Skip to main content
SpringerLink
Log in

Adsorption studies of 17β-estradiol from aqueous solution using a novel stabilized Fe–Mn binary oxide nanocomposite

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

The removal of 17β-estradiol (E2) from contaminated water on nanoscale Fe–Mn binary oxide-loaded multiwalled carbon nanotubes (MWCNTs/FMBO) was evaluated in this work. The characterizations of the mesoporous adsorbent were analyzed by using SEM, TEM, VSM, XRD, XPS, and FTIR measurements. The effects of experimental conditions in E2 removal, including stabilizer additional level, adsorption time, initial E2 concentration, solution pH, reaction temperature, and foreign ions, were examined. The maximum monolayer adsorption capacity (qm) of MWCNTs/FMBO for E2 in the experiment was 47.25 mg/g as verified by the Langmuir sorption isotherm study. The adsorption process was pH-sensitive with an optimum pH of 7.0. On the kinetics study, the adsorption data could be satisfactorily fitted by the pseudo-second-order kinetics. Thermodynamic parameters indicated that the adsorption process was spontaneous and exothermal. In addition, the foreign ions did not show any noticeable inhibition for E2 removal from the water solution except for PO43− that was adversely affected for E2 uptake than other anions in a certain concentration. The adsorption capacities of the mesoporous adsorbent remained at 86.16% even after five adsorption–desorption cycles without significant loss of capacity, which demonstrated the stability and reusability for further removal of E2. Moreover, both hydrogen bond and π–π interaction might be the dominating adsorption mechanisms for E2 adsorption onto MWCNTs/FMBO.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9

Similar content being viewed by others

References

  • An B, Zhao D (2012) Immobilization of As (III) in soil and groundwater using a new class of polysaccharide stabilized Fe–Mn oxide nanoparticles. J Hazard Mater 211:332–341

    Article  CAS  Google Scholar 

  • Awual MR (2017a) New type mesoporous conjugate material for selective optical copper(II) ions monitoring & removal from polluted waters. Chem Eng J 307:85–94

    Article  CAS  Google Scholar 

  • Awual MR (2017b) Novel nanocomposite materials for efficient and selective mercury ions capturing from wastewater. Chem Eng J 307:456–465

    Article  CAS  Google Scholar 

  • Awual MR, Khaleque MA, Ratna Y, Znad H (2015) Simultaneous ultra-trace palladium(II) detection and recovery from wastewater using new class meso-adsorbent. J Ind Eng Chem 21:405–413

    Article  CAS  Google Scholar 

  • Awual MR, Hasan MM, Eldesoky GE, Khaleque MA, Rahman MM, Naushad M (2016) Facile mercury detection and removal from aqueous media involving ligand impregnated conjugate nanomaterials. Chem Eng J 290:243–251

    Article  CAS  Google Scholar 

  • Boparai HK, Joseph M, O’Carroll DM (2011) Kinetics and thermodynamics of cadmium ion removal by adsorption onto nano zerovalent iron particles. J Hazard Mater 186:458–465

    Article  CAS  Google Scholar 

  • Bradley PM, Writer JH (2014) Effect of light on biodegradation of estrone, 17β-estradiol, and 17α-ethinylestradiol in stream sediment. JAWRA J Am Water Resour Assoc 50:334–342

    Article  CAS  Google Scholar 

  • Campbell CG, Borglin SE, Green FB, Grayson A, Wozei E, Stringfellow WT (2006) Biologically directed environmental monitoring, fate, and transport of estrogenic endocrine disrupting compounds in water: a review. Chemosphere 65:1265–1280

    Article  CAS  Google Scholar 

  • Cornell RM, Schwertmann U (1997) The iron oxides: structure, properties, reactions, occurrence and uses. Mineral Mag 61:740–741

    Article  Google Scholar 

  • Cui HJ, Cai JK, Zhao H, Yuan B, Ai CL, Fu ML (2014) Fabrication of magnetic porous Fe-Mn binary oxide nanowires with superior capability for removal of As(III) from water. J Hazard Mater 279:26–31

    Article  CAS  Google Scholar 

  • Fan Z, Casey FX, Hakk H, Larsen GL (2007) Persistence and fate of 17β-estradiol and testosterone in agricultural soils. Chemosphere 67:886–895

    Article  CAS  Google Scholar 

  • Fan L, Luo C, Lv Z, Lu F, Qiu H (2011) Removal of Ag+ from water environment using a novel magnetic thiourea-chitosan imprinted Ag+. J Hazard Mater 194:193–201

    Article  CAS  Google Scholar 

  • Fan Z, Hu J, An W, Yang M (2013) Detection and occurrence of chlorinated byproducts of bisphenol a, nonylphenol, and estrogens in drinking water of China: comparison to the parent compounds. Environ Sci Technol 47:10841–10850

    Article  CAS  Google Scholar 

  • Huang D-L, Zeng G-M, Feng C-L, Hu S, Jiang X-Y, Tang L, Su F-F, Zhang Y, Zeng W, Liu H-L (2008) Degradation of lead-contaminated lignocellulosic waste by Phanerochaete chrysosporium and the reduction of lead toxicity. Environ Sci Technol 42:4946–4951

    Article  CAS  Google Scholar 

  • Jiang L-h, Liu Y-g, Zeng G-m, Xiao F-y, Hu X-j, Hu X, Wang H, Li T-t, Zhou L, Tan X-f (2016) Removal of 17β-estradiol by few-layered graphene oxide nanosheets from aqueous solutions: external influence and adsorption mechanism. Chem Eng J 284:93–102

    Article  CAS  Google Scholar 

  • Jiang L, Gu Y, Guo H, Liu L, Chen J (2017) Efficient removal of 17α-ethinylestradiol (EE2) from water using freshly formed Fe–Mn binary oxide. RSC Adv 7:23802–23811

    Article  Google Scholar 

  • Johnson AC, Dumont E, Williams RJ, Oldenkamp R, Cisowska I, Sumpter JP (2013) Do concentrations of ethinylestradiol, estradiol, and diclofenac in European rivers exceed proposed EU environmental quality standards? Environ Sci Technol 47:12297–12304

    Article  CAS  Google Scholar 

  • Khanal SK, Xie B, Thompson ML, Sung S, Ong S-K, Van Leeuwen J (2006) Fate, transport, and biodegradation of natural estrogens in the environment and engineered systems. Environ Sci Technol 40:6537–6546

    Article  CAS  Google Scholar 

  • Kong S, Wang Y, Hu Q, Olusegun AK (2014) Magnetic nanoscale Fe–Mn binary oxides loaded zeolite for arsenic removal from synthetic groundwater. Colloids Surf A Physicochem Eng Asp 457:220–227

    Article  CAS  Google Scholar 

  • Lee Y, Yoon J, Von Gunten U (2005) Kinetics of the oxidation of phenols and phenolic endocrine disruptors during water treatment with ferrate (Fe (VI)). Environ Sci Technol 39:8978–8984

    Article  CAS  Google Scholar 

  • Lehman JH, Terrones M, Mansfield E, Hurst KE, Meunier V (2011) Evaluating the characteristics of multiwall carbon nanotubes. Carbon 49:2581–2602

    Article  CAS  Google Scholar 

  • Li XQ, Zhang WX (2007) Sequestration of metal cations with zerovalent iron nanoparticles: a study with high resolution X-ray photoelectron spectroscopy (HR-XPS). J Phys Chem C 111:6939–6946

    Article  CAS  Google Scholar 

  • Li J, Chen J, Yu Y, He C (2015) Fe–Mn–Ce/ceramic powder composite catalyst for highly volatile elemental mercury removal in simulated coal-fired flue gas. J Ind Eng Chem 25:352–358

    Article  CAS  Google Scholar 

  • Li H, Chen Y, Long J, Li X, Jiang D, Zhang P, Qi J, Huang X, Liu J, Xu R (2017a) Removal of thallium from aqueous solutions using Fe-Mn binary oxides. J Hazard Mater 338:296–305

    Article  CAS  Google Scholar 

  • Li MF, Liu YG, Liu SB, Shu D, Zeng GM, Hu XJ, Tan XF, Jiang LH, Yan ZL, Cai XX (2017b) Cu(II)-influenced adsorption of ciprofloxacin from aqueous solutions by magnetic graphene oxide/nitrilotriacetic acid nanocomposite: competition and enhancement mechanisms. Chem Eng J 319:219–228

    Article  CAS  Google Scholar 

  • Li MF, Liu YG, Zeng GM, Liu SB, Hu XJ, Shu D, Jiang LH, Tan XF, Cai XX, Yan ZL (2017c) Tetracycline absorbed onto nitrilotriacetic acid-functionalized magnetic graphene oxide: influencing factors and uptake mechanism. J Colloid Interface Sci 485:269–279

    Article  CAS  Google Scholar 

  • Liu R, Frost RL, Martens WN (2009) Absorption of the selenite anion from aqueous solutions by thermally activated layered double hydroxide. Water Res 43:1323–1329

    Article  CAS  Google Scholar 

  • Liu H, Yang Y, Kang J, Fan M, Qu J (2012) Removal of tetracycline from water by Fe-Mn binary oxide. J Environ Sci (China) 24(2):242–247

    Article  CAS  Google Scholar 

  • McArdell CS, Stone AT, Tian J (1998) Reaction of EDTA and related aminocarboxylate chelating agents with CoIIIOOH (heterogenite) and MnIIIOOH (manganite). Environ Sci Technol 32:2923–2930

    Article  CAS  Google Scholar 

  • Moradi O, Yari M, Zare K, Mirza B, Najafi F (2012) Carbon nanotubes: a review of chemistry principles and reactions. Fullerene Sci Technol 20:138–151

    CAS  Google Scholar 

  • Nakada N, Nyunoya H, Nakamura M, Hara A, Iguchi T, Takada H (2004) Identification of estrogenic compounds in wastewater effluent. Environ Toxicol Chem 23:2807–2815

    Article  Google Scholar 

  • Ning Q, Liu Y, Liu S, Jiang L, Zeng G, Zeng Z, Wang X, Li J, Kare Z (2017) Fabrication of hydrochar functionalized Fe–Mn binary oxide nanocomposites: characterization and 17β-estradiol removal. Rsc Advances 7: 37122–37129

  • Petersen EJ, Zhang L, Mattison NT, O’Carroll DM, Whelton AJ, Uddin N, Nguyen T, Huang Q, Henry TB, Holbrook RD (2011) Potential release pathways, environmental fate, and ecological risks of carbon nanotubes. Environ Sci Technol 45:9837–9856

    Article  CAS  Google Scholar 

  • Qin C, Troya D, Shang C, Hildreth S, Helm R, Xia K (2014) Surface catalyzed oxidative oligomerization of 17β-estradiol by Fe3+-saturated montmorillonite. Environ Sci Technol 49:956–964

    Article  CAS  Google Scholar 

  • Rodgers-Gray TP, Jobling S, Kelly C, Morris S, Brighty G, Waldock MJ, Sumpter JP, Tyler CR (2001) Exposure of juvenile roach (Rutilus rutilus) to treated sewage effluent induces dose-dependent and persistent disruption in gonadal duct development. Environ Sci Technol 35:462–470

    Article  CAS  Google Scholar 

  • Rubert KF IV, Pedersen JA (2006) Kinetics of oxytetracycline reaction with a hydrous manganese oxide. Environ Sci Technol 40:7216–7221

    Article  CAS  Google Scholar 

  • Schmitt S, Reifferscheid G, Claus E, Schlüsener M, Buchinger S (2012) Effect directed analysis and mixture effects of estrogenic compounds in a sediment of the river Elbe. Environ Sci Pollut Res 19:3350–3361

    Article  CAS  Google Scholar 

  • Singh SK, Townsend TG, Mazyck D, Boyer TH (2012) Equilibrium and intra-particle diffusion of stabilized landfill leachate onto micro- and meso-porous activated carbon. Water Res 46:491–499

    Article  CAS  Google Scholar 

  • Soria-Sánchez M, Maroto-Valiente A, Álvarez-Rodríguez J, Muñoz-Andrés V, Rodríguez-Ramos I, Guerrero-Ruíz A (2011) Carbon nanostrutured materials as direct catalysts for phenol oxidation in aqueous phase. Appl Catal B Environ 104:101–109

    Article  CAS  Google Scholar 

  • Sun W, Zhou K (2014) Adsorption of 17β-estradiol by multi-walled carbon nanotubes in natural waters with or without aquatic colloids. Chem Eng J 258:185–193

    Article  CAS  Google Scholar 

  • Szlachta M, Gerda V, Chubar N (2012) Adsorption of arsenite and selenite using an inorganic ion exchanger based on Fe–Mn hydrous oxide. J Colloid Interface Sci 365:213–221

    Article  CAS  Google Scholar 

  • Taguchi T (2016) Encapsulation of cesium from contaminated water with highly selective facial organic-inorganic mesoporous hybrid adsorbent. Chem Eng J 291:128–137

    Article  CAS  Google Scholar 

  • Tang L, Zeng G-M, Shen G-L, Li Y-P, Zhang Y, Huang D-L (2008) Rapid detection of picloram in agricultural field samples using a disposable immunomembrane-based electrochemical sensor. Environ Sci Technol 42:1207–1212

    Article  CAS  Google Scholar 

  • Tang J, Huang Y, Gong Y, Lyu H, Wang Q, Ma J (2016) Preparation of a novel graphene oxide/Fe-Mn composite and its application for aqueous Hg (II) removal. J Hazard Mater 316:151–158

    Article  CAS  Google Scholar 

  • Tomoko F, Satoshi I, Makoto K, Osamu S, Ikuo A (2006) Absorbability of estrone and 17beta-estradiol in water onto activated carbon. Water Research 40: 241–248

  • Toupin M, Brousse T, Bélanger D (2004) Charge storage mechanism of MnO2 electrode used in aqueous electrochemical capacitor. Chem Mater 16:3184–3190

    Article  CAS  Google Scholar 

  • Wang J, Chen Z, Chen B (2014) Adsorption of polycyclic aromatic hydrocarbons by graphene and graphene oxide nanosheets. Environ Sci Technol 48:4817–4825

    Article  CAS  Google Scholar 

  • Wang F, Sun W, Pan W, Xu N (2015) Adsorption of sulfamethoxazole and 17β-estradiol by carbon nanotubes/CoFe2O4 composites. Chem Eng J 274:17–29

    Article  CAS  Google Scholar 

  • Wu Z, Zhong H, Yuan X, Wang H, Wang L, Chen X, Zeng G, Wu Y (2014) Adsorptive removal of methylene blue by rhamnolipid-functionalized graphene oxide from wastewater. Water Res 67:330–344

    Article  CAS  Google Scholar 

  • Xie W, Liang Q, Qian T, Zhao D (2015) Immobilization of selenite in soil and groundwater using stabilized Fe–Mn binary oxide nanoparticles. Water Res 70:485–494

    Article  CAS  Google Scholar 

  • Xu L, Xu C, Zhao M, Qiu Y, Sheng GD (2008) Oxidative removal of aqueous steroid estrogens by manganese oxides. Water Res 42:5038–5044

    Article  CAS  Google Scholar 

  • Xu J, Wang L, Zhu Y (2012) Decontamination of bisphenol A from aqueous solution by graphene adsorption. Langmuir 28:8418–8425

    Article  CAS  Google Scholar 

  • Xu H, Qu Z, Zhao S, Mei J, Quan F, Yan N (2015) Different crystal-forms of one-dimensional MnO2 nanomaterials for the catalytic oxidation and adsorption of elemental mercury. J Hazard Mater 299:86–93

    Article  CAS  Google Scholar 

  • Yan Z-l, Liu Y-g, Tan X-f, Liu S-b, Zeng G-m, Jiang L-h, Li M-f, Zhou Z, Liu S, Cai X-x (2017) Immobilization of aqueous and sediment-sorbed ciprofloxacin by stabilized Fe-Mn binary oxide nanoparticles: influencing factors and reaction mechanisms. Chem Eng J 314:612–621

    Article  CAS  Google Scholar 

  • Yin Z, Liu Y, Liu S, Jiang L, Tan X, Zeng G, Li M, Liu S, Tian S, Fang Y (2018) Activated magnetic biochar by one-step synthesis: Enhanced adsorption and coadsorption for 17β-estradiol and copper. Science of the Total Environment 639: 1530

  • Yin Z, Liu Y, Tan X, Jiang L, Zeng G, Liu S, Tian S, Liu S, Liu N, Li M (2019) Adsorption of 17β-estradiol by a novel attapulgite/biochar nanocomposite: Characteristics and influencing factors. Process Safety and Environmental Protection 121: 155–164

  • Zaib Q, Khan IA, Saleh NB, Flora JR, Park Y-G, Yoon Y (2012) Removal of bisphenol A and 17β-estradiol by single-walled carbon nanotubes in aqueous solution: adsorption and molecular modeling. Water Air Soil Pollut 223:3281–3293

    Article  CAS  Google Scholar 

  • Zeng W, Liu Y-g, Hu X-j, Liu S-b, Zeng G-m, Zheng B-h, Jiang L-h, Guo F-y, Ding Y, Xu Y (2016) Decontamination of methylene blue from aqueous solution by magnetic chitosan lignosulfonate grafted with graphene oxide: effects of environmental conditions and surfactant. RSC Adv 6:19298–19307

    Article  CAS  Google Scholar 

  • Zhang H, Huang C-H (2003) Oxidative transformation of triclosan and chlorophene by manganese oxides. Environ Sci Technol 37:2421–2430

    Article  CAS  Google Scholar 

  • Zhang H-B, Lin G-D, Zhou Z-H, Dong X, Chen T (2002) Raman spectra of MWCNTs and MWCNT-based H2-adsorbing system. Carbon 40:2429–2436

    Article  CAS  Google Scholar 

  • Zhang S, Shao T, Bekaroglu SSK, Karanfil T (2010a) Adsorption of synthetic organic chemicals by carbon nanotubes: effects of background solution chemistry. Water Res 44:2067–2074

    Article  CAS  Google Scholar 

  • Zhang S, Shao T, Kose HS, Karanfil T (2010b) Adsorption of aromatic compounds by carbonaceous adsorbents: a comparative study on granular activated carbon, activated carbon fiber, and carbon nanotubes. Environ Sci Technol 44:6377–6383

    Article  CAS  Google Scholar 

  • Zhang Y, Ali SF, Dervishi E, Xu Y, Li Z, Casciano D, Biris AS (2010c) Cytotoxicity effects of graphene and single-wall carbon nanotubes in neural phaeochromocytoma-derived PC12 cells. ACS Nano 4:3181–3186

    Article  CAS  Google Scholar 

  • Zhang C-L, Qiao G-L, Zhao F, Wang Y (2011) Thermodynamic and kinetic parameters of ciprofloxacin adsorption onto modified coal fly ash from aqueous solution. J Mol Liq 163:53–56

    Article  CAS  Google Scholar 

  • Zhang W, Li Y, Wang Q, Wang C, Wang P, Mao K (2013) Performance evaluation and application of surface-molecular-imprinted polymer-modified TiO2 nanotubes for the removal of estrogenic chemicals from secondary effluents. Environ Sci Pollut Res 20:1431–1440

    Article  CAS  Google Scholar 

Download references

Funding

This research was financially supported by the National Natural Science Foundation of China (Grant No. 51609268) and the Key Project of Technological Innovation in the Field of Social Development of Hunan Province, China (Grant Nos. 2016SK2010 and 2016SK2001).

Author information

Authors and Affiliations

  1. College of Environmental Science and Engineering, Hunan University, Changsha, 410082, People’s Republic of China

    Ming-yang Dai, Yun-guo Liu, Guang-ming Zeng & Qi-meng Ning

  2. Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, 410082, People’s Republic of China

    Ming-yang Dai, Yun-guo Liu, Guang-ming Zeng & Qi-meng Ning

  3. School of Metallurgy and Environment, Central South University, Changsha, 410083, People’s Republic of China

    Shao-bo Liu

Authors
  1. Ming-yang Dai
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yun-guo Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Guang-ming Zeng
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Shao-bo Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Qi-meng Ning
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Yun-guo Liu.

Additional information

Responsible editor: Tito Roberto Cadaval Jr

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

ESM 1

(DOCX 376 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Dai, My., Liu, Yg., Zeng, Gm. et al. Adsorption studies of 17β-estradiol from aqueous solution using a novel stabilized Fe–Mn binary oxide nanocomposite. Environ Sci Pollut Res 26, 7614–7626 (2019). https://doi.org/10.1007/s11356-019-04173-7

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-019-04173-7

Keywords

Search

Navigation