Skip to main content
SpringerLink
Log in

Efficient removal of oxytetracycline from aqueous solution by a novel magnetic clay–biochar composite using natural attapulgite and cauliflower leaves

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

Abstract

A novel magnetic attapulgite–biochar composite (MABC) derived from natural attapulgite, cauliflower leaves, and FeCl3 was successfully prepared as a low-cost adsorbent for oxytetracycline (OTC) removal from aqueous solution. Characterization experiments by different techniques suggested that attapulgite clay particles and Fe3O4 nanoparticles were successfully covered on the MABC surface. Compared with the pristine biochar (CLB) and attapulgite–biochar composite (ABC), MABC had the largest surface area, well-developed pore structure, and more surface oxygen-containing functional groups which could interact with organic pollutant via hydrogen bonding, π–π electron coupling, complexation, and ion exchange. The maximum adsorption capacity of MABC by the Langmuir model was 33.31 mg/g, which was dramatically higher than that of CLB and ABC. The effects of solution initial pH had little difference on the adsorption of OTC because of the buffering effect. Adsorbent-regeneration studies of MABC exhibited good reusability and separation property. All the results indicated that MABC could be used as a potential adsorbent because of its easy preparation and separation, high efficiency, wide pH range application, and abundant and cheap raw materials in the global ecosystem.

Graphical abstract

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

Similar content being viewed by others

References

  • Abdelhafez AA, Li J-H (2016) Removal of Pb(II) from aqueous solution by using biochars derived from sugar cane bagasse and orange peel. J Taiwan Inst Chem E 61:367–375

    Article  CAS  Google Scholar 

  • Ankley GT, Brooks BW, Huggett DB, Sumpter AJP (2007) Repeating history: pharmaceuticals in the environment. Environ Sci Technol 41(24):8211–8217

    Article  CAS  Google Scholar 

  • Boxall ABA, Kolpin DW, Hallingsørensen B, Tolls J (2003) Peer reviewed: are veterinary medicines causing environmental risks? Environ Sci Technol 37(15):286(A)

    Article  CAS  Google Scholar 

  • Brigante M, Pecini E, Avena M (2016) Magnetic mesoporous silica for water remediation: synthesis, characterization and application as adsorbent of molecules and ions of environmental concern. Microporous Mesoporous Mater 230:1–10

    Article  CAS  Google Scholar 

  • Buchberger WW (2011) Current approaches to trace analysis of pharmaceuticals and personal care products in the environment. J Chromatogr A 1218(4):603–618

    Article  CAS  Google Scholar 

  • Cadaval TRS, Dotto GL, Pinto LAA (2014) Equilibrium isotherms, thermodynamics, and kinetic studies for the adsorption of food azo dyes onto chitosan films. Chem Eng Commun 202(10):1316–1323. https://doi.org/10.1080/00986445.2014.934449

    Article  CAS  Google Scholar 

  • Cao X, Ma L, Gao B, Harris W (2009) Dairy-manure derived biochar effectively sorbs lead and atrazine. Environ Sci Technol 43(9):3285–3291

    Article  CAS  Google Scholar 

  • Chandraiah MR (2016) Facile synthesis of zero valent iron magnetic biochar composites for Pb(II) removal from the aqueous medium. Alex Eng J 55(1):619–625

    Article  Google Scholar 

  • Chen B-L, Zhou D-D, Zhu L-Z (2008) Transitional adsorption and partition of nonpolar and polar aromatic contaminants by biochars of pine needles with different pyrolytic temperatures. Environ Sci Technol 42(14):5137–5143

    Article  CAS  Google Scholar 

  • Chen B-L, Chen Z-M, Lv S-F (2011) A novel magnetic biochar efficiently sorbs organic pollutants and phosphate. Bioresour Technol 102(2):716–723

    Article  CAS  Google Scholar 

  • Da’na E, Sayari A (2011) Adsorption of copper on amine-functionalized SBA-15 prepared by co-condensation: equilibrium properties. Chem Eng J 166(1):445–453

    Article  CAS  Google Scholar 

  • Dong L, Lin L, Li Q-Y, Huang Z, Tang X-Q, Wu M, Li C, Cao X-H, Scholz M (2018) Enhanced nitrate-nitrogen removal by modified attapulgite-supported nanoscale zero-valent iron treating simulated groundwater. J Environ Manag 213:151–158

    Article  CAS  Google Scholar 

  • Esfandiyari T, Nasirizadeh N, Ehrampoosh MH, Tabatabaee M (2017) Characterization and absorption studies of cationic dye on multi walled carbon nanotube–carbon ceramic composite. J Ind Eng Chem 46:35–43

    Article  CAS  Google Scholar 

  • Faheem YH, Liu J, Shen J-Y, Sun X-Y, Li J-S, Wang L-J (2016) Preparation of MnOx-loaded biochar for Pb2+ removal: adsorption performance and possible mechanism. J Taiwan Inst Chem E 66:313–320

    Article  CAS  Google Scholar 

  • Fan S-S, Wang Y, Wang Z, Tang J, Li X-D (2017) Removal of methylene blue from aqueous solution by sewage sludge-derived biochar: adsorption kinetics, equilibrium, thermodynamics and mechanism. J Environ Chem Eng 5(1):601–611

    Article  CAS  Google Scholar 

  • Gao J, Shi Y-Y, Zhou H-F, Ren X-Q, Ji H (2016) Application of modified attapulgite in phthalate acid ester-contaminated soil: effects on phthalate acid ester dissipation and the composition of soil microbial community. Environ Sci Pollut Res 23:15175–15182

    Article  CAS  Google Scholar 

  • Hao Y-M, Wang Z, Gou J-J, Dong S-Y (2015) Highly efficient adsorption and removal of Chrysoidine Y from aqueous solution by magnetic graphene oxide nanocomposite. Arab J Chem https://doi.org/10.1016/j.arabjc.2015.07.013

  • Huang P, Ge C, Feng D, Yu H, Luo J, Li J, Strong PJ, Sarmah AK, Bolan NS, Wang H (2018) Effects of metal ions and pH on ofloxacin sorption to cassava residue-derived biochar. Sci Total Environ 616–617:1384–1391

    Article  CAS  Google Scholar 

  • Jing X-R, Wang Y-Y, Liu W-J, Wang Y-K, Jiang H (2014) Enhanced adsorption performance of tetracycline in aqueous solutions by methanol-modified biochar. Chem Eng J 248:168–174

    Article  CAS  Google Scholar 

  • Kalderis D, Kayan B, Akay S, Kulaksız E, Gözmen B (2017) Adsorption of 2,4-dichlorophenol on paper sludge/wheat husk biochar: process optimization and comparison with biochars prepared from wood chips, sewage sludge and hog fuel/demolition waste. J Environ Chem Eng 5(3):2222–2231

    Article  CAS  Google Scholar 

  • Larsson DGJ, de PC, Paxeus N (2007) Effluent from drug manufactures contains extremely high levels of pharmaceuticals. J Hazard Mater 148(3):751–755

    Article  CAS  Google Scholar 

  • Li W-P, Lin J-C, Huang K (2014) Analysis about present status of global cauliflower production and its trade (in Chinese). China Veg 1(9):5–10

    Google Scholar 

  • Li X-L, Lu H-J, Zhang Y, He F, Jing L-Y, He X-H (2016) Fabrication of magnetic alginate beads with uniform dispersion of CoFe2O4 by the polydopamine surface functionalization for organic pollutants removal. Appl Surf Sci 389:567–577

    Article  CAS  Google Scholar 

  • Li H-Q, Hu J-T, Meng Y, Su J-H, Wang X-J (2017a) An investigation into the rapid removal of tetracycline using multilayered graphene-phase biochar derived from waste chicken feather. Sci Total Environ 603–604:39–48

    Article  CAS  Google Scholar 

  • Li X-L, Lu H-J, Zhang Y, He F (2017b) Efficient removal of organic pollutants from aqueous media using newly synthesized polypyrrole/CNTs-CoFe2O4 magnetic nanocomposites. Chem Eng J 316:893–902

    Article  CAS  Google Scholar 

  • Li Y, Wang Z-W, Xie X-Y, Zhu J-M, Li R-N, Qin T-T (2017c) Removal of norfloxacin from aqueous solution by clay-biochar composite prepared from potato stem and natural attapulgite. Colloids Surf A – Physicochem Eng Asp 514:126–136

    Article  CAS  Google Scholar 

  • Li Y-X, Pei G-P, Qiao X-L, Zhu Y, Li H (2018) Remediation of cadmium contaminated water and soil using vinegar residue biochar. Environ Sci Pollut Res 25:15754–15764

    Article  CAS  Google Scholar 

  • Liu W-J, Zeng F-X, Jiang H, Zhang X-S (2011) Preparation of high adsorption capacity bio-chars from waste biomass. Bioresour Technol 102:8247–8252

    Article  CAS  Google Scholar 

  • Liu P, Liu W-J, Jiang H, Chen J-J, Li W-W, Yu H-Q (2012) Modification of bio-char derived from fast pyrolysis of biomass and its application in removal of tetracycline from aqueous solution. Bioresour Technol 121:235–240

    Article  CAS  Google Scholar 

  • Liu Y, Zhang Z-H, Wang P, Dong Y-H (2016) Surface charge modification of chloromethylated polystyrene beads with NaH for the removal of sulfamonomethoxine. J Taiwan Inst Chem E 65:22–27

    Article  CAS  Google Scholar 

  • Mandal S, Sarkar B, Bolan N, Sik OY, Naidu R (2017) Enhancement of chromate reduction in soils by surface modified biochar. J Environ Manag 186:277–284

    Article  CAS  Google Scholar 

  • Milonjic S (2007) A consideration of the correct calculation of thermodynamic parameters of adsorption. J Serbian Chem Soc 72(12):1363–1367. https://doi.org/10.2298/jsc0712363m

    Article  CAS  Google Scholar 

  • Mohan D, Singh P, Sarswat A, Steele PH, Pittman CUJ (2015) Lead sorptive removal using magnetic and nonmagnetic fast pyrolysis energy cane biochars. J Colloid Interf Sci 448:238–250

    Article  CAS  Google Scholar 

  • Ocampo-Péreza R, Leyva-Ramosa R, Rivera-Utrillab J, Flores-Canob JV, Sánchez-Polo M (2015) Modeling adsorption rate of tetracyclines on activated carbons from aqueous phase. Chem Eng Res and Des 104:579–588

    Article  CAS  Google Scholar 

  • Oladipo AA, Ifebajo AO (2018) Highly efficient magnetic chicken bone biochar for removal of tetracycline and fluorescent dye from wastewater: two-stage adsorber analysis. J Environ Manag 209:9–16

    Article  CAS  Google Scholar 

  • Pavan FA, Lima EC, Dias SL, Mazzocato AC (2008) Methylene blue biosorption from aqueous solutions by yellow passion fruit waste. J Hazard Mater 150(3):703–712

    Article  CAS  Google Scholar 

  • Peng X, Hu X, Fu D, Lam FLY (2014) Adsorption removal of acid black 1 from aqueous solution using ordered mesoporous carbon. Appl Surf Sci 294:71–80

    Article  CAS  Google Scholar 

  • Pezoti O, Cazetta AL, Bedin KC, Souza LS, Martins AC, Silva TL, Santos Júnior OO, Visentainer JV, Almeida VC (2016) NaOH-activated carbon of high surface area produced from guava seeds as a high-efficiency adsorbent for amoxicillin removal: kinetic, isotherm and thermodynamic studies. Chem Eng J 288:778–788

    Article  CAS  Google Scholar 

  • Qin T-T, Wang Z-W, Xie X-Y, Xie C-R, Zhu J-M, Li Y (2017) A novel biochar derived from cauliflower (Brassica oleracea L.) roots could remove norfloxacin and chlortetracycline efficiently. Water Sci Technol 76(12):3307–3318

    Article  CAS  Google Scholar 

  • Reguyal F, Sarmah AK (2018) Adsorption of sulfamethoxazole by magnetic biochar: effects of pH, ionic strength, natural organic matter and 17α-ethinylestradiol. Sci Total Environ 628–629:722–730

    Article  CAS  Google Scholar 

  • Reguyal F, Sarmah AK, Gao W (2017) Synthesis of magnetic biochar from pine sawdust via oxidative hydrolysis of FeCl2 for the removal sulfamethoxazole from aqueous solution. J Hazard Mater 321:868–878

    Article  CAS  Google Scholar 

  • Saber-Samandari S, Joneidi-Yekta H, Mohseni M (2017) Adsorption of anionic and cationic dyes from aqueous solution using gelatin-based magnetic nanocomposite beads comprising carboxylic acid functionalized carbon nanotube. Chem Eng J 308:1133–1144

    Article  CAS  Google Scholar 

  • Sheikhmohammadi A, Mohseni SM, Khodadadi R, Sardar M, Abtahi M, Mahdavi S, Abtahi M, Mahdavi S, Keramati H, Dahaghin Z, Rezaei S, Almasian M, Sarkhosh M, Faraji M, Nazari S (2017) Application of graphene oxide modified with 8-hydroxyquinoline for the adsorption of Cr (VI) from wastewater: optimization, kinetic, thermodynamic and equilibrium studies. J Mol Liq 233:75–88

    Article  CAS  Google Scholar 

  • Sinegani AAS, Emtiazi G, Shariatmadari H (2005) Sorption and immobilization of cellulase on silicate clay minerals. J Colloid Interf Sci 290(1):39–44

    Article  CAS  Google Scholar 

  • Sun K, Ro K, Guo M-X, Novak J, Mashayekhi H, Xing B (2011) Sorption of bisphenol A, 17alpha-ethinyl estradiol and phenanthrene on thermally and hydrothermally produced biochars. Bioresour Technol 102(10):5757–5763

    Article  CAS  Google Scholar 

  • Sun Y-N, Gao B, Yao Y, Fang J, Zhang M, Zhou Y-M, Chen H, Yang L-Y (2014) Effects of feedstock type, production method, and pyrolysis temperature on biochar and hydrochar properties. Chem Eng J 240:574–578

    Article  CAS  Google Scholar 

  • Taheran M, Naghdi M, Brar SK, Knystautas EJ, Verma M, Ramirez AA, Surampalli RY, Valero JR (2016) Adsorption study of environmentally relevant concentrations of chlortetracycline on pinewood biochar. Sci Total Environ 571:772–777

    Article  CAS  Google Scholar 

  • Travlou NA, Kyzas GZ, Lazaridis NK, Deliyanni EA (2013) Graphite oxide/chitosan composite for reactive dye removal. Chem Eng J 217:256–265

    Article  CAS  Google Scholar 

  • Wang H-Y, Gao B, Wang S-S, Fang J, Xue Y-W, Yang K (2015) Removal of Pb(II), Cu(II), and Cd(II) from aqueous solutions by biochar derived from KMnO4 treated hickory wood. Bioresour Technol 197:356–362

    Article  CAS  Google Scholar 

  • Watkinson AJ, Murby EJ, Costanzo SD (2007) Removal of antibiotics in conventional and advanced wastewater treatment: implications for environmental discharge and wastewater recycling. Water Res 41(18):4164–4176

    Article  CAS  Google Scholar 

  • Wu C, Cui M-Q, Xue S-G, Li W-C, Huang L, Jiang X-X, Qian Z-Y (2018) Remediation of arsenic-contaminated paddy soil by iron-modified biochar. Environ Sci Pollut Res 25:20792–20801

    Article  CAS  Google Scholar 

  • Xu X-B, Hu X, Ding Z-H, Chen Y-J, Gao B (2017) Waste-art-paper biochar as an effective sorbent for recovery of aqueous Pb(II) into value-added PbO nanoparticles. Chem Eng J 308:863–871

    Article  CAS  Google Scholar 

  • Yang W-B, Lu Y-P, Zheng F-F, Xue X-X, Li N, Liu D-M (2012) Adsorption behavior and mechanisms of norfloxacin onto porous resins and carbon nanotube. Chem Eng J 179:112–118

    Article  CAS  Google Scholar 

  • Yao Z-Y, Wang L-H, Qi J-H (2009) Biosorption of methylene blue from aqueous solution using a bioenergy forest waste: Xanthoceras sorbifolia seed coat. CLEAN-Soil Air Water 37(8):642–648

    Article  CAS  Google Scholar 

  • Yao Y, Gao B, Inyang M, Zimmerman AR, Cao X-D, Pullammanappallil P, Yang L-Y (2011) Biochar derived from anaerobically digested sugar beet tailings: characterization and phosphate removal potential. Bioresour Technol 102(10):6273–6278

    Article  CAS  Google Scholar 

  • Yao Y, Gao B, Fang J, Zhang M, Chen H, Zhou Y-M, Creamer AE, Sun Y-N, Yang L-Y (2014) Characterization and environmental applications of clay–biochar composites. Chem Eng J 242:136–143

    Article  CAS  Google Scholar 

  • Yargicoglu EN, Sadasivam BY, Reddy KR, Spokas K (2015) Physical and chemical characterization of waste wood derived biochars. Waste Manag 36:256–268

    Article  CAS  Google Scholar 

  • Yin Z-H, Liu Y-G, Liu S-B, Jiang L-H, Tan X-F, Zeng G-M, Li M-F, Liu S-J, Tian S-R, Fang Y (2018) Activated magnetic biochar by one-step synthesis: enhanced adsorption and coadsorption for 17β-estradiol and copper. Sci Total Environ 639:1530–1542

    Article  CAS  Google Scholar 

  • Yu F, Chen J-H, Chen L, Huai J, Gong W-Y, Yuan Z-W, Wang J-H, Ma J (2012) Magnetic carbon nanotubes synthesis by Fenton's reagent method and their potential application for removal of azo dye from aqueous solution. J Colloid Interf Sci 378(1):175–183

    Article  CAS  Google Scholar 

  • Yu F, Li Y, Han S, Ma J (2016) Adsorptive removal of antibiotics from aqueous solution using carbon materials. Chemosphere 153:365–385

    Article  CAS  Google Scholar 

Download references

Funding

This work was supported by Gansu Natural Science Fund, China (17JR5RA218), and the Fundamental Research Funds for the Central Universities at Lanzhou University (lzujbky-2017-212).

Author information

Authors and Affiliations

  1. Gansu Key Laboratory for Environmental Pollution Prediction and Control, College of Earth and Environmental Sciences, Lanzhou University, Lanzhou, 730000, China

    Zhaowei Wang, Xing Yang, Tingting Qin, Guiwei Liang, Yan Li & Xiaoyun Xie

Authors
  1. Zhaowei Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Xing Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Tingting Qin
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Guiwei Liang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Yan Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Xiaoyun Xie
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Zhaowei Wang.

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.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Wang, Z., Yang, X., Qin, T. et al. Efficient removal of oxytetracycline from aqueous solution by a novel magnetic clay–biochar composite using natural attapulgite and cauliflower leaves. Environ Sci Pollut Res 26, 7463–7475 (2019). https://doi.org/10.1007/s11356-019-04172-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-019-04172-8

Keywords

Search

Navigation