Abstract
Waters are often polluted by antibacterial drugs such as sulfonamides, which are widely used in animal husbandry, aquaculture and other sectors. Actual decontamination methods are limited, thus requiring the development of alternative treatments. Here, we hypothesized that a composite of biochar-supported Fe/Cu (FeCu-biochar) would activate persulfate to remove the antibiotic sulfapyridine from aqueous solutions using batch experiments. FeCu-biochar was characterized by scanning electron microscopy with energy-dispersive spectroscopy (SEM–EDS) and X-ray diffraction (XRD). We tested the effect of catalyst type, initial pH and reusability runs. Results show that, compared to Fe-biochar, 1 g/L FeCu-biochar activated 4 mM persulfate better, removing 97.6% of 20 mg/L sulfapyridine in 5 min at pH 8.2. Such enhancement is attributed to the strong oxidization of ·SO4−, the high catalytic ability of CuO and synergistic effects between Fe and Cu. The removal of sulfapyridine by FeCu-biochar was pH-dependent, and the best catalytic performance occurred in alkaline conditions. FeCu-biochar also displayed excellent stability, easy separation and good recyclability.
Similar content being viewed by others
References
Baran W, Adamek E, Ziemianska J, Sobczak A (2011) Effects of the presence of sulfonamides in the environment and their influence on human health. J Hazard Mater 196(1):1–15. https://doi.org/10.1016/J.JHAZMAT.2011.08.082
Barnes KK, Kolpin DW, Furlong ET, Zaugg SD (2008) A national reconnaissance of pharmaceuticals and other organic wastewater contaminants in the United States—(I) groundwater. Sci Total Environ 402:192–200. https://doi.org/10.1016/J.SCITOTENV.2008.04.028
Chen L, Li F, Wei YS, Li GG, Shen KX, He HJ (2019) High cadmium adsorption on nanoscale zero-valent iron coated Eichhornia crassipes biochar. Environ Chem Lett 17(1):589–594. https://doi.org/10.1007/S10311-018-0811-Y
Choi KJ, Son HJ, Kim SH (2007) Ionic treatment for removal of sulfonamide and tetracycline classes of antibiotic. Sci Total Environ 387(1):247–256. https://doi.org/10.1016/J.SCITOTENV.2007.07.024
Feng Y, Lee PH, Wu D, Shih K (2017) Surface-bound sulfate radical-dominated degradation of 1, 4-dioxane by alumina-supported palladium (Pd/Al2O3) catalyzed peroxymonosulfate. Water Res 120:12–21. https://doi.org/10.1016/J.WATRES.2017.04.070
Guan YH, Ma J, Ren YM, Liu YL, Xiao JY, Lin LQ, Zhang C (2013) Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals. Water Res 47(14):5431–5438. https://doi.org/10.1016/J.WATRES.2013.06.023
Guan CT, Jiang J, Luo CW, Pang SY, Yang Y, Wang Z, Ma J, Yu J, Zhao X (2018) Oxidation of bromophenols by carbon nanotube activated peroxymonosulfate (PMS) and formation of brominated products: comparison to peroxydisulfate (PDS). Chem Eng J 337:40–50. https://doi.org/10.1016/J.CEJ.2017.12.083
Ji YF, Shi YY, Wang L, Lu JH, Ferronato C, Chovelon J-M (2017) Sulfate radical-based oxidation of antibiotics sulfamethazine, sulfapyridine, sulfadiazine, sulfadimethoxine, and sulfachloropyridazine: formation of SO2 extrusion products and effects of natural organic matter. Sci Total Environ 593:704–712. https://doi.org/10.1016/J.SCITOTENV.2017.03.192
Kermani M, Mohammadi F, Kakavandi B, Esrafili A, Rostamifasih Z (2018) Simultaneous catalytic degradation of 2,4-D and MCPA herbicides using sulfate radical-based heterogeneous oxidation over persulfate activated by natural hematite (α-Fe2O3/PS). J Phys Chem Solids 117:49–59. https://doi.org/10.1016/J.JPCS.2018.02.009
Klasson KT, Ledbetter CA, Uchimiya M, Lima IM (2013) Activated biochar removes 100% dibromochloropropane from field well water. Environ Chem Lett 11(3):271–275. https://doi.org/10.1007/S10311-012-0398-7
Kummerer K (2009) Antibiotics in the aquatic environment: a review (part II). Chemosphere 75(4):435–441. https://doi.org/10.1016/j.chemosphere.2008.11.086
Li Z, Luo SX, Yang Y, Chen JW (2019) Highly efficient degradation of trichloroethylene in groundwater based on peroxymonosulfate activation by bentonite supported Fe/Ni bimetallic nanoparticle. Chemosphere 219:499–506. https://doi.org/10.1016/J.CHEMOSPHERE.2018.10.133
Li Z, Sun YQ, Yang Y, Han YT, Wang TS, Chen JW, Tsang CWD (2020a) Biochar-supported nanoscale zero-valent iron as an efficient catalyst for organic degradation in groundwater. J Hazard Mater. https://doi.org/10.1016/j.jhazmat.2019.121240
Li Z, Sun YQ, Yang Y, Han YT, Wang TS, Chen JW, Tsang CWD (2020b) Comparing biochar—and bentonite-supported Fe-based catalysts for selective degradation of antibiotics: mechanisms and pathway. Res Environ. https://doi.org/10.1016/j.envres.2020.109156
Liu H, Pu CJ, Yu XL, Sun Y, Chen JH (2018) Removal of tetracyclines, sulfonamides, and quinolones by industrial-scale composting and anaerobic digestion processes. Environ Sci Pollut Res 25(36):1–10. https://doi.org/10.1007/S11356-018-1487-3
Liu YY, Sohi Saran P, Liu SY, Guan JJ, Zhou JY, Chen JW (2019) Adsorption and reductive degradation of Cr(VI) and TCE by a simply synthesized zero valent iron magnetic biochar. J Environ Manage 235(2019):276–281. https://doi.org/10.1016/J.JENVMAN.2019.01.045
Ma J, Yang Y, Jiang X, Xie Z, Li X, Chen C, Chen H (2018) Impacts of inorganic anions and natural organic matter on thermally activated persulfate oxidation of BTEX in water. Chemosphere 190:296–306. https://doi.org/10.1016/J.CHEMOSPHERE.2017.09.148
Oh WD, Dong Z, Lim TT (2016) Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal: current development, challenges and prospects. Appl Catal B Environ 194:169–201. https://doi.org/10.1016/J.APCATB.2016.04.003
Ren YM, Dong Q, Feng J, Ma J, Wen Q, Zhang ML (2012) Magnetic porous ferrospinel NiFe2O4: a novel ozonation catalyst with strong catalytic property for degradation of di-n-butyl phthalate and convenient separation from water. J Colloid Interface Sci 382:90–96. https://doi.org/10.1016/J.JCIS.2012.05.053
Sahar E, David I, Gelman Y, Chikurel H, Aharoni A, Messalem R, Brenner A (2011) The use of RO to remove emerging micropollutants following CAS/UF or MBR treatment of municipal wastewater. Desalination 273(1):142–147. https://doi.org/10.1016/J.DESAL.2010.11.004
Shi HM, Ni J, Zheng TL, Wang XN, Wu CF, Wang QH (2020) Remediation of wastewater contaminated by antibiotics. A review. Environ Chem Lett 18(2):345–360. https://doi.org/10.1007/S10311-019-00945-2
Tian Y, Gao B, Morales VL, Chen H, Wang Y, Li H (2013) Removal of sulfamethoxazole and sulfapyridine by carbon nanotubes in fixed-bed columns. Chemosphere 90(10):2597–2605. https://doi.org/10.1016/J.CHEMOSPHERE.2012.11.010
Upadhyay RK, Waghmare PR (2020) Eco-friendly preparation of superhydrophobic copper surfaces for oil/water separation. Environ Chem Lett 18(2):505–510. https://doi.org/10.1007/s10311-019-00952-3
Verma P, Samanta SK (2018) Microwave-enhanced advanced oxidation processes for the degradation of dyes in water. Environ Chem Lett 16:969–1007. https://doi.org/10.1007/S10311-018-0739-2
Voigt M, Bartels I, Nickisch-Hartfiel A, Jaeger M (2017) Photo-induced degradation of sulfonamides, kinetic and structural characterization of transformation products, and assessment of environmental toxicity. Toxicol Environ Chem 99:1304–1327. https://doi.org/10.1080/02772248.2017.1373777
Yu YT, Li SQ, Peng XZ, Yang SJ, Zhu YF, Chen L, Wu F, Mailhot G (2016) Efficient oxidation of bisphenol A with oxysulfur radicals generated by iron-catalyzed autoxidation of sulfite at circumneutral pH under UV irradiation. Environ Chem Lett 14(4):527–532. https://doi.org/10.1007/S10311-016-0573-3
Zhang T, Li C, Ma J, Tian H, Qiang Z (2008) Surface hydroxyl groups of synthetic α-FeOOH in promoting oh generation from aqueous ozone: property and activity relationship. Appl Catal B-Environ 82(1–2):131–137. https://doi.org/10.1016/J.APCATB.2008.01.008
Zhang XL, Feng MB, Qu RJ, Liu H, Wang LS, Wang ZY (2016) Catalytic degradation of diethyl phthalate in aqueous solution by persulfate activated with nano-scaled magnetic CuFe2O4/MWCNTs. Chem Eng J 301:1–11. https://doi.org/10.1016/J.CEJ.2016.04.096
Zhang J, Gao Z, Wang S, Wang G, Gao X, Zhang B, Xing S, Zhao S, Qin Y (2019) Origin of synergistic effects in bicomponent cobalt oxide-platinum catalysts for selective hydrogenation reaction. Nat Commun 10(1):4166. https://doi.org/10.1038/S41467-019-11970-8
Zhou H, Wu S, Zhou Y, Yang Y, Zhang J, Luo L, Duan X, Wang S, Wang L, Tsang DCW (2019) Insights into the oxidation of organic contaminants by iron nanoparticles encapsulated within boron and nitrogen co-doped carbon nanoshell: catalyzed Fenton-like reaction at natural pH. Environ Int 128:77–88. https://doi.org/10.1016/J.ENVINT.2019.04.006
Zou J, Ma J, Zhang J (2014) Comment on electrolytic manipulation of persulfate reactivity by iron electrodes for TCE degradation in groundwater. Environ Sci Technol 48(8):4630–4631. https://doi.org/10.1021/ES501061N
Acknowledgements
This study was supported by National Natural Science Foundation of China (41731282, 41472232), National Innovation Experiment Program for University Students (2020-86) and Fundamental Research Funds for the Central Universities (2652018156).
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Cai, S., Liu, Y. & Chen, J. FeCu-biochar enhances the removal of antibacterial sulfapyridine from groundwater by activation of persulfate. Environ Chem Lett 18, 1693–1700 (2020). https://doi.org/10.1007/s10311-020-01026-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10311-020-01026-5