17β-Estradiol (E2) is normally detected in water at nanogram per liter levels, which could alter normal hormone functions and the physiological status of wildlife. In this study, biodegradation of E2 with microorganisms from activated sludge showed a high removal efficiency of 99.2% in 60 h. This was greater than the efficiency using single Escherichia coli. To remove E2 effectively, a system combining electrochemical and biological degradation was used to remove E2 from an aqueous solution. E2 removal efficiency using the combined system was increased at high dissolved oxygen concentrations and low pH and could reach 99.3% after 90 min. An electric current density of 20 mA/cm2 inhibited the growth of most bacterial species; however, dominant bacterial strains such as Bacillus, Lysinibacillus, and Aeromonas survived, leading to promotion of E2 degradation. From analysis of E2 degradation products by gas chromatography–mass spectrometry, E2 degradation was explained by the following process. First, E2 was oxidized to form hydroxylation products. Then, ring-opening oxidization of the products formed macromolecules and small-molecular-weight organic carboxylic acids. Finally, organic carboxylic acids were mineralized. It was also demonstrated that E2 degraded more quickly and completely by the combined system than by biological degradation.
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References
1.
AlbalawiF., and ZuoY. (2018). Photodegradation of 17α-ethynylestradiol (EE2) in the presence of humic acid and carbonate ions in water solutions. Int. J. Chem. Eng. Appl. 9, 71.
2.
BaiX., CaseyF.X.M., and HakkH. (2013). Dissipation and transformation of 17β-estradiol-17-sulfate in soil–water systems. J. Hazard. Mater. 260, 733.
3.
BehnajadyM.A., VahidB., ModirshahlaN., and ShokriM. (2009). Evaluation of electrical energy per order (EEO) with kinetic modeling on the removal of Malachite Green by US/UV/H2O2 process. Desalination, 249, 99.
4.
BosshardP.P., SantiniY., GrüterD., StettlerR., and BachofenR. (2000). Bacterial diversity and community composition in the chemocline of the meromictic alpine Lake Cadagno as revealed by 16S rDNA analysis. FEMS Microbiol. Ecol. 31, 173.
5.
ChenY., ZhangK., and ZuoY. (2013). Direct and indirect photodegradation of estriol in the presence of humic acid, nitrate and iron complexes in water solutions. Sci. Total Environ. 463, 802.
6.
ChoiT.S., SongY.C., and JoicyA. (2018). Influence of conductive material on the bioelectrochemical removal of organic matter and nitrogen from low strength wastewater. Bioresour. Technol. 259, 407.
7.
ClouzotL., MarrotB., DoumenqP., and RocheN. (2008). 17α-Ethinylestradiol: An endocrine disrupter of great concern. Analytical methods and removal processes applied to water purification. A review. Environ. Prog. Sustain., 27, 383.
8.
DaneshvarN., SalariD., and KhataeeA.R. (2003). Photocatalytic degradation of azo dye acid red 14 in water: Investigation of the effect of operational parameters. J. Photochem. Photobiol. A. 157, 111.
9.
DaskalakiV.M., FulgioneI., FrontistisZ., RizzoL., and MantzavinosD. (2013). Solar light-induced photoelectrocatalytic degradation of bisphenol-A on TiO2/ITO film anode and BDD cathode. Catal. Today. 209, 74.
10.
FanM., ZhouN., LiP., ChenL., ChenY., ShenS., and ZhuS. (2017). Anaerobic co-metabolic biodegradation of tetrabromobisphenol A using a bioelectrochemical system. J. Hazard. Mater. 321, 791.
11.
FengY., WangC., LiuJ., and ZhangZ. (2010). Electrochemical degradation of 17-alpha-ethinylestradiol (EE2) and estrogenic activity changes. J. Environ. Monitor. 12, 404.
12.
GongB., WangY., WangJ., HuangW., ZhouJ., and HeQ. (2018). Intensified nitrogen and phosphorus removal by embedding electrolysis in an anaerobic–anoxic–oxic reactor treating low carbon/nitrogen wastewater. Bioresour. Technol. 256, 562.
13.
GuL.P., HuangB., XuZ.X., MaX.D., and PanX.J. (2016). Dissolved organic matter as a terminal electron acceptor in the microbial oxidation of steroid estrogen. Environ. Pollut. 218, 26.
14.
HeH., HuangB., FuG., DuY.N., XiongD., LaiC.C., and PanX.J. (2017). Coupling electrochemical and biological methods for 17α-ethinylestradiol removal from water by different microorganisms. J. Hazard. Mater. 340, 120.
15.
HeH., HuangB., GuL.P., XiongD., LaiC.C., TangJ., and PanX.J. (2016). Stimulated dissolved organic matter by electrochemical route to produce activity substances for removing of 17α-ethinylestradiol. J. Electroanal. Chem. 780, 233.
16.
HuangB., SunW.W., LiX.M., LiuJ.L., LiQ., WangR.M., and PanX.J. (2015). Effects and bioaccumulation of 17β-estradiol and 17α-ethynylestradiol following long-term exposure in crucian carp. Ecotoxicol. Environ. Saf. 112, 169.
17.
HuangB., WangB., RenD., JinW., LiuJ.L., PengJ.H., and PanX.J. (2013). Occurrence, removal and bioaccumulation of steroid estrogens in Dianchi Lake catchment, China. Environ. Int. 59, 262.
18.
KatsumataH., KawabeS., KanecoS., SuzukiT., and OhtaK. (2004). Degradation of bisphenol A in water by the photo-Fenton reaction. J. Photochem. Photobiol. A. 162, 297.
19.
KumarG., SarataleR.G., KadierA., SivagurunathanP., ZhenG., KimS.H., and SarataleG.D. (2017). A review on bio-electrochemical systems (BESs) for the syngas and value added biochemicals production. Chemosphere, 177, 84.
20.
LarcherS., and YargeauV. (2013). Biodegradation of 17α-ethinylestradiol by heterotrophic bacteria. Environ. Pollut. 173, 17.
21.
LeeH.B., and LiuD. (2002). Degradation of 17β-estradiol and its metabolites by sewage bacteria. Water Air Soil Pollut. 134, 351.
22.
LiY., and LiH. (2014). Type IV pili of Acidithiobacillus ferrooxidans can transfer electrons from extracellular electron donors. J. Basic Microbiol. 54, 226.
23.
LiuJ.L., WangR.M., HuangB., LinC., WangY., and PanX.J. (2011a). Distribution and bioaccumulation of steroidal and phenolic endocrine disrupting chemicals in wild fish species from Dianchi Lake, China. Environ. Pollut. 159, 2815.
24.
LiuY., ZhangY., QuanX., ZhangJ., ZhaoH., and ChenS. (2011b). Effects of an electric field and zero valent iron on anaerobic treatment of azo dye wastewater and microbial community structures. Bioresour. Technol. 102, 2578.
25.
MasoudW., TakamiyaM., and VogensenF.K. (2011). Characterization of bacterial populations in Danish raw milk cheeses made with different starter cultures by denaturating gradient gel electrophoresis and pyrosequencing. Int. Dairy J. 21, 142.
26.
MazellierP., MéitéL., and De LaatJ. (2008). Photodegradation of the steroid hormones 17β-estradiol (E2) and 17α-ethinylestradiol (EE2) in dilute aqueous solution. Chemosphere, 73, 1216.
27.
MoreiraF.C., SolerJ., FonsecaA., SaraivaI., BoaventuraR.A., BrillasE., and VilarV.J. (2015). Incorporation of electrochemical advanced oxidation processes in a multistage treatment system for sanitary landfill leachate. Water Res. 81, 375.
28.
MurugananthanM., YoshiharaS., RakumaT., UeharaN., and ShirakashiT. (2007). Electrochemical degradation of 17β-estradiol (E2) at boron-doped diamond (Si/BDD) thin film electrode. Electrochim. Acta, 52, 3242.
29.
PengX., PanX., WangX., LiD., HuangP., QiuG., and ChuX. (2018). Accelerated removal of high concentration p-chloronitrobenzene using bioelectrocatalysis process and its microbial communities analysis. Bioresour. Technol. 249, 844.
30.
PuyolD., BatstoneD.J., HulsenT., AstalsS., PecesM., and KromerJ.O. (2017). Resource recovery from wastewater by biological technologies: Opportunities, challenges, and prospects. Front. Microbiol. 7, 2106.
31.
QiaoY., LiC.M., BaoS.J., LuZ., and HongY. (2008). Direct electrochemistry and electrocatalytic mechanism of evolved Escherichia coli cells in microbial fuel cells. Chem. Commun. 1290.
32.
SarataleG.D., SarataleR.G., ShahidM.K., ZhenG., KumarG., ShinH.S., and KimS.H. (2017). A comprehensive overview on electro-active biofilms, role of exo-electrogens and their microbial niches in microbial fuel cells (MFCs). Chemosphere, 178, 534.
33.
SongL.J., ZhuN.W., YuanH.P., HongY., and DingJ. (2010). Enhancement of waste activated sludge aerobic digestion by electrochemical pre-treatment. Water Res. 44, 4371.
34.
VelvizhiG., and MohanS.V. (2015). Bioelectrogenic role of anoxic microbial anode in the treatment of chemical wastewater: Microbial dynamics with bioelectro-characterization. Water Res. 70, 52.
35.
WoźnicaA., DzirbaJ., MańkaD., and ŁabużekS. (2003). Effects of electron transport inhibitors on iron reduction in Aeromonas hydrophila strain KB1. Anaerobe, 9, 125.
36.
YuC.P., RohH., and ChuK.H. (2007). 17β-Estradiol-degrading bacteria isolated from activated sludge. Environ. Sci. Technol. 41, 486.
37.
ZhangY., and AngelidakiI. (2014). Microbial electrolysis cells turning to be versatile technology: Recent advances and future challenges. Water Res. 56, 11.
38.
ZhengW., YatesS.R., and BradfordS.A. (2007). Analysis of steroid hormones in a typical dairy waste disposal system. Environ. Sci. Technol. 42, 530.
39.
ZuoY., Ed. (2014). High-Performance Liquid Chromatography (HPLC): Principles, Procedures and Practices. New York: Nova Science Publishers, Inc.
40.
ZuoY., ZhangK., and DengY. (2006). Occurrence and photochemical degradation of 17α-ethinylestradiol in Acushnet river estuary. Chemosphere, 63, 1583.
41.
ZuoY., ZhangK., and ZhouS. (2013). Determination of estrogenic steroids and microbial and photochemical degradation of 17α-ethinylestradiol (EE2) in lake surface water, a case study. Environ. Sci. Process. Impacts, 15, 1529.
