Through elemental analysis, ultraviolet-visible spectra and fluorescence index, the composition and structure of the humic acid with and without 15 days biological modification were analyzed, and compared the binding function of three kinds of humic acid on 17β-estradiol (E2). And the binding function between 17β-estradiol (E2) and three different kinds of humic acid that before and after bio-modification were then compared. At last, the microbial degradation influences of E2 mediated by humic acid were studied. The elemental analysis results showed that the (N+O)/C values of humic acid (OLHA, OLFA, OSHA) that before bio-modification and humic acid (BLHA, BLFA, BSHA) that after biological modification were 0.801, 1.214, 0.820 and 0.629, 1.080, 0.797, respectively. The ultraviolet-visible spectrum results showed that the values of SUVA254were 0.146, 0.023, 0.073 and 0.179, 0.036, respectively. And the fluorescence index (FI) were 0.723, 3.385, 2.757 and 0.681, 3.017, 1.702, respectively. The above three kinds of characterization analysis results showed that the polarity of humic acid were consistent, suggesting that the polarity of modified humic acid were weaker than former. Moreover, the binding efficiency of 3 mg/L E2 by 5 mgC/L three humic acid before and after the bio-modification within 30h were 31.37%, 4.96%, 25.86% and 37.78%, 6.03%, 29.92%, respectively, which showed that the binding functions of E2 were increased obviously after humic acid bio-modification treatment. The biodegradation efficiency of 3 mg/L E2 by 5 mgC/L three humic acid before and after the bio-modification within 30h were 46.28%, 15.96%, 38.76% and 51.11%, 17.30%, 44.33%, respectively. Meanwhile, the stronger binding function of the same humic acid concentrations on E2, the greater efficiency of combined humic acid mediated microbial degradation of E2.
Kang S, Xing B. Humic acid fractionation upon sequential adsorption onto goethite[J]. Langmuir, 2008,24(6):2525-2531.
[2]
Hur J, Park M-H, Schlautman M A. Microbial transformation of dissolved leaf litter organic matter and its effects on selected organic matter operational descriptors[J]. Environmental Science and Technology, 2009,43(7):2315-2321.
Hur J, Schlautman M A. Using selected operational descriptors to examine the heterogeneity within a bulk humic substance[J]. Environmental Science and Technology, 2003,37(5):880-887.
[5]
Pan B, Ghosh S, Xing B. Nonideal binding between dissolved humic acids and polyaromatic hydrocarbons[J]. Environmental Science and Technology, 2007,41(18):6472-6478.
[6]
Tyler C, Jobling S, Sumpter J. Endocrine disruption in wildlife:a critical review of the evidence[J]. CRC Critical Reviews in Toxicology, 1998,28(4):319-361.
[7]
Jürgens M D, Holthaus K I, Johnson A C, et al. The potential for estradiol and ethinylestradiol degradation in English rivers[J]. Environmental Toxicology and Chemistry, 2002,21(3):480-488.
[8]
Hansen P-D, Dizer H, Hock B, et al. Vitellogenin-a biomarker for endocrine disruptors[J]. TrAC Trends in Analytical Chemistry, 1998,17(7):448-451.
[9]
Jobling S, Williams R, Johnson A, et al. Predicted exposures to steroid estrogens in UK rivers correlate with widespread sexual disruption in wild fish populations[J]. Environ. Heal. Perspect., 2005,114(S-1):32-39.
[10]
Lee O, Takesono A, Tada M, et al. Biosensor zebrafish provide new insights into potential health effects of environmental estrogens[J]. Environ. Heal. Perspect., 2012,120(7):990.
[11]
Silva C P, Otero M, Esteves V. Processes for the elimination of estrogenic steroid hormones from water:a review[J]. Environmental Pollution, 2012,165:38-58.
[12]
Fang H, Gao Y, Li G, et al. Advanced oxidation kinetics and mechanism of preservative propylparaben degradation in aqueous suspension of TiO2 and risk assessment of its degradation products[J]. Environ. Sci. Technol., 2013,47(6):2704-2712.
[13]
Ji H, Jiang L-Y, Zhang L, et al. Degradation Kinetics of Ethinyl Estradiol (EE2) Removal by Aqueous Manganese Dioxide[J]. Environ. Sci. Technol., 2011,12:008.
[14]
Carlson J C, Stefan M I, Parnis J M, et al. Direct UV Photolysis of Selected Pharmaceuticals, Personal Care Products and Endocrine Disruptors in Aqueous Solution[J]. Water Research, 2015,84:350-361.
[15]
Lee Y, Escher B I, Von Gunten U. Efficient removal of estrogenic activity during oxidative treatment of waters containing steroid estrogens[J]. Environ. Sci. Technol., 2008,42(17):6333-6339.
[16]
Kuramitz H, Nakata Y, Kawasaki M, et al. Electrochemical oxidation of bisphenol A. Application to the removal of bisphenol A using a carbon fiber electrode[J]. Chemosphere, 2001, 45(1):37-43.
[17]
Borrás M, Laios I, El Khissiin A, et al. Estrogenic and antiestrogenic regulation of the half-life of covalently labeled estrogen receptor in MCF-7breast cancer cells[J]. J. Steroid Biochemistry and Molecular Biology, 1996,57(3):203-213.
[18]
Huang B, Wang B, Ren D, et al. Occurrence, removal and bioaccumulation of steroid estrogens in Dianchi Lake catchment, China[J]. Environment International, 2013,59:262-273.
[19]
Bagnall J, Ito A, McAdam E, et al. Resource dependent biodegradation of estrogens and the role of ammonia oxidising and heterotrophic bacteria[J]. J. Hazardous Materials, 2012,239:56-63.
Larcher S, Yargeau V. Biodegradation of 17α-ethinylestradiol by heterotrophic bacteria[J]. Environ. Poll., 2013,173:17-22.
[22]
Bai X, Casey F X, Hakk H, et al. Dissipation and transformation of 17β-estradiol-17-sulfate in soil-water systems[J]. Journal of Hazardous Materials, 2013,260:733-739.
Hur J, Lee M-H, Song H, et al. Microbial transformation of dissolved organic matter from different sources and its influence on disinfection byproduct formation potentials[J]. Environmental Science and Pollution Research, 2013,20(6):4176-4187.
[25]
Stubbins A, Hood E, Raymond P A, et al. Anthropogenic aerosols as a source of ancient dissolved organic matter in glaciers[J]. Nature Geoscience, 2012,5(3):198-201.
[26]
Hur J, Lee B-M, Shin H-S. Microbial degradation of dissolved organic matter (DOM) and its influence on phenanthrene-DOM interactions[J]. Chemosphere, 2011,85(8):1360-1367.
[27]
Kang K H, Shin H S, Park H. Characterization of humic substances present in landfill leachates with different landfill ages and its implications[J]. Water Research, 2002,36(16):4023-4032.
[28]
Chin Y-P, Aiken G R, Danielsen K M. Binding of pyrene to aquatic and commercial humic substances:the role of molecular weight and aromaticity[J]. Environmental Science and Technology, 1997,31(6):1630-1635.
[29]
Wen B, Zhang J-j, Zhang S-z, et al. Phenanthrene sorption to soil humic acid and different humin fractions[J]. Environmental Science and Technology, 2007,41(9):3165-3171.
Weishaar J L, Aiken G R, Bergamaschi B A, et al. Evaluation of specific ultraviolet absorbance as an indicator of the chemical composition and reactivity of dissolved organic carbon[J]. Environmental Science and Technology, 2003,37(20):4702-4708.
[32]
Zhao H, Chen J, Qiao X, et al. Polybrominated diphenyl ethers in soils of the modern Yellow River Delta, China:occurrence, distribution and inventory[J]. Chemosphere, 2012,88(7):791-797.
Nkhili E, Boguta P, Bejger R, et al. Photosensitizing properties of water-extractable organic matter from soils[J]. Chemosphere, 2014,95:317-323.
[35]
Sakultantimetha A, Keenan H E, Beattie T K, et al. Effects of organic nutrients and growth factors on biostimulation of tributyltin removal by sediment microorganisms and Enterobacter cloacae[J]. Appl. Microbiol. Biotechnol., 2011,90(1):353-360.
[36]
Ye J, Yin H, Peng H, et al. Biosorption and biodegradation of triphenyltin by Brevibacillus brevis[J]. Bioresource Technology, 2013,129:236-241.
[37]
Yan Z, Song N, Cai H, et al. Enhanced degradation of phenanthrene and pyrene in freshwater sediments by combined employment of sediment microbial fuel cell and amorphous ferric hydroxide[J]. J. Hazardous Materials, 2012,199:217-225.
[38]
Li J, Fu J, Xiang X, et al. Kinetics, equilibrium, and mechanisms of sorption and desorption of 17α-ethinyl estradiol in two natural soils and their organic fractions[J]. Science of the Total Environment, 2013,452:404-410.
[39]
Meng X, Liu G, Zhou J, et al. Effects of redox mediators on azo dye decolorization by Shewanella algae under saline conditions[J]. Bioresource Technology, 2014,151:63-68.