Antibiotics Removal via Novel N-Doped Carbon Derived from Carbonization of Different Forms of Polyaniline
Publication: Journal of Hazardous, Toxic, and Radioactive Waste
Volume 27, Issue 3
Abstract
N-doped carbon (CP) was synthesized through carbonization of a polyaniline (PANI) prepared using interfacial polymerization. Different forms of PANI, such as emeraldine salt (ES), emeraldine base (EB), and aniline oligomers, were carbonized at different temperatures (700°C–1,000°C) in the presence of the N2 atmosphere to form CPs (CP7–CP10). CP prepared under different conditions was applied as adsorbent for antibiotics. It was observed that ES-PANI carbonized at 1,000°C formed graphitic N-doped carbon (CP10) and showed better adsorption of metronidazole (MET) compared with other CPs. The adsorption results showed that CP10 derived from the ES-form of PANI (PA1) achieved ∼97% MET removal within 5 min following pseudo-second-order kinetics (k = 0.347 g mg−1 min−1). CP10 has a high specific surface area (Sa) of 800.65 m2 g−1 and high graphitic nitrogen content (52.26% of total N) responsible for the rapid adsorption of the antibiotics through π-π electron acceptor-donor interaction, hydrogen bonding, and electrostatic attraction. In addition, CP10 has an adsorption capacity of 200.8 mg g−1 for MET. The highest activity of CP10 was due to high graphitic nitrogen content and high Sa. However, CPs formed from EB-PANI and aniline oligomers did not perform efficiently due to low Sa and graphitic nitrogen content. Similarly, CP10 applied for the adsorption of the ciprofloxacin (CIP) and tetracycline (TET) achieved maximum adsorption capacity of 344.8 and 263.2 mg g−1, respectively. Therefore, CP10 is a promising adsorbent for removing emerging pollutants from an aqueous solution.
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Data Availability Statement
All data, models, or code that support the findings of this study are available from the corresponding author upon reasonable request.
Acknowledgments
Authors wish to thank Ministry of Human Resource Development (MHRD), India, for providing funding to execute this research work (SB22230187CEPMRF008671).
References
Aarab, N., A. Hsini, A. Essekri, M. Laabd, R. Lakhmiri, and A. Albourine. 2020. “Removal of an emerging pharmaceutical pollutant (metronidazole) using PPY-PANi copolymer: Kinetics, equilibrium and DFT identification of adsorption mechanism.” Groundwater Sustainable Dev. 11: 100416. https://doi.org/10.1016/j.gsd.2020.100416.
Ahmed, M. J., and S. K. Theydan. 2013. “Microwave assisted preparation of microporous activated carbon from Siris seed pods for adsorption of metronidazole antibiotic.” Chem. Eng. J. 214: 310–318. https://doi.org/10.1016/j.cej.2012.10.101.
Anumol, T., A. Vijayanandan, M. Park, L. Philip, and S. A. Snyder. 2016. “Occurrence and fate of emerging trace organic chemicals in wastewater plants in Chennai, India.” Environ. Int. 92–93: 33–42. https://doi.org/10.1016/j.envint.2016.03.022.
Balakrishna, K., A. Rath, Y. Praveen Kumar Reddy, and K. Siri. 2017. “A review of the occurrence of pharmaceuticals and personal care products in Indian water bodies.” Ecotoxicol. Environ. Saf. 137: 113–120. https://doi.org/10.1016/j.ecoenv.2016.11.014.
Bonyadi, Z., F. Noghani, A. Dehghan, J. P. van der Hoek, D. A. Giannakoudakis, S. K. Ghadiri, I. Anastopoulos, M. Sarkhosh, J. Colmenares, and M. Shams. 2021. “Biomass-derived porous aminated graphitic nanosheets for removal of the pharmaceutical metronidazole: Optimization of physicochemical features and exploration of process mechanisms.” Colloids Surf., A 611: 125791. https://doi.org/10.1016/j.colsurfa.2020.125791.
Carrales-Alvarado, D. H., I. Rodríguez-Ramos, R. Leyva-Ramos, E. Mendoza-Mendoza, and D. E. Villela-Martínez. 2020. “Effect of surface area and physical–chemical properties of graphite and graphene-based materials on their adsorption capacity towards metronidazole and trimethoprim antibiotics in aqueous solution.” Chem. Eng. J. 402: 126155. https://doi.org/10.1016/j.cej.2020.126155.
Díaz-Blancas, V., R. Ocampo-Pérez, R. Leyva-Ramos, P. A. Alonso-Dávila, and A. I. Moral-Rodríguez. 2018. “3D modeling of the overall adsorption rate of metronidazole on granular activated carbon at low and high concentrations in aqueous solution.” Chem. Eng. J. 349: 82–91. https://doi.org/10.1016/j.cej.2018.05.076.
Ekande, O. S., and M. Kumar. 2021a. “Facile synthesis of graphitic carbon nitride from acetic acid pretreatment to activate persulfate in presence of blue light for photocatalytic removal of metronidazole.” Chemosphere 276: 130171. https://doi.org/10.1016/j.chemosphere.2021.130171.
Ekande, O. S., and M. Kumar. 2021b. “Review on polyaniline as reductive photocatalyst for the construction of the visible light active heterojunction for the generation of reactive oxygen species.” J. Environ. Chem. Eng. 9 (4): 105725. https://doi.org/10.1016/j.jece.2021.105725.
Fick, J., H. Soderstrom, R. Lindberg, C. Phan, and D. Larsson. 2009. “Contamination of surface, ground, and drinking water from pharmaceutical production.” Environ. Toxicol. Chem. 28 (12): 2522–2527. https://doi.org/10.1897/09-0731.
Gao, Y., Z. Chen, Y. Zhu, T. Li, and C. Hu. 2019. “New insights into the generation of singlet oxygen in the metal-free peroxymonosulfate activation process: Important role of electron-deficient carbon atoms.” Environ. Sci. Technol. 54 (2): 1232–1241. https://doi.org/10.1021/acs.est.9b05856.
Gao, Y., J. Ying, X. Xu, and L. Cai. 2018. “Nitrogen-enriched carbon nanofibers derived from polyaniline and their capacitive properties.” Appl. Sci. 8 (7): 1079. https://doi.org/10.3390/app8071079.
Golba, S., M. Popczyk, S. Miga, J. Jurek-Suliga, M. Zubko, J. Kubisztal, and K. Balin. 2020. “Impact of acidity profile on nascent polyaniline in the modified rapid mixing process—Material electrical conductivity and morphological study.” Materials 13 (22): 5108. https://doi.org/10.3390/ma13225108.
Hamadeen, H. M., and E. A. Elkhatib. 2022. “New nanostructured activated biochar for effective removal of antibiotic ciprofloxacin from wastewater: Adsorption dynamics and mechanisms.” Environ. Res. 210: 112929. https://doi.org/10.1016/j.envres.2022.112929.
Liu, S., Z. Zhang, F. Huang, Y. Liu, L. Feng, J. Jiang, L. Zhang, F. Qi, and C. Liu. 2021. “Carbonized polyaniline activated peroxymonosulfate (PMS) for phenol degradation: Role of PMS adsorption and singlet oxygen generation.” Appl. Catal., B 286: 119921. https://doi.org/10.1016/j.apcatb.2021.119921.
Manjunath, S. V., R. S. Baghel, and M. Kumar. 2020. “Antagonistic and synergistic analysis of antibiotic adsorption on Prosopis juliflora activated carbon in multicomponent systems.” Chem. Eng. J. 381: 122713. https://doi.org/10.1016/j.cej.2019.122713.
Manjunath, S. V., and M. Kumar. 2018. “Evaluation of single-component and multi-component adsorption of metronidazole, phosphate and nitrate on activated carbon from Prosopıs julıflora.” Chem. Eng J. 346: 525–534. https://doi.org/10.1016/j.cej.2018.04.013.
Mirzaei, A., Z. Chen, F. Haghighat, and L. Yerushalmi. 2017. “Removal of pharmaceuticals from water by homo/heterogonous Fenton-type processes–A review.” Chemosphere 174: 665–688. https://doi.org/10.1016/j.chemosphere.2017.02.019.
Morávková, Z., M. Trchová, E. Tomsik, A. Zhigunov, and J. Stejskal. 2013. “Transformation of oligoaniline microspheres to platelike nitrogen-containing carbon.” J. Phys. Chem. C 117 (5): 2289–2299. https://doi.org/10.1021/jp306783m.
Mukherjee, S., H. Ramireddy, A. Baidya, A. K. Amala, C. Sudhakar, B. Mondal, L. Philip, and T. Pradeep. 2019. “Nanocellulose-reinforced organo-inorganic nanocomposite for synergistic and affordable defluoridation of water and an evaluation of its sustainability metrics.” ACS Sustainable Chem. Eng. 8 (1): 139–147. https://doi.org/10.1021/acssuschemeng.9b04822.
Peñafiel, M. E., J. M. Matesanz, E. Vanegas, D. Bermejo, R. Mosteo, and M. P. Ormad. 2021. “Comparative adsorption of ciprofloxacin on sugarcane bagasse from Ecuador and on commercial powdered activated carbon.” Sci. Total Environ. 750: 141498. https://doi.org/10.1016/j.scitotenv.2020.141498.
Rozlivkova, Z., M. Trchova, M. Exnerova, and J. Stejskal. 2011. “The carbonization of granular polyaniline to produce nitrogen-containing carbon.” Synth. Met. 161 (11–12): 1122–1129. https://doi.org/10.1016/j.synthmet.2011.03.034.
Samadi, A., M. Xie, J. Li, H. Shon, C. Zheng, and S. Zhao. 2021. “Polyaniline-based adsorbents for aqueous pollutants removal: A review.” Chem. Eng. J. 418: 129425. https://doi.org/10.1016/j.cej.2021.129425.
Stejskal, J., and M. Trchova. 2012. “Aniline oligomers versus polyaniline.” Polym. Int. 61 (2): 240–251. https://doi.org/10.1002/pi.3179.
Sun, M., X. Wang, L. R. Winter, Y. Zhao, W. Ma, T. Hedtke, J. Kim, and M. Elimelech. 2021. “Electrified membranes for water treatment applications.” ACS ES&T Eng. 1 (4): 725–752. https://doi.org/10.1021/acsestengg.1c00015.
Sun, Z., L. Zhao, C. Liu, Y. Zhen, and J. Ma. 2020. “Fast adsorption of BPA with high capacity based on π-π electron donor-acceptor and hydrophobicity mechanism using an in-situ sp2 C dominant N-doped carbon.” Chem. Eng. J. 381: 122510. https://doi.org/10.1016/j.cej.2019.122510.
Talha, K., B. Wang, J. H. Liu, R. Ullah, F. Feng, J. Yu, S. Chen, and J. R. Li. 2020. “Effective adsorption of metronidazole antibiotic from water with a stable Zr (IV)-MOFs: Insights from DFT, kinetics and thermodynamics studies.” J. Environ. Chem. Eng. 8 (1): 103642. https://doi.org/10.1016/j.jece.2019.103642.
Tang, S. J., A. T. Wang, S. Y. Lin, K. Y. Huang, C. C. Yang, J. M. Yeh, and K. C. Chiu. 2011. “Polymerization of aniline under various concentrations of APS and HCl.” Polym. J. 43 (8): 667–675. https://doi.org/10.1038/pj.2011.43.
Tong, Y., P. J. McNamara, and B. K. Mayer. 2019. “Adsorption of organic micropollutants onto biochar: A review of relevant kinetics, mechanisms and equilibrium.” Environ. Sci. Water Res. Technol. 5 (5): 821–838. https://doi.org/10.1039/C8EW00938D.
Verlicchi, P., M. Al Aukidy, and E. Zambello. 2012. “Occurrence of pharmaceutical compounds in urban wastewater: Removal, mass load and environmental risk after a secondary treatment—A review.” Sci. Total Environ. 429: 123–155. https://doi.org/10.1016/j.scitotenv.2012.04.028.
Wang, J., and B. Chen. 2015. “Adsorption and co-adsorption of organic pollutants and a heavy metal by graphene oxide and reduced graphene materials.” Chem. Eng. J. 281: 379–388. https://doi.org/10.1016/j.cej.2015.06.102.
Wang, L., Y. Li, Y. Wang, W. Kong, Q. Lu, X. Liu, D. Zhang, and L. Qu. 2019. “Chlorine-doped graphene quantum dots with enhanced anti-and pro-oxidant properties.” ACS Appl. Mater. Interfaces 11 (24): 21822–21829. https://doi.org/10.1021/acsami.9b03194.
Yuan, D. S., T. X. Zhou, S. L. Zhou, W. J. Zou, S. S. Mo, and N. N. Xia. 2011. “Nitrogen-enriched carbon nanowires from the direct carbonization of polyaniline nanowires and its electrochemical properties.” Electrochem. Commun. 13 (3): 242–246. https://doi.org/10.1016/j.elecom.2010.12.023.
Zhang, X., Y. Li, M. Wu, Y. Pang, Z. Hao, M. Hu, R. Qiu, and Z. Chen. 2021. “Enhanced adsorption of tetracycline by an iron and manganese oxides loaded biochar: Kinetics, mechanism and column adsorption.” Bioresour. Technol. 320: 124264. https://doi.org/10.1016/j.biortech.2020.124264.
Zou, Y., X. Chen, W. Guo, X. Liu, and Y. Li. 2020. “Flexible and robust polyaniline composites for highly efficient and durable solar desalination.” ACS Appl. Energy Mater. 3 (3): 2634–2642. https://doi.org/10.1021/acsaem.9b02341.
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Received: Oct 10, 2022
Accepted: Jan 7, 2023
Published online: Mar 21, 2023
Published in print: Jul 1, 2023
Discussion open until: Aug 21, 2023
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