Abstract
Industrial wastewater treatment processes produce a large quantity of iron-rich sludge due to the extensive utilization of iron salt reagent. Reuse of iron-rich sludge is an attractive route for excess sludge disposal and management. In this study, sludge-derived magnetic photocatalyst was prepared using industrial iron-rich sludge as raw materials for the first time. The photocatalytic degradation system constructed by the sludge-derived photocatalysts were evaluated using tetracycline (TC) as the target contaminant, achieving a high degradation rate of 98.3% within 5 h under optimal conditions. Major reactive oxygen species in the photocatalytic systems were investigated using radical quenching experiments and electron paramagnetic resonance spectroscopy. The results suggested that •OH and O2•- were activated by photogenerated electrons and holes, respectively. Moreover, bound persistent free radicals induced by quinone-like structure in sludge-derived biochar were the predominant factors affecting radical 1O2 formation under the light irradiation. The reactive oxygen species of •OH, O2•-, and 1O2 played main roles in the degradation of TC. The used magnetic biochar can be effectively separated and recovered in aqueous solutions by the magnetism. This method provides a new cost-effective strategy for antibiotics removal from aqueous solution.
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The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.
References
An X, Chen Y, Ao M, Jin Y, Zhan L, Yu B, Wu Z, Jiang P (2022) Sequential photocatalytic degradation of organophosphorus pesticides and recovery of orthophosphate by biochar/α-Fe2O3/MgO composite: a new enhanced strategy for reducing the impacts of organophosphorus from wastewater. Chem Eng J 435:135087. https://doi.org/10.1016/j.cej.2022.135087
Ariza-Tarazona MC, Villarreal-Chiu JF, Hernandez-Lopez JM, Rivera De la Rosa J, Barbieri V, Siligardi C, Cedillo-Gonzalez EI (2020) Microplastic pollution reduction by a carbon and nitrogen-doped TiO2: effect of pH and temperature in the photocatalytic degradation process. J Hazard Mater 395:122632. https://doi.org/10.1016/j.jhazmat.2020.122632
Azalok KA, Oladipo AA, Gazi M (2021) Hybrid MnFe-LDO-biochar nanopowders for degradation of metronidazole via UV-light-driven photocatalysis: characterization and mechanism studies. Chemosphere 268:128844. https://doi.org/10.1016/j.chemosphere.2020.128844
Bautista P, Mohedano AF, Casas JA, Zazo JA, Rodriguez JJ (2008) An overview of the application of Fenton oxidation to industrial wastewaters treatment. J Chem Technol Biot 83:1323–1338. https://doi.org/10.1002/jctb.1988
Bokare AD, Choi W (2014) Review of iron-free Fenton-like systems for activating H2O2 in advanced oxidation processes. J Hazard Mater 275:121–135. https://doi.org/10.1016/j.jhazmat.2014.04.054
Chen L, Duan J, Du P, Sun W, Lai B, Liu W (2022) Accurate identification of radicals by in-situ electron paramagnetic resonance in ultraviolet-based homogenous advanced oxidation processes. Water Res 221:118747. https://doi.org/10.1016/j.watres.2022.118747
Cui X, Zhang S-S, Geng Y, Zhen J, Zhan J, Cao C, Ni S-Q (2021) Synergistic catalysis by Fe3O4-biochar/peroxymonosulfate system for the removal of bisphenol a. Sep Purif Technol 276:119351. https://doi.org/10.1016/j.seppur.2021.119351
Daraei H, Mittal A, Toolabian K, Mittal J, Mariyam A (2023) Study on the biodegradability improvement of 2,4 dinitrophenol in wastewater using advanced oxidation/reduction process with UV/SO3/ZnO. Environ Sci Pollut Res Int 30:22273–22283. https://doi.org/10.1007/s11356-022-23231-1
Ding L, Guo X, Du S, Cui F, Zhang Y, Liu P, Ouyang Z, Jia H, Zhu L (2022) Insight into the photodegradation of microplastics boosted by iron (hydr)oxides. Environ Sci Technol 56:17785–17794. https://doi.org/10.1021/acs.est.2c07824
Fang G, Liu C, Wang Y, Dionysiou DD, Zhou D (2017) Photogeneration of reactive oxygen species from biochar suspension for diethyl phthalate degradation. Appl Catal B-Environ 214:34–45. https://doi.org/10.1016/j.apcatb.2017.05.036
Feng Z, Yuan R, Wang F, Chen Z, Zhou B, Chen H (2021) Preparation of magnetic biochar and its application in catalytic degradation of organic pollutants: a review. Sci Total Environ 765:142673. https://doi.org/10.1016/j.scitotenv.2020.142673
Gholami P, Khataee A, Soltani RDC, Dinpazhoh L, Bhatnagar A (2020) Photocatalytic degradation of gemifloxacin antibiotic using Zn-Co-LDH@biochar nanocomposite. J Hazard Mater 382:121070. https://doi.org/10.1016/j.jhazmat.2019.121070
Guan K, Zhou P, Zhang J, Zhu L (2020) Synthesis and characterization of ZnO@RSDBC composites and their photo-oxidative degradation of acid orange 7 in water. J Mol Struct 1203:127425. https://doi.org/10.1016/j.molstruc.2019.127425
Gupta VK, Jain R, Mittal A, Mathur M, Sikarwar S (2007) Photochemical degradation of the hazardous dye Safranin-T using TiO2 catalyst. J Colloid Interface Sci 309:464–469. https://doi.org/10.1016/j.jcis.2006.12.010
Gupta VK, Jain R, Mittal A, Saleh TA, Nayak A, Agarwal S, Sikarwar S (2012) Photo-catalytic degradation of toxic dye amaranth on TiO2/UV in aqueous suspensions. Mater Sci Eng C Mater Biol Appl. 32:12–17. https://doi.org/10.1016/j.msec.2011.08.018
Jain R, Mathur M, Sikarwar S, Mittal A (2007) Removal of the hazardous dye rhodamine B through photocatalytic and adsorption treatments. J Environ Manage 85:956–964. https://doi.org/10.1016/j.jenvman.2006.11.002
Jin J, Li Y, Zhang J, Wu S, Cao Y, Liang P, Zhang J, Wong MH, Wang M, Shan S, Christie P (2016) Influence of pyrolysis temperature on properties and environmental safety of heavy metals in biochars derived from municipal sewage sludge. J Hazard Mater 320:417–426. https://doi.org/10.1016/j.jhazmat.2016.08.050
Ke J, Ge Y, Yang Q, Liu Y, Show P-L, Guo R, Chen J (2022) Degradation of sulfamethazine using sludge-derived photocatalysts from dyeing industry and livestock farm: preparation and mechanism. J Hazard Mater 440:129837. https://doi.org/10.1016/j.jhazmat.2022.129837
Khan A, Wang H, Liu Y, Jawad A, Ifthikar J, Liao Z, Wang T, Chen Z (2018) Highly efficient α-Mn2O3@α-MnO2-500 nanocomposite for peroxymonosulfate activation: comprehensive investigation of manganese oxides. J Mater Chem A 6:1590–1600. https://doi.org/10.1039/c7ta07942g
Leary R, Westwood A (2011) Carbonaceous nanomaterials for the enhancement of TiO2 photocatalysis. Carbon 49:741–772. https://doi.org/10.1016/j.carbon.2010.10.010
Li S, Wang Z, Zhao X, Yang X, Liang G, Xie X (2019) Insight into enhanced carbamazepine photodegradation over biochar-based magnetic photocatalyst Fe3O4/BiOBr/BC under visible LED light irradiation. Chem Eng J 360:600–611. https://doi.org/10.1016/j.cej.2018.12.002
Li T, Zhong W, Jing C, Li X, Zhang T, Jiang C, Chen W (2020a) Enhanced hydrolysis of p-Nitrophenyl phosphate by iron (hydr)oxide nanoparticles: roles of exposed facets. Environ Sci Technol 54:8658–8667. https://doi.org/10.1021/acs.est.9b07473
Li X, Wang C, Zhang J, Liu J, Liu B, Chen G (2020b) Preparation and application of magnetic biochar in water treatment: a critical review. Sci Total Environ 711:134847. https://doi.org/10.1016/j.scitotenv.2019.134847
Liu XQ, Ding HS, Wang YY, Liu WJ, Jiang H (2016) Pyrolytic temperature fependent and ash catalyzed formation of sludge char with ultra-high adsorption to 1-naphthol. Environ Sci Technol 50:2602–2609. https://doi.org/10.1021/acs.est.5b04536
Liu Y, Zhao Y, Wang J (2021) Fenton/Fenton-like processes with in-situ production of hydrogen peroxide/hydroxyl radical for degradation of emerging contaminants: advances and prospects. J Hazard Mater 404:124191. https://doi.org/10.1016/j.jhazmat.2020.124191
Luo H, Sun Y, Taylor M, Nguyen C, Strawn M, Broderick T, Wang ZW (2021) Impacts of aluminum- and iron-based coagulants on municipal sludge anaerobic digestibility, dewaterability, and odor emission. Water Environ Res 94:e1684. https://doi.org/10.1002/wer.1684
Mittal J, Arora C, Mittal A (2022) Application of biochar for the removal of methylene blue from aquatic environments, vol 29-76. Elsevier eBooks. https://doi.org/10.1016/B978-0-323-91914-2.00010-6
Mojica ER, Nguyen E, Rozov M, Bright FV (2014) pH-dependent spectroscopy of tetracycline and its analogs. J Fluoresc 24:1183–1198. https://doi.org/10.1007/s10895-014-1399-7
Muscetta M, Russo D (2021) Photocatalytic applications in wastewater and air treatment: a patent review (2010–2020). Catalysts 11:834. https://doi.org/10.3390/catal11070834
Neyens E, Baeyens J, Dewil R, de Heyder B (2004) Advanced sludge treatment affects extracellular polymeric substances to improve activated sludge dewatering. J Hazard Mater 106:83–92. https://doi.org/10.1016/j.jhazmat.2003.11.014
Orozco-Hernandez JM, Gomez Olivan LM, Heredia-Garcia G, Luja-Mondragon M, Islas-Flores H, SanJuan-Reyes N, Dublan-Garcia O (2019) Genotoxic and cytotoxic alterations induced by environmentally-relevant concentrations of amoxicillin in blood cells of Cyprinus carpio. Chemosphere 236:124323. https://doi.org/10.1016/j.chemosphere.2019.07.054
Pan H, Wang X, Xiong Z, Sun M, Murugananthan M, Zhang Y (2021) Enhanced photocatalytic CO2 reduction with defective TiO2 nanotubes modified by single-atom binary metal components. Environ Res 198:111176. https://doi.org/10.1016/j.envres.2021.111176
Pan Y, Su H, Zhu Y, Vafaei Molamahmood H, Long M (2018) CaO2 based Fenton-like reaction at neutral pH: accelerated reduction of ferric species and production of superoxide radicals. Water Res 145:731–740. https://doi.org/10.1016/j.watres.2018.09.020
Rajapaksha AU, Chen SS, Tsang DC, Zhang M, Vithanage M, Mandal S, Gao B, Bolan NS, Ok YS (2016) Engineered/designer biochar for contaminant removal/immobilization from soil and water: potential and implication of biochar modification. Chemosphere 148:276–291. https://doi.org/10.1016/j.chemosphere.2016.01.043
Rangarajan G, Jayaseelan A, Farnood R (2022) Photocatalytic reactive oxygen species generation and their mechanisms of action in pollutant removal with biochar supported photocatalysts: a review. J Clean Prod 346:131155. https://doi.org/10.1016/j.jclepro.2022.131155
Rebosura M Jr, Salehin S, Pikaar I, Keller J, Sharma K, Yuan Z (2021) The impact of primary sedimentation on the use of iron-rich drinking water sludge on the urban wastewater system. J Hazard Mater 402:124051. https://doi.org/10.1016/j.jhazmat.2020.124051
Rodrigues S, Antunes SC, Correia AT, Golovko O, Zlabek V, Nunes B (2019) Assessment of toxic effects of the antibiotic erythromycin on the marine fish gilthead seabream (Sparus aurata L.) by a multi-biomarker approach. Chemosphere 216:234–247. https://doi.org/10.1016/j.chemosphere.2018.10.124
Shahbeig H, Nosrati M (2020) Pyrolysis of municipal sewage sludge for bioenergy production: thermo-kinetic studies, evolved gas analysis, and techno-socio-economic assessment. Renew Sust Energ Rev 119:109567. https://doi.org/10.1016/j.rser.2019.109567
Shan J, Wu X, Li C, Hu J, Zhang Z, Liu H, Huang X (2023) Photocatalytic degradation of tetracycline hydrochloride by a Fe3O4/g-C3N4/rGO magnetic nanocomposite mechanism: modeling and optimization. Environ Sci Pollut Res Int 30:8098–8109. https://doi.org/10.1007/s11356-022-22770-x
Sutar S, Otari S, Jadhav J (2022) Biochar based photocatalyst for degradation of organic aqueous waste: a review. Chemosphere 287:132200. https://doi.org/10.1016/j.chemosphere.2021.132200
Tao S, Liang S, Chen Y, Yu W, Hou H, Qiu J, Zhu Y, Xiao K, Hu J, Liu B, Wang Y, Yang J (2020) Enhanced sludge dewaterability with sludge-derived biochar activating hydrogen peroxide: synergism of Fe and Al elements in biochar. Water Res 182:115927. https://doi.org/10.1016/j.watres.2020.115927
Tao S, Yang J, Hou H, Liang S, Xiao K, Qiu J, Hu J, Liu B, Yu W, Deng H (2019) Enhanced sludge dewatering via homogeneous and heterogeneous Fenton reactions initiated by Fe-rich biochar derived from sludge. Chem Eng J 372:966–977. https://doi.org/10.1016/j.cej.2019.05.002
Velo-Gala I, López-Peñalver JJ, Sánchez-Polo M, Rivera-Utrilla J (2017) Role of activated carbon surface chemistry in its photocatalytic activity and the generation of oxidant radicals under UV or solar radiation. Appl Catal B-Environ 207:412–423. https://doi.org/10.1016/j.apcatb.2017.02.028
Wang M, Mao M, Zhang M, Wen G, Yang Q, Su B, Ren Q (2019) Highly efficient treatment of textile dyeing sludge by CO2 thermal plasma gasification. Waste Manage 90:29–36. https://doi.org/10.1016/j.wasman.2019.04.025
Wang X, Pan H, Murugananthan M, Sun M, Zhang Y (2022) Gas-phase photoelectrocatalytic oxidation of volatile organic compounds using defective WO3/TiO2 nanotubes mesh. Environ Sci-Nano 9:2172–2181. https://doi.org/10.1039/d2en00130f
Wei Y, Dai J, Mackey HR, Chen GH (2017) The feasibility study of autotrophic denitrification with iron sludge produced for sulfide control. Water Res 122:226–233. https://doi.org/10.1016/j.watres.2017.05.073
Wen Q, Liu Y, Yu W, Zhu Q, Zhu Y, Bian S, Yang J (2023) Evaluation of sludge deep-dewatering filtrate recirculation to wastewater treatment plant by toxicity detection with microbial fuel cells. ACS ES&T Water 3:565–575. https://doi.org/10.1021/acsestwater.2c00571
Xiao P, Yi X, Wu M, Wang X, Zhu S, Gao B, Liu Y, Zhou H (2022) Catalytic performance and periodate activation mechanism of anaerobic sewage sludge-derived biochar. J Hazard Mater 424:127692. https://doi.org/10.1016/j.jhazmat.2021.127692
Xiong Z, Zhang Y (2021) Construction of novel in-situ photo-Fenton system based on modified g-C3N4 composite photocatalyst. Environ Res 195:110785. https://doi.org/10.1016/j.envres.2021.110785
Xu G, Zou J, Li G (2008) Ceramsite made with water and wastewater sludge and its characteristics affected by SiO2 and Al2O3. Environ Sci Technol 42:7417–7423. https://doi.org/10.1021/es801446h
Ye S, Yan M, Tan X, Liang J, Zeng G, Wu H, Song B, Zhou C, Yang Y, Wang H (2019) Facile assembled biochar-based nanocomposite with improved graphitization for efficient photocatalytic activity driven by visible light. Appl Catal B-Environ 250:78–88. https://doi.org/10.1016/j.apcatb.2019.03.004
Yi Y, Huang Z, Lu B, Xian J, Tsang EP, Cheng W, Fang J, Fang Z (2020) Magnetic biochar for environmental remediation: a review. Bioresource Technol 298:122468. https://doi.org/10.1016/j.biortech.2019.122468
Yu W, Duan H, Wang Z, Yang J, Yuan Z, Zheng M (2022) Transforming anaerobically digested sludge into high-quality biosolids with an integrated physiochemical approach. Resour Conserv Recy 184:106416. https://doi.org/10.1016/j.resconrec.2022.106416
Yu W, Wen Q, Yang J, Xiao K, Zhu Y, Tao S, Hu J (2020) Novel insights into extracellular polymeric substance degradation, hydrophilic/hydrophobic characteristics, and dewaterability of waste activated sludge pretreated by hydroxylamine enhanced Fenton oxidation. ACS ES&T Eng 1:385–392. https://doi.org/10.1021/acsestengg.0c00128
Yuan D, Zhang C, Tang S, Li X, Tang J, Rao Y, Wang Z, Zhang Q (2019) Enhancing CaO2 fenton-like process by Fe(II)-oxalic acid complexation for organic wastewater treatment. Water Res 163:114861. https://doi.org/10.1016/j.watres.2019.114861
Yuan J, Zhang Y, Zhang X, Zhao L, Shen H, Zhang S (2022) Template-free synthesis of core—shell Fe3O4@MoS2@mesoporous TiO2 magnetic photocatalyst for wastewater treatment. Int J Min Met Marter 30:177–191. https://doi.org/10.1007/s12613-022-2473-9
Zhang B, Wu T, Sun D, Chen W, Li G, Li Y (2019) NH2-MCM-41 supported on nitrogen-doped graphene as bifunctional composites for removing phenol compounds: synergistic effect between catalytic degradation and adsorption. Carbon 147:312–322. https://doi.org/10.1016/j.carbon.2019.02.084
Zhang K, Khan A, Sun P, Zhang Y, Taraqqi AKA, Zhang Y (2020) Simultaneous reduction of Cr(VI) and oxidization of organic pollutants by rice husk derived biochar and the interactive influences of coexisting Cr(VI). Sci Total Environ 706:135763. https://doi.org/10.1016/j.scitotenv.2019.135763
Zhang S, Wei Y, Metz J, He S, Alvarez PJJ, Long M (2022) Persistent free radicals in biochar enhance superoxide-mediated Fe(III)/Fe(II) cycling and the efficacy of CaO2 Fenton-like treatment. J Hazard Mater 421:126805. https://doi.org/10.1016/j.jhazmat.2021.126805
Zhang Y, Pan H, Murugananthan M, Sun P, Dionysiou DD, Zhang K, Khan A, Zhang Y (2020b) Glucose and melamine derived nitrogen-doped carbonaceous catalyst for nonradical peroxymonosulfate activation. Carbon 156:399–409. https://doi.org/10.1016/j.carbon.2019.09.050
Zhang Y, Yang W, Zhang K, Kumaravel A, Zhang Y (2021) Sulfite activation by glucose-derived carbon catalysts for As(III) oxidation: the role of ketonic functional groups and conductivity. Environ Sci Technol 55:11961–11969. https://doi.org/10.1021/acs.est.1c02499
Zhao Y, Yuan X, Li X, Jiang L, Wang H (2021) Burgeoning prospects of biochar and its composite in persulfate-advanced oxidation process. J Hazard Mater 409:124893. https://doi.org/10.1016/j.jhazmat.2020.124893
Zhou X, Li W, Mabon R, Broadbelt LJ (2018) A mechanistic model of fast pyrolysis of hemicellulose. Energ Environ Sci 11:1240–1260. https://doi.org/10.1039/c7ee03208k
Zhou X, Zeng Z, Zeng G, Lai C, Xiao R, Liu S, Huang D, Qin L, Liu X, Li B, Yi H, Fu Y, Li L, Zhang M, Wang Z (2020) Insight into the mechanism of persulfate activated by bone char: unraveling the role of functional structure of biochar. Chem Eng J 401:126127. https://doi.org/10.1016/j.cej.2020.126127
Funding
This work was supported by the Natural Science Foundation of China (No. 41967030), Guangxi Natural Science Foundation (2020GXNSFAA159170), the Young Scholar Innovation Team of Guangxi Minzu University (2022), Basic Ability Improvement Project for Young and Middle-Aged Teachers in Guangxi Province (No. 2019KY0187), Scientific Research Foundation for introduced Talents of Guangxi Minzu University (No. 2018KJQD07 and 2018KJQD08), and China Postdoctoral Science Foundation (No. 2022MD713733).
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Xixiang Liu: data curation, investigation, writing—original draft
Hengyi Wang: formal analysis, validation, methodology
Xinyi Shi: data curation, formal analysis
Zheng Zhou: writing—review
Nan Li: writing—review
Honghui Pan: conceptualization, resources, writing—review and editing
Qin Shi: funding acquisition, project administration, writing—review and editing
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Liu, ., Wang, H., Shi, X. et al. Efficient photocatalytic degradation of tetracycline using magnetic biochar derived by iron-rich sludge. Environ Sci Pollut Res 30, 90708–90720 (2023). https://doi.org/10.1007/s11356-023-28769-2
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DOI: https://doi.org/10.1007/s11356-023-28769-2