• WALEED K. ABDULSAHIB Pharmacology and Toxicology Department, College of Pharmacy, Al-Farahidi University, Baghdad, Iraq
  • SAFAA H. GANDUH Pharmacology and Toxicology Department, College of Pharmacy, University of Al-Qadisiyah, Al-Qadisiyah, Iraq
  • MAKARIM A. MAHDI Department of Chemistry, College of Education, University of Al-Qadisiyah, Al-Qadisiyah, Iraq
  • LAYTH S. JASIM Department of Chemistry, College of Education, University of Al-Qadisiyah, Al-Qadisiyah, Iraq



Doxycycline, Adsorption, Graphene oxide, Composite and removal


Objective: Preparation of novel, safe, and low-cost composite by addition of graphene oxide (GO) to polyvinylpyrrolidone-acrylic acid composite (PVP-AAc) to remove the doxycycline hydrochloride (D) from polluted aquatic environment.

Methods: Different concentrations of D were used to study the adsorption process of the antibiotic on the surface of GO/(PVP-AAc) hydrogel composite. The aquatic solution of D was used for studying the adsorption process through a series of different experiments to determine the contact time, adsorbate amount, appropriate temperature, the preferred pH, ionic strength, adsorption kinetics and isotherms on the adsorbent surface of GO/PVP-AAc composite. Fourier transform infrared (FT-IR) spectroscopy and Field-emission scanning electron microscopy (FE-SEM) were used to detect the structure, functional groups and surface morphology of the composite before and after D adsorption.

Results: Doxycycline is adsorb on the surface of GO/PVP-AAc hydrogel composite through by physical interactions. The adsorption kinetics correlated to the pseudo-second-order model, contact time studies of D equal to 180 min and the high R2 value of 0.98 indicates that Langmuir isotherm model better fitted to the data for the removal of D at 15 °C. The results of thermodynamic parameters show that the nature of the adsorption process is physical, exothermic, orderly and spontaneous. The adsorption capacity of D favors the acidic media. When NaCl is added to the solution, the adsorption capacity of D will increase.

Conclusion: Graphene oxide/PVP-AAc composite is a novel, worthy and efficient adsorbent for the removal of the doxycycline polluted the water because of its low cost, hydrophilic properties, large surface area and special structure that give impressive dispersible activity in aquatic solutions.


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Yu F, Li Y, Han S, Ma J. Adsorptive removal of antibiotics from aqueous solution using carbon materials. Chemosphere 2016;153:365–85.

Joshi M, Lata S, Kanwar P, Mishra T. Application of nanostructures in antimicrobial therapy. Int J Appl Pharm 2018;10:11–25.

Abdulsahib WK, Fadhil OQ, Abood SJ. Antimicrobial susceptibility pattern isolated from different clinical samples in Baghdad hospitals. J Adv Pharm Educ Res 2020;10:51-9.

Priya SS, Radha KV. Brief review of spectrophotometric methods for the detection of tetracycline antibiotics. Int J Pharm Pharm Sci 2014;6:48–51.

Wu L, Wang J, Zhang Y, Wang L, Ye J. Aquatic toxicity of antibiotic contaminant doxycycline hydrochloride on cyanobacterium microcystis aeruginosa. Asian J Water Environ Pollut 2014;11:45–50.

Palasuk J, Windsor LJ, Platt JA, Lvov Y, Geraldeli S, Bottino MC. Doxycycline-loaded nanotube-modified adhesives inhibit MMP in a dose-dependent fashion. Clin Oral Investig 2018;22:1243–52.

Hadjimichael AC, Foukas AF, Savvidou OD, Mavrogenis AF, Psyrri AK, Papagelopoulos PJ. The anti-neoplastic effect of doxycycline in osteosarcoma as a metalloproteinase (MMP) inhibitor: a systematic review. Clin Sarcoma Res 2020;10:1–10.

Redelsperger IM, Taldone T, Riedel ER, Lepherd ML, Lipman NS, Wolf FR. Stability of doxycycline in feed and water and minimal effective doses in tetracycline-inducible systems. J Am Assoc Lab Anim Sci 2016;55:467–74.

Zhang M, He LY, Liu YS, Zhao JL, Liu WR, Zhang JN, et al. Fate of veterinary antibiotics during animal manure composting. Sci Total Environ 2019;650:1363–70.

Liu Y, Guan Y, Gao B, Yue Q. Antioxidant responses and degradation of two antibiotic contaminants in Microcystis aeruginosa. Ecotoxicol Environ Saf 2012;86:23–30.

Yan Q, Li X, Ma B, Zou Y, Wang Y, Liao X, et al. Different concentrations of doxycycline in swine manure affect the microbiome and degradation of doxycycline residue in soil. Front Microbiol 2018;9:3129.

Jechalke S, Heuer H, Siemens J, Amelung W, Smalla K. Fate and effects of veterinary antibiotics in soil. Trends Microbiol 2014;22:536–45.

Blau K, Jacquiod S, Sørensen SJ, Su JQ, Zhu YG, Smalla K, et al. Manure and doxycycline affect the bacterial community and its resistome in lettuce rhizosphere and bulk soil. Front Microbiol 2019;10:725.

Yu F, Sun S, Han S, Zheng J, Ma J. Adsorption removal of ciprofloxacin by multi-walled carbon nanotubes with different oxygen contents from aqueous solutions. Chem Eng J 2016;285:588–95.

Atyaa AI, Radhy ND, Jasim LS. Synthesis and characterization of graphene oxide/hydrogel composites and their applications to adsorptive removal congo red from aqueous solution. In: Journal of Physics: Conference Series. IOP Publishing; 2019. p. 12095.

Ahmed MB, Zhou JL, Ngo HH, Guo W. Adsorptive removal of antibiotics from water and wastewater: progress and challenges. Sci Total Environ 2015;532:112–26.

Alnajrani MN, Alsager OA. Removal of antibiotics from water by the polymer of intrinsic microporosity: isotherms, kinetics, thermodynamics, and adsorption mechanism. Sci Rep 2020; 10:794.

Zeng ZW, Tan XF, Liu YG, Tian SR, Zeng GM, Jiang LH, et al. Comprehensive adsorption studies of doxycycline and ciprofloxacin antibiotics by biochars prepared at different temperatures. Front Chem 2018;6:80.

Rocher V, Bee A, Siaugue JM, Cabuil V. Dye removal from aqueous solution by magnetic alginate beads crosslinked with epichlorohydrin. J Hazard Mater 2010;178:434–9.

Lin S, Li Q, Zhong Y, Li J, Zhao X, Wang M, et al. Cross-linked double network graphene oxide/polymer composites for efficient coagulation-flocculation. Glob Challenges (Hoboken, NJ) 2020;4:1900051.

Zhu Y, Murali S, Cai W, Li X, Suk JW, Potts JR, et al. Graphene and graphene oxide: synthesis, properties, and applications. Adv Mater 2010;22:3906–24.

Fan L, Luo C, Sun M, Li X, Lu F, Qiu H. Preparation of novel magnetic chitosan/graphene oxide composite as effective adsorbents toward methylene blue. Bioresour Technol 2012;114:703–6.

Huang Y, Zeng M, Ren J, Wang J, Fan L, Xu Q. Preparation and swelling properties of graphene oxide/poly (acrylic acid-co-acrylamide) super-absorbent hydrogel nanocomposites. Colloids Surf A 2012;401:97–106.

Liu M, Li X, Du Y, Han R. Adsorption of methyl blue from solution using walnut shell and reuse in secondary adsorption for congo red. Bioresour Technol Reports 2019;5:238–42.

Priya SS, Radha K. Equilibrium, isotherm, kinetic and thermodynamic adsorption studies of tetracycline hydrochloride onto commercial-grade granular activated carbon. Int J Pharm Pharm Sci 2015;7:42–51.

Radhy ND, Jasim LS. Synthesis of graphene oxide/hydrogel composites and their ability for efficient adsorption of crystal violet. J Pharm Sci Res 2019;11:456–63.

Zhu H, Chen T, Liu J, Li D. Adsorption of tetracycline antibiotics from an aqueous solution onto graphene oxide/calcium alginate composite fibers. RSC Adv 2018;8:2616–21.

Tabatabai Yazdi F, Ebrahimian Pirbazari A, Esmaeili Khalilsaraei F, Asasian Kolur N, Gilani N. Photocatalytic treatment of tetracycline antibiotic wastewater by silver/TiO2 nanosheets/reduced graphene oxide and artificial neural network modeling. Water Environ Res 2020;92:662–76.

Rostamian R, Behnejad H. Insights into doxycycline adsorption onto graphene nanosheet: a combined quantum mechanics, thermodynamics, and kinetic study. Environ Sci Pollut Res 2018;25:2528–37.

Balarak D, Mostafapour FK, Azarpira H, Joghataei A. Langmuir, Freundlich, Temkin and Dubinin–radushkevich isotherms studies of equilibrium sorption of ampicilin unto montmorillonite nanoparticles. J Pharm Res Int 2017;20:1–9.

Abdulsahib WK, Ganduh SH, Radia ND, Jasim LS. New approach for sulfadiazine toxicity management using carboxymethyl cellulose grafted acrylamide hydrogel. Int J Drug Delivery Technol 2020;10:1–7.

Ali MMM, Ahmed MJ. Adsorption behavior of doxycycline antibiotic on NaY zeolite from wheat (Triticum aestivum) straws ash. J Taiwan Inst Chem Eng 2017;81:218–24.

Abbas RF, Hami HK, Mahdi NI. Removal of doxycycline hyclate by adsorption onto cobalt oxide at three different temperatures: isotherm, thermodynamic and error analysis. Int J Environ Sci Technol 2019;16:5439–46.

Brigante M, Avena M. Biotemplated synthesis of mesoporous silica for doxycycline removal. Effect of pH, temperature, ionic strength and Ca2+concentration on the adsorption behaviour. Microporous Mesoporous Mater 2016;225:534–42.

Hiew BYZ, Lee LY, Lee XJ, Thangalazhy Gopakumar S, Gan S, Lim SS, et al. Review on the synthesis of 3D graphene-based configurations and their adsorption performance for hazardous water pollutants. Process Saf Environ Prot 2018;116:262–86.

Li M, Liu C, Xie Y, Cao H, Zhao H, Zhang Y. The evolution of surface charge on graphene oxide during the reduction and its application in electroanalysis. Carbon NY 2014;66:302–11.

Gao Y, Li Y, Zhang L, Huang H, Hu J, Shah SM, et al. Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide. J Colloid Interface Sci 2012;368:540–6.



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