Skip to main content
Log in

Enhanced removal of tetracycline via advanced oxidation of sodium persulfate and biochar adsorption

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

Abstract

Advanced oxidation of antibiotic tetracycline (TC) is becoming an accessible and efficient technology. The removal of TC from the complex wastewater needs to be lucubrated. In this study, a TC removal system involving degradation and adsorption was established. TC degradation was accomplished by enhanced advanced oxidation via the addition of sodium persulfate (SP) and biochar into simulated wastewater containing Mn2+ and TC wastewater. The adsorption of TC and its derivatives was removed by biochar. The results indicate that the optimized reaction parameters were 3.0 g/L of biochar prepared at 600 °C (B600) and 400 mg/L of SP under acidic condition, and the removal percentage of TC was 87.48%, including 74.23% of degradation and 13.28% of adsorption; the anions Cl, NO3, and H2PO4 had negligible effects on the removal of TC in this Mn2+/B600/SP system. The system also functioned well with an aqueous solution with a high chemical oxygen demand (COD) concentration. Electron paramagnetic resonance (EPR) analysis indicated that ·OH and SO4 free radicals were present in the Mn2+/B600/SP system. Based on the testing and analysis results, a removal mechanism and potential TC degradation pathway for this system were proposed. TC can be degraded by ·OH and SO4 via three degradation pathways. Mn2+ can be precipitated as MnO2, and a part of the TC and its derivatives can be adsorbed on the biochar surface. The Mn2+/B600/SP system also performed satisfactorily for a complex aqueous solution with various cations and antibiotics.

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

Similar content being viewed by others

Data availability

All data generated or analyzed during this study are included in this manuscript.

References

  • Amasha M, Baalbaki A, Ghauch A (2018) A comparative study of the common persulfate activation techniques for the complete degradation of an NSAID: the case of ketoprofen. Chem Eng J 350:395–410

    Article  CAS  Google Scholar 

  • Amor C, Rodríguez-Chueca J, Fernandes JL, Domínguez JR, Lucas MS, Peres JA (2019) Winery wastewater treatment by sulphate radical based-advanced oxidation processes (SR-AOP): thermally vs UV-assisted persulphate activation. Process Saf Environ Prot 122:94–101

    Article  CAS  Google Scholar 

  • Angın D (2013) Effect of pyrolysis temperature and heating rate on biochar obtained from pyrolysis of safflower seed press cake. Bioresour Technol 128:593–597

    Article  Google Scholar 

  • Anipsitakis GP, Dionysiou DD (2004) Radical generation by the interaction of transition metals with common oxidants. Environ Sci Technol 38:3705–3712

    Article  CAS  Google Scholar 

  • Chanikya P, Nidheesh PV, Babu DS, Gopinath A, Kumar MS (2021) Treatment of dyeing wastewater by combined sulfate radical based electrochemical advanced oxidation and electrocoagulation processes. Sep Purif Technol 254:117570

    Article  CAS  Google Scholar 

  • Chen LW, Ding DH, Liu C, Cai H, Qu Y, Yang SJ, Gao Y, Cai TM (2018) Degradation of norfloxacin by CoFe2O4-GO composite coupled with peroxymonosulfate: a comparative study and mechanistic consideration. Chem Eng J 334:273–284

    Article  CAS  Google Scholar 

  • Chen JH, Yu XL, Li C, Tang X, Sun Y (2020a) Removal of tetracycline via the synergistic effect of biochar adsorption and enhanced activation of persulfate. Chem Eng J 382:122916

    Article  CAS  Google Scholar 

  • Chen YM, Xu WJ, Ling DS, Zhan LT, Gao W (2020b) A degradation-consolidation model for the stabilization behavior of landfilled municipal solid waste. Comput Geotech 118:103341

    Article  Google Scholar 

  • Chi HZ, Wang ZY, He X, Zhang JQ, Wang D, Ma J (2019) Activation of peroxymonosulfate system by copper-based catalyst for degradation of naproxen: mechanisms and pathways. Chemosphere 228:54–64

    Article  CAS  Google Scholar 

  • Costa TBBC, Lacerda ALT, Mas CD, Brietzke E, Pontes JGM, Marins LAN, Martins LG, Nunes MV, Pedrini M, Carvalho MSC, Mitrovitch MP, Hayashi MAF, Saldanha NL, Poppi RJ, Tasic L (2019) Insights into the effects of crack abuse on the human metabolome using a NMR approach. J Proteome Res 18:341–348

    CAS  Google Scholar 

  • Duan N, Dan ZG, Wang F, Pan CX, Zhou CB, Jiang LH (2011) Electrolytic manganese metal industry experience based China’s new model for cleaner production promotion. J Clean Prod 19:2082–2087

    Article  Google Scholar 

  • Duan ZH, Scheutz C, Kjeldsen P (2021) Trace gas emissions from municipal solid waste landfills: a review. Waste Manag 119:39–62

    Article  CAS  Google Scholar 

  • ELSawy EET, EL-Hebeary MR, El Mahallawi ISE (2017) Effect of manganese, silicon and chromium additions on microstructure and wear characteristics of grey cast iron for sugar industries applications. Wear 390(391):113–124

    Article  Google Scholar 

  • Furman OS, Teel AL, Watts RJ (2010) Mechanism of base activation of persulfate. Environ Sci Technol 44:6423–6428

    Article  CAS  Google Scholar 

  • Gallego-Schmid A, Tarpani RRZ (2019) Life cycle assessment of wastewater treatment in developing countries: a review. Water Res 153:63–79

    Article  CAS  Google Scholar 

  • Ghauch A, Tuqan AM, Kibbi N (2012) Ibuprofen removal by heated persulfate in aqueous solution: a kinetics study. Chem Eng J 197:483–492

    Article  CAS  Google Scholar 

  • Gu NN, Liu JY, Ye JJ, Chang N, Li YY (2019) Bioenergy, ammonia and humic substances recovery from municipal solid waste leachate: a review and process integration. Bioresour Technol 293:122159

    Article  CAS  Google Scholar 

  • Gu ZP, Chen WM, Wang F, Li QB (2020) A pilot-scale comparative study of bioreactor landfills for leachate decontamination and municipal solid waste stabilization. Waste Manag 103:113–121

    Article  CAS  Google Scholar 

  • Guo JY, Wen XY, Yang JW, Fan T (2020) Removal of benzo(a)Pyrene in polluted aqueous solution and soil using persulfate activated by corn straw biochar. J Environ Manage 272:111058

    Article  CAS  Google Scholar 

  • He J, Xiao Y, Tang JC, Chen H, Sun H (2019) Persulfate activation with sawdust biochar in aqueous solution by enhanced electron donor-transfer effect. Sci Total Environ 690:768–777

    Article  CAS  Google Scholar 

  • Hoslett J, Ghazal H, Katsou E, Jouhara H (2021) The removal of tetracycline from water using biochar produced from agricultural discarded material. Sci Total Environ 751:141755

    Article  CAS  Google Scholar 

  • Huang JZ, Zhang HC (2019) Mn-based catalysts for sulfate radical-based advanced oxidation processes: a review. Environ Int 133:105141

    Article  CAS  Google Scholar 

  • Huang Y, Han C, Liu YQ, Nadagouda MN, Machala L, O’Shea KE, Sharma VK, Dionysiou DD (2018) Degradation of atrazine by ZnxCu1−xFe2O4 nanomaterial-catalyzed sulfite under UV-vis light irradiation: green strategy to generate SO4−. Appl Catal B Environ 221:380–392

    Article  CAS  Google Scholar 

  • Koshy L, Paris E, Ling S, Jones T, BéruBé K (2007) Bioreactivity of leachate from municipal solid waste landfills-assessment of toxicity. Sci Total Environ 384:171–181

    Article  CAS  Google Scholar 

  • Leichtweis J, Silvestri S, Carissimi E (2020) New composite of pecan nutshells biochar-ZnO for sequential removal of acid red 97 by adsorption and photocatalysis. Biomass Bioenergy 140:105648

    Article  CAS  Google Scholar 

  • Li QY, Faramarzi A, Zhang S, Wang Y, Hu X, Gholizadeh M (2020) Progress in catalytic pyrolysis of municipal solid waste. Energy Convers Manag 226:113525

    Article  CAS  Google Scholar 

  • Minale M, Gu ZL, Guadie A, Kabtamu DM, Li Y, Wang XJ (2020) Application of graphene-based materials for removal of tetracyclines using adsorption and photocatalytic-degradation: a review. J Environ Manage 276:111310

    Article  CAS  Google Scholar 

  • Moradian F, Ramavandi B, Jaafarzadeh N, Kouhgardi E (2020) Effective treatment of high-salinity landfill leachate using ultraviolet/ultrasonication/peroxymonosulfate system. Waste Manag 118:591–599

    Article  CAS  Google Scholar 

  • Munagala S, Jagarapu DCK, Reddy BRR (2020) Determination of water quality index for ground water near municipal dump site in Guntur. Mater Today Proc 33:724–727

    Article  CAS  Google Scholar 

  • Nguyen TMH, Suwan P, Koottatep T, Beck SE (2019) Application of a novel, continuous-feeding ultraviolet light emitting diode (UV-LED) system to disinfect domestic wastewater for discharge or agricultural reuse. Water Res 153:53–62

    Article  CAS  Google Scholar 

  • Ning D, Wang F, Zhou CB, Zhu CL, Yu HB (2010) Analysis of pollution materials generated from electrolytic manganese industries in China. Resour Conserv Recycl 54:506–511

    Article  Google Scholar 

  • Ouyang D, Yan JC, Qian LB, Chen Y, Han L, Su AQ, Zhang WY, Ni H, Chen MF (2017) Degradation of 1, 4-dioxane by biochar supported nano magnetite particles activating persulfate. Chemosphere 184:609–617

    Article  CAS  Google Scholar 

  • Peiris C, Gunatilake SR, Mlsna TE, Mohan D, Vithanage M (2017) Biochar based removal of antibiotic sulfonamides and tetracyclines in aquatic environments: a critical review. Bioresour Technol 246:150–159

    Article  CAS  Google Scholar 

  • Pronk W, Ding A, Morgenroth E, Derlon N, Desmond P, Burkhardt M, Wu B, Fane AG (2019) Gravity-driven membrane filtration for water and wastewater treatment: a review. Water Res 149:553–565

    Article  CAS  Google Scholar 

  • Pulicharla R, Drouinaud R, Brar SK, Drogui P, Proulx F, Verma M, Surampalli RY (2018) Activation of persulfate by homogeneous and heterogeneous iron catalyst to degrade chlortetracycline in aqueous solution. Chemosphere 207:543–551

    Article  CAS  Google Scholar 

  • Reardon S (2014) Antibiotic resistance sweeping developing world. Nature 509:141–142

    Article  CAS  Google Scholar 

  • Rudi NN, Muhamad MS, Chuan L, Alipal J, Omar S, Hamidon N, Abdul Hamid NH, Mohamed Sunar N, Ali R, Harun H (2020) Evolution of adsorption process for manganese removal in water via agricultural waste adsorbents. Heliyon 6:e05049

    Article  Google Scholar 

  • Shu S, Zhu W, Wang SW, Ng CWW, Chen YM, Chiu ACF (2018) Leachate breakthrough mechanism and key pollutant indicator of municipal solid waste landfill barrier systems: centrifuge and numerical modeling approach. Sci Total Environ 612:1123–1131

    Article  CAS  Google Scholar 

  • Sikosana ML, Sikhwivhilu K, Moutloali R, Madyira DM (2019) Municipal wastewater treatment technologies: a review. Procedia Manuf 35:1018–1024

    Article  Google Scholar 

  • Soares ATG, de Castro SA, Tinkov AA, Khan H, Santamaría A, Skalnaya MG, Skalny AV, Tsatsakis A, Bowman AB, Aschner M, Ávila DS (2020) The impact of manganese on neurotransmitter systems. J Trace Elem Med Biol 61:126554

    Article  CAS  Google Scholar 

  • Son DJ, Kim WY, Jung BR, Chang D, Hong KH (2020) Pilot-scale anoxic/aerobic biofilter system combined with chemical precipitation for tertiary treatment of wastewater. J Water Process Eng 35:101224

    Article  Google Scholar 

  • Sun ZY, Gao MM, Yu X, Wang M, Wang SG, Wang XH (2021) Creating a bipolar electrode system for electrochemical advanced oxidative processes with efficient electricity consumption. J Environ Chem Eng 9:105694

    Article  CAS  Google Scholar 

  • Venna S, Sharma HB, Reddy PHP, Chowdhury S, Dubey BK (2021) Landfill leachate as an alternative moisture source for hydrothermal carbonization of municipal solid wastes to solid biofuels. Bioresour Technol 320:124410

    Article  CAS  Google Scholar 

  • Wan SL, Wu JY, Zhou SS, Wang R, Gao B, He F (2018) Enhanced lead and cadmium removal using biochar-supported hydrated manganese oxide (HMO) nanoparticles: behavior and mechanism. Sci Total Environ 616(617):1298–1306

    Article  Google Scholar 

  • Wang PL, Wu D, You XX, Li WY, Xie B (2019) Distribution of antibiotics, metals and antibiotic resistance genes during landfilling process in major municipal solid waste landfills. Environ Pollut 255:113222

    Article  CAS  Google Scholar 

  • Wang JY, An XL, Huang FY, Su JQ (2020) Antibiotic resistome in a landfill leachate treatment plant and effluent-receiving river. Chemosphere 242:125207

    Article  CAS  Google Scholar 

  • Wu CW, Chen WM, Gu ZP, Li QB (2021) A review of the characteristics of Fenton and ozonation systems in landfill leachate treatment. Sci Total Environ 762:143131

    Article  CAS  Google Scholar 

  • Yan JC, Han L, Gao WG, Xue S, Chen MF (2015) Biochar supported nanoscale zerovalent iron composite used as persulfate activator for removing trichloroethylene. Bioresour Technol 175:269–274

    Article  CAS  Google Scholar 

  • Yang X, Zhang SQ, Liu L, Ju MT (2020) Study on the long-term effects of DOM on the adsorption of BPS by biochar. Chemosphere 242:125165

    Article  CAS  Google Scholar 

  • Yazici GS (2019) Optimization of COD removal from leachate nanofiltration concentrate using H2O2/Fe+2/heat - activated persulfate oxidation processes. Process Saf Environ Prot 126:7–17

    Article  Google Scholar 

  • You XX, Wu D, Wei HW, Xie B, Lu J (2018) Fluoroquinolones and β-lactam antibiotics and antibiotic resistance genes in autumn leachates of seven major municipal solid waste landfills in China. Environ Int 113:162–169

    Article  CAS  Google Scholar 

  • Zhang SQ, Yang X, Ju MT, Liu L, Zheng K (2019a) Mercury adsorption to aged biochar and its management in China. Environ Sci Pollut Res Int 26:4867–4877

    Article  CAS  Google Scholar 

  • Zhang SQ, Zhang HQ, Liu F, Yang F, Zhou SN, Zheng K, Chu CL, Liu L, Ju MT (2019b) Effective removal of Cr(vi) from aqueous solution by biochar supported manganese sulfide. RSC Adv 9:31333–31342

    Article  CAS  Google Scholar 

  • Zhang SC, Ning SY, Liu HF, Wang XP, Wei YZ, Yin XB (2021a) Preparation of ion-exchange resin via in situ polymerization for highly selective separation and continuous removal of palladium from electroplating wastewater. Sep Purif Technol 258:117670

    Article  CAS  Google Scholar 

  • Zhang SQ, Zhang ZF, Li B, Dai WL, Si YM, Yang LX, Luo SL (2021b) Hierarchical Ag3PO4@ZnIn2S4 nanoscoparium: an innovative Z-scheme photocatalyst for highly efficient and predictable tetracycline degradation. J Colloid Interface Sci 586:708–718

    Article  CAS  Google Scholar 

  • 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

    Article  Google Scholar 

  • Zhou YY, Liu XC, Xiang YJ, Wang P, Zhang JC, Zhang FF, Wei JH, Luo L, Lei M, Tang L (2017) Modification of biochar derived from sawdust and its application in removal of tetracycline and copper from aqueous solution: adsorption mechanism and modelling. Bioresour Technol 245:266–273

    Article  CAS  Google Scholar 

  • Zhou Z, Liu XT, Sun K, Lin CY, Ma J, He MC, Wei OY (2019) Persulfate-based advanced oxidation processes (AOPs) for organic-contaminated soil remediation: a review. Chem Eng J 372:836–851

    Article  CAS  Google Scholar 

Download references

Acknowledgements

The authors thank the editor and reviewers for their comments on this paper. The authors also thank Dr. Shengnan Zhou’s help during the revision process.

Funding

This study was supported by Shandong Provincial Natural Science Foundation [Grant number. ZR2021QB216; ZR2021QH281], Research Innovation Team of College of Chemistry and Environmental Science of Hebei University [Grant number. hxkytd-py2104], and the Doctoral Foundation of Southwest University of Science and Technology [Grant number. 21zx7131].

Author information

Authors and Affiliations

Authors

Contributions

Conceptualization: Shiqiu Zhang, Qin Yin; methodology: Shiqiu Zhang, Kui Zheng, Geng Xu, Bolong Liang, Qin Yin; formal analysis and investigation: Shiqiu Zhang, Kui Zheng, Geng Xu, Bolong Liang, Qin Yin; writing—original draft preparation: Shiqiu Zhang; Qin Yin; writing—review and editing: Shiqiu Zhang, Kui Zheng, Geng Xu, Bolong Liang, Qin Yin; funding acquisition: Shiqiu Zhang, Kui Zheng, Bolong Liang; resources: Shiqiu Zhang, Kui Zheng, Geng Xu, Bolong Liang, Qin Yin; supervision: Shiqiu Zhang, Qin Yin.

Corresponding author

Correspondence to Qin Yin.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Responsible editor: Guilherme L. Dotto

Publisher's note

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

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOC 1975 KB)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, S., Zheng, K., Xu, G. et al. Enhanced removal of tetracycline via advanced oxidation of sodium persulfate and biochar adsorption. Environ Sci Pollut Res 29, 72556–72567 (2022). https://doi.org/10.1007/s11356-022-20817-7

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-022-20817-7

Keywords

Navigation