Skip to main content
Log in

Adsorption of an emerging contaminant (primidone) onto activated carbon: kinetic, equilibrium, thermodynamic, and optimization studies

  • Published:
Environmental Monitoring and Assessment Aims and scope Submit manuscript

Abstract

The current study addresses the removal of an emerging environmental contaminant (primidone) in batch adsorption experiments using commercial-grade powdered activated charcoal (PAC). The experiments for the removal of primidone were performed to identify the effect of various adsorption parameters. The second-order rate expression best represented the adsorption kinetics data. The Freundlich isotherm equation was best fitted to the experimental adsorption data at equilibrium for removal of primidone using PAC. The values for change in entropy (ΔSo) were positive, which indicates that the degree of freedom of the process increases. The negative values of change in enthalpy (ΔHo) and change in Gibb’s free energy (ΔGo) indicate that the physical adsorption is a dominant phenomenon, and the process is feasible and spontaneous. The negative value of ΔHo also represented the exothermicity of the adsorption process. The Taguchi optimization technique calculated the influence of variation of different process parameters, viz., initial pH (pH0), PAC dosage (m), initial adsorbate concentration (C0), solution temperature (T), and process contact time (t), on the removal of primidone by adsorption from aqueous solution. Each of the above parameters was examined at three levels to study their effects on the adsorptive uptake of primidone using PAC (qe, mg g−1), and the optimum value necessary to maximize qe was determined. The findings from the ANOVA indicate that the PAC dose (m) is the most notable parameter contributing 62.16% to qe and a 71.96% to the signal to noise (S/N) ratio data, respectively. The confirmation experiments performed at the optimum parameter condition validated the applicability of the Taguchi design of experiments. The percent removal and adsorptive uptake at the optimal condition were 86.11% and 0.258 mg g−1, respectively.

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

Access this article

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

Instant access to the full article PDF.

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

Similar content being viewed by others

References

  • Alagumurthi, N., Palaniradja, K., & Soundararajan, V. (2006). Optimization of grinding process through design of experiment (DOE)—a comparative study. Materials and Manufacturing Processes, 21(1), 19–21.

    Article  CAS  Google Scholar 

  • Alkhamis, K. A., & Wurster, D. E. (2002). Prediction of adsorption from multicomponent solutions by activated carbon using single-solute parameters. Part II—Proposed equation. AAPS PharmSciTech, 3(3), 53–60.

    Article  Google Scholar 

  • Altmann, J., Massa, L., Sperlich, A., Gnirss, R., & Jekel, M. (2016). UV254 absorbance as real-time monitoring and control parameter for micropollutant removal in advanced wastewater treatment with powdered activated carbon. Water research, 94, 240-245

  • Altmann, J., Ruhl, A. S., Zietzschmann, F., & Jekel, M. (2014). Direct comparison of ozonation and adsorption onto powdered activated carbon for micropollutant removal in advanced wastewater treatment. Water Research, 55, 185–193.

  • Amin, N. K. (2009). Removal of direct blue-106 dye from aqueous solution using new activated carbons developed from pomegranate peel: adsorption equilibrium and kinetics. Journal of Hazardous Materials, 165(1–3), 52–62.

    Article  CAS  Google Scholar 

  • Antony, J., Perry, D., Wang, C., & Kumar, M. (2006). An application of Taguchi method of experimental design for new product design and development process. Assembly Automation, 26(1), 18–24.

    Article  Google Scholar 

  • Appa, R., Mhaisalkar, V. A., Bafana, A., Devi, S. S., Krishnamurthi, K., Chakrabarti, T., & Naoghare, P. K. (2018). Simultaneous quantitative monitoring of four indicator contaminants of emerging concern (CEC) in different water sources of Central India using SPE/LC-(ESI) MS-MS. Environmental Monitoring and Assessment, 190(8), 489.

    Article  Google Scholar 

  • Arya, V., & Philip, L. (2017). Removal of pharmaceuticals from water using adsorption. In Trends in Asian Water Environmental Science and Technology (pp. 105–114). Cham: Springer.

    Chapter  Google Scholar 

  • Banerjee, S., & Chattopadhyaya, M. C. (2017). Adsorption characteristics for the removal of a toxic dye, tartrazine from aqueous solutions by a low cost agricultural by-product. Arabian Journal of Chemistry, 10, S1629–S1638.

    Article  CAS  Google Scholar 

  • Beardall, J. (2015). The fate of pharmaceuticals and personal care products in conventional and engineered on-site wastewater drain fields. Logan: Utah State University.

    Google Scholar 

  • Chen, F., Ying, G. G., Kong, L. X., Wang, L., Zhao, J. L., Zhou, L. J., & Zhang, L. J. (2011). Distribution and accumulation of endocrine-disrupting chemicals and pharmaceuticals in wastewater irrigated soils in Hebei, China. Environmental Pollution, 159(6), 1490–1498.

    Article  CAS  Google Scholar 

  • Cizmas, L., Sharma, V. K., Gray, C. M., & McDonald, T. J. (2015). Pharmaceuticals and personal care products in waters: occurrence, toxicity, and risk. Environmental Chemistry Letters, 13(4), 381–394.

    Article  CAS  Google Scholar 

  • Dos Santos, J. L., Chelucci, R., Chiquetto, R., Chung, M. C., Campos, M. L., & Peccinini, R. G. (2010). Synthesis, characterization and pharmacological evaluation of 1-(2-Chloro-6-Fluorophenyl)-5-Methylindolin-2-One: A new anti-inflammatory compound with reduced gastric ulceration properties.Molecules, 15(11), 8039–8047

  • Freundlich, H. M. F. (1906). Over the adsorption in solution. The Journal of Physical Chemistry, 57(385471), 1100–1107.

    Google Scholar 

  • Grassi, M., Kaykioglu, G., Belgiorno, V., & Lofrano, G. (2012). Removal of emerging contaminants from water and wastewater by adsorption process. In Emerging compounds removal from wastewater (pp. 15–37). Dordrecht: Springer.

    Chapter  Google Scholar 

  • Guo, Y. C., & Krasner, S. W. (2009). Occurrence of primidone, carbamazepine, caffeine, and precursors for N-nitrosodimethylamine in drinking water sources impacted by wastewater. JAWRA Journal of the American Water Resources Association, 45(1), 58–67.

    Article  CAS  Google Scholar 

  • Gupta, T.B., & Lataye, D. H. (2018) Adsorption of indigo carmine and methylene blue dye: Taguchi’s design of experiment to optimize removal efficiency, Sadhana, Academy Proceedings in Engineering Sciences, Springer (Manuscript accepted for publication).

  • Ho, Y. S., & McKay, G. (1999). Pseudo-second order model for sorption processes. Process Biochemistry, 34(5), 451–465.

    Article  CAS  Google Scholar 

  • Huber, M. M., Canonica, S., Park, G. Y., & Von Gunten, U. (2003). Oxidation of pharmaceuticals during ozonation and advanced oxidation processes. Environmental science & technology, 37(5), 1016–1024.

  • Hughes, S. R., Kay, P., & Brown, L. E. (2012). Global synthesis and critical evaluation of pharmaceutical data sets collected from river systems. Environmental Science & Technology, 47(2), 661–677.

    Article  Google Scholar 

  • Ikehata, K., JodeiriNaghashkar, N., & Gamal El-Din, M. (2006). Degradation of aqueous pharmaceuticals by ozonation and advanced oxidation processes: a review. Ozone: Science and Engineering, 28(6), 353–414.

    Article  CAS  Google Scholar 

  • Jelic, A., Gros, M., Ginebreda, A., Cespedes-Sánchez, R., Ventura, F., Petrovic, M., & Barcelo, D. (2011). Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment. Water Research, 45(3), 1165–1176.

    Article  CAS  Google Scholar 

  • Jodeh, S., Abdelwahab, F., Jaradat, N., Warad, I., & Jodeh, W. (2016). Adsorption of diclofenac from aqueous solution using Cyclamen persicum tubers based activated carbon (CTAC). Journal of the Association of Arab Universities for Basic and Applied Sciences, 20, 32–38.

    Article  Google Scholar 

  • Kandar, M. M., & Akil, H. M. (2016). Application of design of experiment (DoE) for parameters optimization in compression moulding for flax reinforced biocomposites. Procedia Chemistry, 19, 433–440.

  • Kårelid, V. (2016). Towards application of activated carbon treatment for pharmaceutical removal in municipal wastewater(Doctoral dissertation, KTH Royal Institute of Technology).

  • Kass, R. E. (1990). Nonlinear regression analysis and its applications. Journal of the American Statistical Association, 85(410), 594–596.

    Article  Google Scholar 

  • Korzh, E. A., Smolin, S. K., & Klymenko, N. A. (2016). Kinetics of adsorption of pharmaceutical substances from aqueous solutions on activated carbons. Journal of Water Chemistry and Technology, 38(4), 187–193.

    Article  Google Scholar 

  • Lagergren, S. (1898). Zur theorie der sogenannten adsorption geloster stoffe. Kungliga svenska vetenskapsakademiens. Handlingar, 24, 1–39.

  • Lakshmi, U. R., Srivastava, V. C., Mall, I. D., & Lataye, D. H. (2009). Rice husk ash as an effective adsorbent: Evaluation of adsorptive characteristics for indigo carmine dye. Journal of Environmental Management, 90(2), 710–720.

    Article  CAS  Google Scholar 

  • Langmuir, I. (1918). The adsorption of gases on plane surfaces of glass, mica and platinum. Journal of the American Chemical Society, 40(9), 1361–1403.

    Article  CAS  Google Scholar 

  • Lataye, D. H., Mishra, I. M., & Mall, I. D. (2006). Removal of pyridine from aqueous solution by adsorption on bagasse fly ash. Industrial & Engineering Chemistry Research, 45(11), 3934–3943.

    Article  CAS  Google Scholar 

  • Lataye, D. H., Mishra, I. M., & Mall, I. D. (2008). Multicomponent sorptive removal of toxics pyridine, 2-picoline, and 4-picoline from aqueous solution by bagasse fly ash: optimization of process parameters. Industrial & Engineering Chemistry Research, 47(15), 5629–5635.

    Article  CAS  Google Scholar 

  • Lataye, D. H., Mishra, I. M., & Mall, I. D. (2009a). Adsorption of α-picoline onto rice husk ash and granular activated carbon from aqueous solution: equilibrium and thermodynamic study. Chemical Engineering Journal, 147(2–3), 139–149.

    Article  CAS  Google Scholar 

  • Lataye, D. H., Mishra, I. M., & Mall, I. D. (2009b). Multicomponent sorption of pyridine and its derivatives from aqueous solution onto rice husk ash and granular activated carbon. Practice Periodical of Hazardous, Toxic, and Radioactive Waste Management, 13(4), 218–228.

    Article  CAS  Google Scholar 

  • Lataye, D. H., Mishra, I. M., & Mall, I. D. (2009c). Adsorption of α-picoline onto rice husk ash and granular activated carbon from aqueous solution: equilibrium and thermodynamic study. Chemical Engineering Journal, 147(2–3), 139–149.

    Article  CAS  Google Scholar 

  • Macdonald, R. L., & Kelly, K. M. (1995). Antiepileptic drug mechanisms of action. Epilepsia, 36(s2), S2–S12.

    Article  CAS  Google Scholar 

  • Maheshwari, M., Vyas, R. K., & Sharma, M. (2013). Kinetics, equilibrium and thermodynamics of ciprofloxacin hydrochloride removal by adsorption on coal fly ash and activated alumina. Desalination and Water Treatment, 51(37–39), 7241–7254.

    Article  CAS  Google Scholar 

  • Maiti, M., Srivastava, V. K., Shewale, S., Jasra, R. V., Chavda, A., & Modi, S. (2014). Process parameter optimization through design of experiments in synthesis of high cis-polybutadiene rubber. Chemical Engineering Science, 107, 256–265.

    Article  CAS  Google Scholar 

  • Mohammadi, N., Khani, H., Gupta, V. K., Amereh, E., & Agarwal, S. (2011). Adsorption process of methyl orange dye onto mesoporous carbon material–kinetic and thermodynamic studies. Journal of Colloid and Interface Science, 362(2), 457–462.

    Article  CAS  Google Scholar 

  • Montgomery, D. C., Peck, E. A., & Vining, G. G. (2012). Introduction to linear regression analysis (Vol. 821). Hoboken: John Wiley & Sons.

    Google Scholar 

  • National Center for Biotechnology Information. PubChem Compound Database; CID=4909. (n.d.). https://pubchem.ncbi.nlm.nih.gov/compound/4909. Accessed 14 Feb 2019

  • Pathak, P. D., Mandavgane, S. A., & Kulkarni, B. D. (2015). Fruit peel waste as a novel low-cost bio adsorbent. Reviews in Chemical Engineering, 31(4), 361–381.

    Article  CAS  Google Scholar 

  • Pathania, D., Sharma, S., & Singh, P. (2017). Removal of methylene blue by adsorption onto activated carbon developed from Ficus carica bast. Arabian Journal of Chemistry, 10, S1445–S1451.

    Article  CAS  Google Scholar 

  • Rasoulifard, M. H., Khanmohammadi, S., & Heidari, A. (2016). Adsorption of cefixime from aqueous solutions using modified hardened paste of Portland cement by perlite; optimization by Taguchi method. Water Science and Technology, 74(5), 1069–1078.

    Article  CAS  Google Scholar 

  • Rehman, M. S. U., Rashid, N., Ashfaq, M., Saif, A., Ahmad, N., & Han, J. I. (2015). Global risk of pharmaceutical contamination from highly populated developing countries. Chemosphere, 138, 1045–1055.

    Article  CAS  Google Scholar 

  • Rivera-Utrilla, J., Ocampo-Perez, R., Sanchez-Polo, M., Lopez-Penalver, J. J., & Gomez-Pacheco, C. V. (2018). Removal of tetracyclines from water by adsorption/bioadsorption and advanced oxidation processes. A short review. Current Organic Chemistry, 22(10), 1005–1021.

    Article  CAS  Google Scholar 

  • Roy, R. K. (2001). Design of experiments using the Taguchi approach: 16 steps to product and process improvement. Hoboken: John Wiley & Sons.

    Google Scholar 

  • Satorra, A. (1988). Scaling corrections for chi-square statistics in covariance structure analysis. In American Statistical Association 1988 proceedings of business and economics sections (pp. 308–313). Boston: American Statistical Association.

    Google Scholar 

  • Sauvé, S., & Desrosiers, M. (2014). A review of what is an emerging contaminant. Chemistry Central Journal, 8(1), 15.

    Article  Google Scholar 

  • Schaffer, M., Boxberger, N., Börnick, H., Licha, T., & Worch, E. (2012). Sorption influenced transport of ionizable pharmaceuticals onto a natural sandy aquifer sediment at different pH. Chemosphere, 87(5), 513–520.

    Article  CAS  Google Scholar 

  • Sharma, P., Verma, A., Sidhu, R. K., & Pandey, O. P. (2005). Process parameter selection for strontium ferrite sintered magnets using Taguchi L9 orthogonal design. Journal of Materials Processing Technology, 168(1), 147–151.

    Article  CAS  Google Scholar 

  • Siddique, S., Kubwabo, C., & Harris, S. A. (2016). A review of the role of emerging environmental contaminants in the development of breast cancer in women. Emerging Contaminants, 2(4), 204–219.

    Article  Google Scholar 

  • Smith, J. M. (1950). Introduction to chemical engineering thermodynamics.

  • Srivastava, V. C., Swamy, M. M., Mall, I. D., Prasad, B., & Mishra, I. M. (2006). Adsorptive removal of phenol by bagasse fly ash and activated carbon: equilibrium, kinetics and thermodynamics. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 272(1–2), 89–104.

    Article  CAS  Google Scholar 

  • Srivastava, V. C., Mall, I. D., & Mishra, I. M. (2008). Optimization of parameters for adsorption of metal ions onto rice husk ash using Taguchi’s experimental design methodology. Chemical Engineering Journal, 140(1–3), 136–144.

    Article  CAS  Google Scholar 

  • Taguchi, G., & Wu, Y. (1979). Introduction to off-line quality control, Central Japan Quality Control Association, Meieki Nakamura-Ku Magaya, Japan.

  • Ternes, T. A., Meisenheimer, M., McDowell, D., Sacher, F., Brauch, H. J., Haist-Gulde, B., et al. (2002). Removal of pharmaceuticals during drinking water treatment. Environmental Science & Technology, 36(17), 3855–3863.

    Article  CAS  Google Scholar 

  • Trenholm, R. A., Vanderford, B. J., & Snyder, S. A. (2009). On-line solid phase extraction LC–MS/MS analysis of pharmaceutical indicators in water: a green alternative to conventional methods. Talanta, 79(5), 1425–1432.

    Article  CAS  Google Scholar 

  • Wurster, D. E., Alkhamis, K. A., & Matheson, L. E. (2000). Prediction of adsorption from multicomponent solutions by activated carbon using single-solute parameters. AAPS PharmSciTech, 1(3), 79–93.

    Article  Google Scholar 

  • Yang, X., Flowers, R. C., Weinberg, H. S., & Singer, P. C. (2011). Occurrence and removal of pharmaceuticals and personal care products (PPCPs) in an advanced wastewater reclamation plant. Water Research, 45(16), 5218–5228.

    Article  CAS  Google Scholar 

  • Yang, B., Ying, G. G., Zhao, J. L., Liu, S., Zhou, L. J., & Chen, F. (2012). Removal of selected endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) during ferrate (VI) treatment of secondary wastewater effluents. Water Research, 46(7), 2194–2204.

    Article  CAS  Google Scholar 

  • Zuim, D. R., Carpiné, D., Distler, G. A. R., de Paula Scheer, A., Igarashi-Mafra, L., & Mafra, M. R. (2011). Adsorption of two coffee aromas from synthetic aqueous solution onto granular activated carbon derived from coconut husks. Journal of Food Engineering, 104(2), 284–292.

    Article  CAS  Google Scholar 

  • Zupanc, M., Kosjek, T., Petkovšek, M., Dular, M., Kompare, B., Širok, B., et al. (2013). Removal of pharmaceuticals from wastewater by biological processes, hydrodynamic cavitation and UV treatment. Ultrasonics Sonochemistry, 20(4), 1104–1112.

    Article  CAS  Google Scholar 

Download references

Funding

The authors are grateful to CSIR-NEERI, Nagpur, and VNIT, Nagpur, for facilitating financial aids and facilities (KRC no.: CSIR-NEERI/KRC/2018/AUG/EISD/3).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Pravin K. Naoghare.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

Additional information

Publisher’s note

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

Electronic supplementary material

ESM 1

(DOCX 17 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Appa, R., Mhaisalkar, V.A., Naoghare, P.K. et al. Adsorption of an emerging contaminant (primidone) onto activated carbon: kinetic, equilibrium, thermodynamic, and optimization studies. Environ Monit Assess 191, 215 (2019). https://doi.org/10.1007/s10661-019-7302-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s10661-019-7302-x

Keywords

Navigation