, M. (2014). Cometabolic degradation of organic wastewater micropollutants by activated sludge and sludge-inherent microorganisms. Applied Microbiology and Biotechnology, 98(15), 6583–6597. https://doi.org/10.1007/s00253-014-5826-0
Gani, K. M., & Kazmi, A. A. (2020). Ecotoxicological risk evaluation and regulatory compliance of endocrine disruptor phthalates in a sustainable wastewater treatment scheme. Environmental Science and Pollution Research, 27(8), 7785–7794. https://doi.org/10.1007/s11356-019-07418-7
Gani, K. M., Rajpal, A., & Kazmi, A. A. (2016). Contamination level of four priority phthalates in North Indian wastewater treatment plants and their fate in sequencing batch reactor systems. Environmental Science: Processes and Impacts, 18(3), 406–416. https://doi.org/10.1039/c5em00583c
Gani, K. M., Tyagi, V. K., & Kazmi, A. A. (2017). Occurrence of phthalates in aquatic environment and their removal during wastewater treatment processes: A review. Environmental Science and Pollution Research, 24(21), 17267–17284. https://doi.org/10.1007/s11356-017-9182-3
Gao, D., Li, Z., Wen, Z., & Ren, N. (2014). Occurrence and fate of phthalate esters in full-scale domestic wastewater treatment plants and their impact on receiving waters along the Songhua River in China. Chemosphere, 95, 24–32. https://doi.org/10.1016/j.chemosphere.2013.08.009
Glassmeyer, S. T., Furlong, E. T., Kolpin, D. W., Cahill, J. D., Zaugg, S. D., Werner, S. L., et al. (2005). Transport of chemical and microbial compounds from known wastewater discharges: Potential for use as indicators of human fecal contamination. Environmental Science and Technology, 39(14), 5157–5169. https://doi.org/10.1021/es048120k
Gogoi, A., Mazumder, P., Tyagi, V. K., Tushara Chaminda, G. G., An, A. K., & Kumar, M. (2018). Occurrence and fate of emerging contaminants in water environment: A review. Groundwater for Sustainable Development, 6, 169–180. https://doi.org/10.1016/j.gsd.2017.12.009
Gracia-Lor, E., Martínez, M., Sancho, J. V., Peñuela, G., & Hernández, F. (2012). Multi-class determination of personal care products and pharmaceuticals in environmental and wastewater samples by ultra-high performance liquid-chromatography-tandem mass spectrometry. Talanta, 99, 1011–1023. https://doi.org/10.1016/j.talanta.2012.07.091
Guo, Q., Wei, D., Zhao, H., & Du, Y. (2020). Predicted no-effect concentrations determination and ecological risk assessment for benzophenone-type UV filters in aquatic environment. Environmental Pollution, 256, 113460. https://doi.org/10.1016/j.envpol.2019.113460
Harris, C. A., Henttu, P., Parker, M. G., & Sumpter, J. P. (1997). The estrogenic activity of phthalate esters in vitro. Environmental Health Perspectives, 105(8), 802–811.
Hu, B., Wheatley, A., Ishtchenko, V., & Huddersman, K. (2011). The effect of shock loads on SAF bioreactors for sewage treatment works. Chemical Engineering Journal, 166(1), 73–80. https://doi.org/10.1016/j.cej.2010.10.005
ICH. (2005). ICH Topic Q2 (R1) Validation of analytical procedures: Text and methodology. International Conference on Harmonization 17. http://www.ich.org/fileadmin/Public_Web_Site/ICH_Products/Guidelines/Quality/Q2_R1/Step4/Q2_R1__Guideline.pdf. Accessed 20 Aug 2020.
Karthikraj, R., & Kannan, K. (2017). Mass loading and removal of benzotriazoles, benzothiazoles, benzophenones, and bisphenols in Indian sewage treatment plants. Chemosphere, 181, 216–223. https://doi.org/10.1016/j.chemosphere.2017.04.075
Kawaguchi, M., Ito, R., Honda, H., Endo, N., Okanouchi, N., Saito, K., et al. (2008). Simultaneous analysis of benzophenone sunscreen compounds in water sample by stir bar sorptive extraction with in situ derivatization and thermal desorption-gas chromatography-mass spectrometry. Journal of Chromatography A, 1200(2), 260–263. https://doi.org/10.1016/j.chroma.2008.05.084
Kora, E., Theodorelou, D., Gatidou, G., Fountoulakis, M. S., & Stasinakis, A. S. (2020). Removal of polar micropollutants from domestic wastewater using a methanogenic—Aerobic moving bed biofilm reactor system. Chemical Engineering Journal, 382(May), 122983. https://doi.org/10.1016/j.cej.2019.122983
Kosek, K., Luczkiewicz, A., Fudala-Książek, S., Jankowska, K., Szopińska, M., Svahn, O., et al. (2020). Implementation of advanced micropollutants removal technologies in wastewater treatment plants (WWTPs)—Examples and challenges based on selected EU countries. Environmental Science and Policy, 112(April), 213–226. https://doi.org/10.1016/j.envsci.2020.06.011
Kotowska, U., Kapelewska, J., & Sawczuk, R. (2020). Occurrence, removal, and environmental risk of phthalates in wastewaters, landfill leachates, and groundwater in Poland. Environmental Pollution, 267, 115643. https://doi.org/10.1016/j.envpol.2020.115643
Li, M. H. (2012). Acute toxicity of benzophenone-type UV filters and paraben preservatives to freshwater planarian. Dugesia Japonica. Toxicological and Environmental Chemistry, 94(3), 566–573. https://doi.org/10.1080/02772248.2012.655695
Liu, B., Jiang, T., Li, Z., Ge, W., Wu, J., Song, N., & Chai, C. (2021). Phthalate esters in surface sediments from fishing ports in Circum-Bohai-Sea region. China. Marine Pollution Bulletin, 171, 112782. https://doi.org/10.1016/j.marpolbul.2021.112782
Liu, W., Song, X., Huda, N., Xie, M., Li, G., & Luo, W. (2020). Comparison between aerobic and anaerobic membrane bioreactors for trace organic contaminant removal in wastewater treatment. Environmental Technology & Innovation, 17, 100564. https://doi.org/10.1016/j.eti.2019.100564
Loraine, G. A., & Pettigrove, M. E. (2006). Seasonal variations in concentrations of pharmaceuticals and personal care products in drinking water and reclaimed wastewater in Southern California. Environmental Science and Technology, 40(3), 687–695. https://doi.org/10.1021/es051380x
Mao, F., He, Y., & Gin, K. Y. H. (2019). Occurrence and fate of benzophenone-type UV filters in aquatic environments: A review. Environmental Science: Water Research and Technology, 5(2), 209–223. https://doi.org/10.1039/c8ew00539g
Nantaba, F., Palm, W. U., Wasswa, J., Bouwman, H., Kylin, H., & Kümmerer, K. (2021). Temporal dynamics and ecotoxicological risk assessment of personal care products, phthalate ester plasticizers, and organophosphorus flame retardants in water from Lake Victoria. Uganda. Chemosphere, 262, 127716. https://doi.org/10.1016/j.chemosphere.2020.127716
Ødegaard, H. (2006). Innovations in wastewater treatment : The moving bed biofilm process. Water Science & Technology, 53(7491), 17–33. https://doi.org/10.2166/wst.2006.284
Ødegaard, H., Cimbritz, M., Christensson, M., & Dahl, C. P. (2012). Separation of biomass from moving bed biofilm reactors (MBBRs). Proceedings of the Water Environment Federation, 2010(7), 212–233. https://doi.org/10.2175/193864710798208368
Oliver, R., May, E., & Williams, J. (2005). The occurrence and removal of phthalates in a trickle filter STW. Water Research, 39(18), 4436–4444. https://doi.org/10.1016/j.watres.2005.08.011
Ping, L., Zhuang, H., & Shan, S. (2019). New insights into pollutants removal, toxicity reduction and microbial profiles in a lab-scale IC-A / O-membrane reactor system for paper wastewater reclamation. Science of the Total Environment, 674, 374–382. https://doi.org/10.1016/j.scitotenv.2019.04.164
Pugajeva, I., Rusko, J., Perkons, I., Lundanes, E., & Bartkevics, V. (2017). Journal of Pharmaceutical and Biomedical Analysis. Determination of pharmaceutical residues in wastewater using high performance liquid chromatography coupled to quadrupole-Orbitrap mass spectrometry. Journal of Pharmaceutical and Biomedical Analysis, 133, 64–74. https://doi.org/10.1016/j.jpba.2016.11.008
Ramos, S., Homem, V., & Santos, L. (2019). Development and optimization of a QuEChERS-GC–MS/MS methodology to analyse ultraviolet-filters and synthetic musks in sewage sludge. Science of the Total Environment, 651, 2606–2614. https://doi.org/10.1016/j.scitotenv.2018.10.143
Ribani, M., Grespan Bottoli, C. B., Collins, C. H., Fontes Jardim, I. C. S., & Costa Melo, L. F. (2004). Validation for chromatographic and electrophoretic methods. Quimica Nova, 27(5), 771–780. https://doi.org/10.1590/S0100-40422004000500017
Rogers, H. R. (1996). Sources, behaviour and fate of organic contaminants during sewage treatment and in sewage sludges. Science of the Total Environment, 185(1–3), 3–26. https://doi.org/10.1016/0048-9697(96)05039-5
Rusten, B., Eikebrokk, B., Ulgenes, Y., & Lygren, E. (2006). Design and operations of the Kaldnes moving bed biofilm reactors. Aquacultural Engineering, 34, 322–331. https://doi.org/10.1016/j.aquaeng.2005.04.002
Rusten, B., McCoy, M., Proctor, R., & Siljudalen, J. G. (1998). The innovative moving bed biofilm reactor/solids contact reaeration process for secondary treatment of municipal wastewater. Water Environment Research, 70(5), 1083–1089. https://doi.org/10.2175/106143098x123435
Salaudeen, T., Okoh, O., Agunbiade, F., & Okoh, A. (2018a). Fate and impact of phthalates in activated sludge treated municipal wastewater on the water bodies in the Eastern Cape, South Africa. Chemosphere, 203, 336–344. https://doi.org/10.1016/j.chemosphere.2018.03.176
Salaudeen, T., Okoh, O., Agunbiade, F., & Okoh, A. (2018b). Phthalates removal efficiency in different wastewater treatment technology in the Eastern Cape. South Africa. Environmental Monitoring and Assessment, 190(5), 299. https://doi.org/10.1007/s10661-018-6665-8
Shi, J., Fujisawa, S., Nakai, S., & Hosomi, M. (2004). Biodegradation of natural and synthetic estrogens by nitrifying activated sludge and ammonia-oxidizing bacterium Nitrosomonas europaea. Water Research, 38(9), 2323–2330. https://doi.org/10.1016/j.watres.2004.02.022
da Silva, A. S. A., de Castro, R. A., Martins, S. B., Alvim, R. D., de Salomão, A. L., & S., & Marques, M. . (2020). Extração de biomassa aderida ao meio-suporte de um reator de leito móvel com biofilme: Agitação mecânica e ultrassom. Engenharia Sanitaria e Ambiental, 25(6), 901–908. https://doi.org/10.1590/s1413-4152202020180113
Song, H. L., Yang, X. L., Xia, M. Q., & Chen, M. (2017). Co-metabolic degradation of steroid estrogens by heterotrophic bacteria and nitrifying bacteria in MBRs. Journal of Environmental Science and Health - Part A Toxic/hazardous Substances and Environmental Engineering, 52(8), 778–784. https://doi.org/10.1080/10934529.2017.1305168
Sun, H. Q., Du, Y., Zhang, Z. Y., Jiang, W. J., Guo, Y. M., Lu, X. W., et al. (2016). Acute toxicity and ecological risk assessment of benzophenone and N,N-diethyl-3 methylbenzamide in personal care products. International Journal of Environmental Research and Public Health, 13(9). https://doi.org/10.3390/ijerph13090925
Tran, N. H., Reinhard, M., & Gin, K. Y. H. (2018). Occurrence and fate of emerging contaminants in municipal wastewater treatment plants from different geographical regions—A review. Water Research, 133, 182–207. https://doi.org/10.1016/j.watres.2017.12.029
Wang, Y., Li, Y., Hu, A., Rashid, A., Ashfaq, M., Wang, Y., et al. (2018). Monitoring, mass balance and fate of pharmaceuticals and personal care products in seven wastewater treatment plants in Xiamen City. China. Journal of Hazardous Materials, 354(January), 81–90. https://doi.org/10.1016/j.jhazmat.2018.04.064
Wijekoon, K. C., Mcdonald, J. A., Khan, S. J., Hai, F. I., Price, W. E., & Nghiem, L. D. (2015). Bioresource technology development of a predictive framework to assess the removal of trace organic chemicals by anaerobic membrane bioreactor. Bioresource Technology, 189, 391–398. https://doi.org/10.1016/j.biortech.2015.04.034
Wu, M., & hong, Li, J., Xu, G., Ma, L. dan, Li, J. jun, Li, J. song, & Tang, L. . (2018). Pollution patterns and underlying relationships of benzophenone-type UV-filters in wastewater treatment plants and their receiving surface water. Ecotoxicology and Environmental Safety, 152, 98–103. https://doi.org/10.1016/j.ecoenv.2018.01.036
Ye, L., Liu, J., Yang, X., Peng, Y., & Xu, L. (2011). Orthogonal array design for the optimization of ionic liquid-based dispersive liquid-liquid microextraction of benzophenone-type UV filters. Journal of Separation Science, 34(6), 700–706. https://doi.org/10.1002/jssc.201000552
Zeng, F., Cui, K., Xie, Z., Liu, M., Li, Y., Lin, Y., et al. (2008). Occurrence of phthalate esters in water and sediment of urban lakes in a subtropical city, Guangzhou. South China. Environment International, 34(3), 372–380. https://doi.org/10.1016/j.envint.2007.09.002
Zhang, Q., Ma, X., Dzakpasu, M., & Wang, X. C. (2017). Evaluation of ecotoxicological effects of benzophenone UV filters: Luminescent bacteria toxicity, genotoxicity and hormonal activity. Ecotoxicology and Environmental Safety, 142(April), 338–347. https://doi.org/10.1016/j.ecoenv.2017.04.027
Zhao, X., Shen, J., & min, Zhang, H., Li, X., Chen, Z. lin, & Wang, X. chun. . (2020). The occurrence and spatial distribution of phthalate esters (PAEs) in the Lanzhou section of the Yellow River. Environmental Science and Pollution Research, 27(16), 19724–19735. https://doi.org/10.1007/s11356-020-08443-7
Funding
This study was financially supported by the Research Support Foundation of the State of Rio de Janeiro (FAPERJ) to the fourth author (E-26/202.261/2018, E-26/202.262/2018) and to the last author (E-26/202.894/2018). The Brazilian National Council for Scientific and Technological Development (CNPq) has also supported the last author (435883/2018–6; 308.335/2017–1).
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
do Amaral, A.F., da Silva, A.S.A., Coutinho, R. et al. Benzophenone and Diethyl Phthalate Removal from Real Wastewater by a Multi-stage Hybrid Reactor. Water Air Soil Pollut 232, 418 (2021). https://doi.org/10.1007/s11270-021-05388-6
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-021-05388-6