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Degradation of tetracycline by activating persulfate using biochar-based CuFe2O4 composite

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Abstract

Biochar derived from Lentinus edodes (LBC) and CuFe2O4 (CuFe2O4@LBC) composites were prepared by the hydrothermal method, and were applied to activate persulfate (PDS) for degrading tetracycline (TC) in a wide pH range. The CuFe2O4@LBC composites were characterized by XRD, FTIR, SEM, and XPS. LBC-derived biochars greatly reduced the aggregation of CuFe2O4 particles and enhanced the catalytic performance of CuFe2O4. CuFe2O4@LBC catalyst could remove 85% of tetracycline within 100 min under visible light. In addition, the removal rate of TC reached 76% after five cycles, indicating that the composite had good stability and reusability. Simple classical quenching experiments suggested that the degradation of TC could be mainly attributed to •OH and •S \({\text{O}}_{4}^{-}\).

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References

  • Al-Dhabi NA, Esmail GA, Valan Arasu M (2021) Effective degradation of tetracycline by manganese peroxidase producing Bacillus velezensis strain Al-Dhabi 140 from Saudi Arabia using fibrous-bed reactor. Chemosphere 268:128726

    Article  CAS  Google Scholar 

  • Alhujaily A, Mao Y, Zhang J, Ifthikar J, Zhang X, Ma F (2020) Facile fabrication of Mg-Fe-biochar adsorbent derived from spent mushroom waste for phosphate removal. J Taiwan Inst Chem Eng 117:75–85

    Article  CAS  Google Scholar 

  • Chen L, Zhang YZ, Lin CH, Yang W, Meng Y, Guo Y, Li ML, Xiao D (2014) Hierarchically porous nitrogen-rich carbon derived from wheat straw as an ultra-high-rate anode for lithium ion batteries. J Mater Chem A 2:9684–9690

    Article  CAS  Google Scholar 

  • Chen Q, Wu S, Xin Y (2016) Synthesis of Au–CuS–TiO2 nanobelts photocatalyst for efficient photocatalytic degradation of antibiotic oxytetracycline. Chem Eng J 302:377–387

    Article  CAS  Google Scholar 

  • Chen QL, An XL, Zhu YG, Su JQ, Gillings MR, Ye ZL, Cui L (2017) Application of Struvite Alters the Antibiotic Resistome in Soil, Rhizosphere, and Phyllosphere. Environ Sci Technol 51:8149–8157

    Article  CAS  Google Scholar 

  • Chen L, Ding D, Liu C, Cai H, Qu Y, Yang S, Gao Y, Cai T (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 

  • Chopra I, Roberts M (2001) Tetracycline antibiotics: mode of action, applications, molecular biology, and epidemiology of bacterial resistance. Microbiol Mol Biol Rev 65:232–60 ; second page, table of contents

  • Colantoni A, Evic N, Lord R, Retschitzegger S, Proto AR, Gallucci F, Monarca D (2016) Characterization of biochars produced from pyrolysis of pelletized agricultural residues. Renew Sustain Energy Rev 64:187–194

    Article  CAS  Google Scholar 

  • Ding YB, Zhu LH, Wang N, Tang HQ (2013) Sulfate radicals induced degradation of tetrabromobisphenol A with nanoscaled magnetic CuFe2O4 as a heterogeneous catalyst of peroxymonosulfate. Appl Catal B-Environ 129:153–162

    Article  CAS  Google Scholar 

  • Dou RY, Ma JF, Huang DQ, Fan CH, Zhao WC, Peng MG, Komarneni S (2018) Bisulfite assisted photocatalytic degradation of methylene blue by Ni-Fe-Mn oxide from MnO4 intercalated LDH. Appl Clay Sci 161:235–241

    Article  CAS  Google Scholar 

  • Du Z, Feng L, Guo Z, Yan T, Hu Q, Lin J, Huang Y, Tang C, Fang Y (2021) Ultrathin h-BN/Bi2MoO6 heterojunction with synergetic effect for visible-light photocatalytic tetracycline degradation. J Colloid Interface Sci 589:545–555

    Article  CAS  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 

  • Gao Y, Li Y, Zhang L, Huang H, Hu J, Shah SM, Su X (2012) Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide. J Colloid Interface Sci 368:540–546

    Article  CAS  Google Scholar 

  • Ghodake GS, Shinde SK, Kadam AA, Saratale RG, Saratale GD, Kumar M, Palem RR, AL-Shwaiman HA, Elgorban AM, Syed A, Kim DY (2021) Review on biomass feedstocks, pyrolysis mechanism and physicochemical properties of biochar: State-of-the-art framework to speed up vision of circular bioeconomy. J Clean Prod 297

  • Guan C, Jiang J, Pang S, Luo C, Ma J, Zhou Y, Yang Y (2017) Oxidation Kinetics of Bromophenols by Nonradical Activation of Peroxydisulfate in the Presence of Carbon Nanotube and Formation of Brominated Polymeric Products. Environ Sci Technol 51:10718–10728

    Article  CAS  Google Scholar 

  • Guo YP, Zeng ZQ, Zhu YC, Huang ZG, Cui Y, Yang JY (2018) Catalytic oxidation of aqueous organic contaminants by persulfate activated with sulfur-doped hierarchically porous carbon derived from thiophene. Appl Catal B-Environ 220:635–644

    Article  CAS  Google Scholar 

  • He G, Jiang X, Yao L, Liu G, Yang Y, Jiang Y, Liu W (2021) Effects of tetracycline on nitrogen and carbon cycling rates and microbial abundance in sediments with and without biochar amendment. Chemosphere 270:129509

    Article  CAS  Google Scholar 

  • Hu XB, Zhu ZG, Li ZH, Xie LL, Wu YH, Zheng LY (2018) Heterostructure of CuO microspheres modified with CuFe2O4 nanoparticles for highly sensitive H2S gas sensor. Sensors Actuators B-Chem 264:139–149

    Article  CAS  Google Scholar 

  • Huang DQ, Ma JF, Yu LM, Wu DR, Wang K, Yang MR, Papoulis D, Komarneni S (2015) AgCl and BiOCl composited with NiFe-LDH for enhanced photo-degradation of Rhodamine B. Sep Purif Technol 156:789–794

    Article  CAS  Google Scholar 

  • Huang WH, Lee DJ, Huang C (2021) Modification on biochars for applications: A research update. Bioresour Technol 319:124100

    Article  CAS  Google Scholar 

  • Huang WQ, Xiao S, Zhong H, Yan M, Yang X (2021) Activation of persulfates by carbonaceous materials: A review. Chem Eng J 418:129297

    Article  CAS  Google Scholar 

  • Huang ZH, Ji ZY, Zhao YY, Liu J, Li F, Yuan JS (2020) Treatment of wastewater containing 2-methoxyphenol by persulfate with thermal and alkali synergistic activation: Kinetics and mechanism. Chem Eng J 380

  • Jin Y, Zhang M, Jin Z, Wang G, Li R, Zhang X, Liu X, Qu J, Wang H (2021) Characterization of biochars derived from various spent mushroom substrates and evaluation of their adsorption performance of Cu(II) ions from aqueous solution. Environ Res 196:110323

    Article  CAS  Google Scholar 

  • Kong Y, Ou J, Liu Z, Xue SK, Tao YX, Ma JF (2014) The electrocatalytic characteristics of poly(azure B) and its application in the sensitive determination of hydroquinone. Anal Methods 6:3735–3740

    Article  CAS  Google Scholar 

  • Kong Y, Shan X, Ma J, Chen M, Chen Z (2014) A novel voltammetric sensor for ascorbic acid based on molecularly imprinted poly(o-phenylenediamine-co-o-aminophenol). Anal Chim Acta 809:54–60

    Article  CAS  Google Scholar 

  • Laokul P, Amornkitbamrung V, Seraphin S, Maensiri S (2011) Characterization and magnetic properties of nanocrystalline CuFe2O4, NiFe2O4, ZnFe2O4 powders prepared by the Aloe vera extract solution. Curr Appl Phys 11:101–108

    Article  Google Scholar 

  • Lei CS, Ma JF, Li DL, Zhang WY, Guang XH, Ma J (2010) Composite denitrification reagent for high concentration ammonia removal by air stripping. Chin Sci Bull 55:2657–2661

    Article  CAS  Google Scholar 

  • Leichtweis J, Silvestri S, Welter N, Vieira Y, Zaragoza-Sanchez PI, 2Chavez-Mejia AC, Carissimi E (2021) Wastewater containing emerging contaminants treated by residues from the brewing industry based on biochar as a new CuFe2O4 / biochar photocatalyst. Process Saf Environ Protect 150, 497-509

  • Li X, Huang X, Xi S, Miao S, Ding J, Cai W, Liu S, Yang X, Yang H, Gao J, Wang J, Huang Y, Zhang T, Liu B (2018) Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis. J Am Chem Soc 140:12469–12475

    Article  CAS  Google Scholar 

  • Li M, Lu MJ, Yang JR, Xiao J, Han LN, Zhang YJ, Bo XJ (2019) Facile design of ultrafine CuFe2O4 nanocrystallines coupled porous carbon nanowires: Highly effective electrocatalysts for hydrogen peroxide reduction and the oxygen evolution reaction. J Alloys Compd 809

  • Li JH, Shi C, Bao A (2021) Design of boron-doped mesoporous carbon materials for multifunctional applications: Dye adsorption and CO2 capture. J Environ Chem Eng 9

  • Liu S, Liu Y, Chen M, Li L, Tu W, Huang Z (2021) CuFe2O4 modified expanded graphite synthesized by urea-assisted hydrothermal method for tetracycline treatment through persulfate activation: Characterization, mechanism and degradation intermediates. Chem Eng J

  • Lou Z, Sun Y, Bian S, Ali Baig S, Hu B, Xu X (2017) Nutrient conservation during spent mushroom compost application using spent mushroom substrate derived biochar. Chemosphere 169:23–31

    Article  CAS  Google Scholar 

  • Ma JF, Zou J, Li LY, Yao C, Zhang TL, Li DL (2013) Synthesis and characterization of Ag3PO4 immobilized in bentonite for the sunlight-driven degradation of Orange II. Appl Catal B-Environ 134:1–6

    Article  CAS  Google Scholar 

  • Ma J, Zou J, Li L, Yao C, Kong Y, Cui B, Zhu R, Li D (2014) Nanocomposite of attapulgite–Ag3PO4 for Orange II photodegradation. Appl Catal B 144:36–40

    Article  CAS  Google Scholar 

  • Ma JF, Ding JF, Li LY, Zou J, Kong Y, Komarneni S (2015) In situ reduction for synthesis of nano-sized Cu2O particles on MgCuAl-LDH layers for degradation of orange II under visible light. Ceram Int 41:3191–3196

    Article  CAS  Google Scholar 

  • Ma JF, Wang K, Li LY, Zhang T, Kong Y, Komarneni S (2015) Visible-light photocatalytic decolorization of Orange II on Cu2O/ZnO nanocomposites. Ceram Int 41:2050–2056

    Article  CAS  Google Scholar 

  • Ni QZ, Ma JF, Fan CH, Kong Y, Peng MG, Komarneni S (2018) Spinel-type cobalt-manganese oxide catalyst for degradation of Orange II using a novel heterogeneous photo-chemical catalysis system. Ceram Int 44:19474–19480

    Article  CAS  Google Scholar 

  • Niu L, Zhang G, Xian G, Ren Z, Wei T, Li Q, Zhang Y, Zou Z (2021) Tetracycline degradation by persulfate activated with magnetic γ-Fe2O3/CeO2 catalyst: Performance, activation mechanism and degradation pathway. Sep Purif Technol 259:118156

    Article  CAS  Google Scholar 

  • Oginni O, Singh K (2020) Influence of high carbonization temperatures on microstructural and physicochemical characteristics of herbaceous biomass derived biochars. J Environ Chem Eng 8

  • Pang Y, Kong L, Lei H, Chen D, Yuvaraja G (2018) Combined microwave-induced and photocatalytic oxidation using zinc ferrite catalyst for efficient degradation of tetracycline hydrochloride in aqueous solution. J Taiwan Inst Chem Eng 93:397–404

    Article  CAS  Google Scholar 

  • Ren Y, Lin L, Ma J, Yang J, Feng J, Fan Z (2015) Sulfate radicals induced from peroxymonosulfate by magnetic ferrospinel MFe2O4 (M = Co, Cu, Mn, and Zn) as heterogeneous catalysts in the water. Appl Catal B 165:572–578

    Article  CAS  Google Scholar 

  • Santana RMD, Charamba LCV, do Nascimento GE, de Oliveira JGC, Sales DCS, Duarte MMMB, Napoleao DC (2019) Degradation of Textile Dyes Employing Advanced Oxidative Processes: Kinetic, Equilibrium Modeling, and Toxicity Study of Seeds and Bacteria. Water Air Soil Pollut 230

  • Sun M, Lei Y, Cheng H, Ma J, Qin Y, Kong Y, Komarneni S (2020) Mg doped CuO–Fe2O3 composites activated by persulfate as highly active heterogeneous catalysts for the degradation of organic pollutants. J Alloys Compd 825

  • Tang MY, Xia FL, Gao CJ, Qiu HX (2016) Preparation of magnetically recyclable CuFe2O4/RGO for catalytic hydrolysis of sodium borohydride. Int J Hydrogen Energy 41:13058–13068

    Article  CAS  Google Scholar 

  • Tang L, Liu YI, Wang JJ, Zeng GM, Deng YC, Dong HR, Feng HP, Wang JJ, Peng B (2018) Enhanced activation process of persulfate by mesoporous carbon for degradation of aqueous organic pollutants: Electron transfer mechanism. Appl Catal B-Environ 231:1–10

    Article  CAS  Google Scholar 

  • Wang J, Wang Z, Huang B, Ma Y, Liu Y, Qin X, Zhang X, Dai Y (2012) Oxygen vacancy induced band-gap narrowing and enhanced visible light photocatalytic activity of ZnO. ACS Appl Mater Interfaces 4:4024–4030

    Article  CAS  Google Scholar 

  • Wang X, Qin Y, Zhu L, Tang H (2015) Nitrogen-Doped Reduced Graphene Oxide as a Bifunctional Material for Removing Bisphenols: Synergistic Effect between Adsorption and Catalysis. Environ Sci Technol 49:6855–6864

    Article  CAS  Google Scholar 

  • Wang H, Guo W, Liu B, Wu Q, Luo H, Zhao Q, Si Q, Sseguya F, Ren N (2019) Edge-nitrogenated biochar for efficient peroxydisulfate activation: An electron transfer mechanism. Water Res 160:405–414

    Article  CAS  Google Scholar 

  • Wang B, Li Q, Lv Y, Fu H, Liu D, Feng Y, Xie H, Qu H (2021a) Insights into the mechanism of peroxydisulfate activated by magnetic spinel CuFe2O4/SBC as a heterogeneous catalyst for bisphenol S degradation. Chem Eng J 416

  • Wang BY, Li QQ, Lv Y, Fu HB, Liu DY, Feng YF, Xie HF, Qu HX (2021b) Insights into the mechanism of peroxydisulfate activated by magnetic spinel CuFe2O4/SBC as a heterogeneous catalyst for bisphenol S degradation. Chem Eng J 416

  • Xiao PF, An L, Wu DD (2020) The use of carbon materials in persulfate-based advanced oxidation processes: A review. New Carbon Mater 35:667–681

    Article  Google Scholar 

  • Xie X, Zhang B, Wang Q, Zhao X, Wu D, Wu H, Sun X, Hou C, Yang X, Yu R, Zhang S, Murugadoss V, Du W (2021) Efficient microwave absorber and supercapacitors derived from puffed-rice-based biomass carbon: Effects of activating temperature. J Colloid Interface Sci 594:290–303

    Article  CAS  Google Scholar 

  • Yue Y, Liu YJ, Wang J, Vukanti R, Ge Y (2021) Enrichment of potential degrading bacteria accelerates removal of tetracyclines and their epimers from cow manure biochar amended soil. Chemosphere 278:130358

    Article  CAS  Google Scholar 

  • Zhang T, Zhu H, Croue JP (2013) Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water: efficiency, stability, and mechanism. Environ Sci Technol 47:2784–2791

    Article  CAS  Google Scholar 

  • Zhou XR, Zhu Y, Niu QY, Zeng GM, Lai C, Liu SY, Huang DL, Qin L, Liu XG, Li BS, Yi H, Fu YK, Li L, Zhang MM, Zhou CY, Liu JH (2021) New notion of biochar: A review on the mechanism of biochar applications in advannced oxidation processes. Chem Eng J 416

  • Zhu LF, Huang DQ, Ma HF, Wu DR, Yang MR, Komarneni S (2015) Fabrication of AgBr/Ag2CrO4 composites for enhanced visible-light photocatalytic activity. Ceram Int 41:12509–12513

    Article  CAS  Google Scholar 

  • Zhu BY, Cheng H, Qin Y, Ma JF, Kong Y, Komarneni S (2020a) Copper sulfide as an excellent co-catalyst with K2S2O8 for dye decomposition in advanced oxidation process. Sep Purif Technol 233

  • Zhu LJ, Cheng H, Ma JF, Kong Y, Qin Y, Komarneni S (2020b) Decolorization of methyl orange by MnO2/organic acid system: The role of Mn(III). Mater Res Bull 122

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Acknowledgements

This work was supported by “Qing Lan Project” of Jiangsu Province, “333 Project” of Jiangsu Province.

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Jianfeng Ma: Data curation, Methodology and Formal analysis, Writing—original draft, Wei Zhang, Jianfeng Ma and Shijun Feng, Writing—review & editing Fang Zhu and Sridhar Komarneni.

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Correspondence to Jianfeng Ma or Sridhar Komarneni.

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Zhang, W., Feng, S., Ma, J. et al. Degradation of tetracycline by activating persulfate using biochar-based CuFe2O4 composite. Environ Sci Pollut Res 29, 67003–67013 (2022). https://doi.org/10.1007/s11356-022-20500-x

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