Abstract
In this work, tea waste biochar was prepared and used to activate peroxodisulfate (PDS) for the removal of tetracycline (TC) efficiently. And SEM, XRD, Raman, and FTIR were used to characterize the biochar. The effects of reaction conditions including initial pH, biochar dosage, and PDS concentration on the removal of TC were explored, and the result showed that compared with the biochar prepared at 400 °C and 500 °C, the biochar pyrolyzed at 600 °C (TBC600) had the highest TC removal performance due to its higher sp2 hybrid carbon content, richer defective structure, and stronger electron deliverability. Under the optimal dosage of PDS (4 mM) and TBC600 (0.8 g L−1), the removal efficiency of TC (10 mg L−1) reached 81.65%. After four cycles of TBC600, the removal rate could still reach 75.51%, indicating that TBC600 has excellent stability. In addition, quenching experiments and electron paramagnetic resonance (EPR) verified that the active oxygen including SO4·−, ·OH, O2·−, and singlet oxygen (1O2) was involved, among which 1O2 and OH were the main active substance in the TC removal. Therefore, this work provided a green and efficient persulfate activator and a method for recycling tea waste.
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References
Akhtar L, Ahmad M, Iqbal S, Abdelhafez AA, Mehran MT (2021) Biochars’ adsorption performance towards moxifloxacin and ofloxacin in aqueous solution: Role of pyrolysis temperature and biomass type. Environ. Technol. Innovation 24:101912. https://doi.org/10.1016/j.eti.2021.101912
Alatalo S-M, Daneshvar E, Kinnunen N, Meščeriakovas A, Thangaraj SK, Jänis J, Tsang DCW, Bhatnagar A, Lähde A (2019) Mechanistic insight into efficient removal of tetracycline from water by Fe/graphene. Chem Eng J 373:821–830. https://doi.org/10.1016/j.cej.2019.05.118
Amarasinghe HAHI, Gunathilake SK, Karunarathna AK (2016) Ascertaining of optimum pyrolysis conditions in producing refuse tea biochar as a soil amendment. Procedia Food Sci 6:97–102. https://doi.org/10.1016/j.profoo.2016.02.021
Bilal M, Ashraf SS, Barceló D, Iqbal HMN (2019) Biocatalytic degradation/redefining “removal” fate of pharmaceutically active compounds and antibiotics in the aquatic environment. Sci Total Environ 691:1190–1211. https://doi.org/10.1016/j.scitotenv.2019.07.224
Çelebi H (2020) Recovery of detox tea wastes: usage as a lignocellulosic adsorbent in Cr6+ adsorption. J Environ Chem Eng 8:104310. https://doi.org/10.1016/j.jece.2020.104310
Dong H, Jiang Z, Zhang C, Deng J, Hou K, Cheng Y, Zhang L, Zeng G (2018) Removal of tetracycline by Fe/Ni bimetallic nanoparticles in aqueous solution. J Colloid Interface Sci 513:117–125. https://doi.org/10.1016/j.jcis.2017.11.021
Du L, Xu W, Liu S, Li X, Huang D, Tan X, Liu Y (2020) Activation of persulfate by graphitized biochar for sulfamethoxazole removal: the roles of graphitic carbon structure and carbonyl group. J Colloid Interface Sci 577:419–430. https://doi.org/10.1016/j.jcis.2020.05.096
Duan X, Sun H, Ao Z, Zhou L, Wang G, Wang S (2016) Unveiling the active sites of graphene-catalyzed peroxymonosulfate activation. Carbon 107:371–378. https://doi.org/10.1016/j.carbon.2016.06.016
Duan X, Sun H, Wang S (2018) Metal-free carbocatalysis in advanced oxidation reactions. Acc Chem Res 51:678–687. https://doi.org/10.1021/acs.accounts.7b00535
Ezzariai A, Hafidi M, Khadra A, Aemig Q, El Fels L, Barret M, Merlina G, Patureau D, Pinelli E (2018) Human and veterinary antibiotics during composting of sludge or manure: global perspectives on persistence, degradation, and resistance genes. J Hazard Mater 359:465–481. https://doi.org/10.1016/j.jhazmat.2018.07.092
Guan R, Yuan X, Wu Z, Wang H, Jiang L, Zhang J, Li Y, Zeng G, Mo D (2018) Accelerated tetracycline degradation by persulfate activated with heterogeneous magnetic NixFe3−xO4 catalysts. Chem Eng J 350:573–584. https://doi.org/10.1016/j.cej.2018.05.195
Guan Y-H, Ma J, Ren Y-M, Liu Y-L, Xiao J-Y, Lin L-q, 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 47:5431–5438. https://doi.org/10.1016/j.watres.2013.06.023
Han S-W, Jung D-W, Jeong J-H, Oh E-S (2014) Effect of pyrolysis temperature on carbon obtained from green tea biomass for superior lithium ion battery anodes. Chem Eng J 254:597–604. https://doi.org/10.1016/j.cej.2014.06.021
He J, Xiao Y, Tang J, 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. https://doi.org/10.1016/j.scitotenv.2019.07.043
Howard E, Levitt LS (1953) The persulfate oxidation of sulfoxides in buffered solution.1 I. J Am Chem Soc 75:6170–6173. https://doi.org/10.1021/ja01120a018
Jiang X, Guo Y, Zhang L, Jiang W, Xie R (2018) Catalytic degradation of tetracycline hydrochloride by persulfate activated with nano Fe0 immobilized mesoporous carbon. Chem Eng J 341:392–401. https://doi.org/10.1016/j.cej.2018.02.034
Jin J, Yang Z, Xiong W, Zhou Y, Xu R, Zhang Y, Cao J, Li X, Zhou C (2019) Cu and Co nanoparticles co-doped MIL-101 as a novel adsorbent for efficient removal of tetracycline from aqueous solutions. Sci Total Environ 650:408–418. https://doi.org/10.1016/j.scitotenv.2018.08.434
Kumar A, Pal D (2018) Antibiotic resistance and wastewater: correlation, impact and critical human health challenges. J Environ Chem Eng 6:52–58. https://doi.org/10.1016/j.jece.2017.11.059
Lee H, Lee H-J, Jeong J, Lee J, Park N-B, Lee C (2015) Activation of persulfates by carbon nanotubes: oxidation of organic compounds by nonradical mechanism. Chem Eng J 266:28–33. https://doi.org/10.1016/j.cej.2014.12.065
Li B, Zhang Y, Xu J, Xie Z, Tang J, Li X, Fan S (2021) Simultaneous carbonization, activation, and magnetization for producing tea waste biochar and its application in tetracycline removal from the aquatic environment. J Environ Chem Eng 9:105324. https://doi.org/10.1016/j.jece.2021.105324
Li J, Yu G, Pan L, Li C, You F, Xie S, Wang Y, Ma J, Shang X (2018) Study of ciprofloxacin removal by biochar obtained from used tea leaves. J Environ Sci 73:20–30. https://doi.org/10.1016/j.jes.2017.12.024
Li W, Liu B, Wang Z, Wang K, Lan Y, Zhou L (2020) Efficient activation of peroxydisulfate (PDS) by rice straw biochar modified by copper oxide (RSBC-CuO) for the degradation of phenacetin (PNT). Chem Eng J 395:125094. https://doi.org/10.1016/j.cej.2020.125094
Li X, Liu J, Rykov AI, Han H, Jin C, Liu X, Wang J (2015) Excellent photo-Fenton catalysts of Fe–Co Prussian blue analogues and their reaction mechanism study. Appl Catal B 179:196–205. https://doi.org/10.1016/j.apcatb.2015.05.033
Lian F, Xing BS (2017) Black carbon (Biochar) in water/soil environments: molecular structure, sorption, stability, and potential risk. Environ Sci Technol 51:13517–13532. https://doi.org/10.1021/acs.est.7b02528
Liu BH, Guo WQ, Wang HZ, Si QS, Zhao Q, Luo HC, Ren NQ (2020) B-doped graphitic porous biochar with enhanced surface affinity and electron transfer for efficient peroxydisulfate activation. Chem Eng J 396:125119. https://doi.org/10.1016/j.cej.2020.125119
Liu C, Chen L, Ding D, Cai T (2019) From rice straw to magnetically recoverable nitrogen doped biochar: efficient activation of peroxymonosulfate for the degradation of metolachlor. Appl Catal B 254:312–320. https://doi.org/10.1016/j.apcatb.2019.05.014
Lu X, Qiu W, Ma J, Xu H, Wang D, Cheng H, Zhang W, He X (2020) The overestimated role of singlet oxygen for pollutants degradation in some non-photochemical systems. Chem Eng J 401:126128. https://doi.org/10.1016/j.cej.2020.126128
Luo C, Gao J, Wu D, Jiang J, Liu Y, Zhou W, Ma J (2019) Oxidation of 2,4-bromophenol by UV/PDS and formation of bromate and brominated products: a comparison to UV/H2O2. Chem Eng J 358:1342–1350. https://doi.org/10.1016/j.cej.2018.10.084
Ma Y, Xiong H, Zhao Z, Yu Y, Zhou D, Dong S (2018) Model-based evaluation of tetracycline hydrochloride removal and mineralization in an intimately coupled photocatalysis and biodegradation reactor. Chem Eng J 351:967–975. https://doi.org/10.1016/j.cej.2018.06.167
Nasseri S, Mahvi AH, Seyedsalehi M, Yaghmaeian K, Nabizadeh R, Alimohammadi M, Safari GH (2017) Degradation kinetics of tetracycline in aqueous solutions using peroxydisulfate activated by ultrasound irradiation: effect of radical scavenger and water matrix. J Mol Liq 241:704–714. https://doi.org/10.1016/j.molliq.2017.05.137
Niu J, Xie Y, Luo H, Wang Q, Zhang Y, Wang Y (2019) Cobalt oxide loaded graphitic carbon nitride as adsorptive photocatalyst for tetracycline removal from aqueous solution. Chemosphere 218:169–178. https://doi.org/10.1016/j.chemosphere.2018.11.111
Ouyang D, Yan J, Qian L, Chen Y, Han L, Su A, Zhang W, Ni H, Chen M (2017) Degradation of 1,4-dioxane by biochar supported nano magnetite particles activating persulfate. Chemosphere 184:609–617. https://doi.org/10.1016/j.chemosphere.2017.05.156
Rajapaksha AU, Vithanage M, Zhang M, Ahmad M, Mohan D, Chang SX, Ok YS (2014) Pyrolysis condition affected sulfamethazine sorption by tea waste biochars. Bioresour Technol 166:303–308. https://doi.org/10.1016/j.biortech.2014.05.029
Salehi E, Askari M, Velashjerdi M, Arab B (2020) Phosphoric acid-treated spent tea residue biochar for wastewater decoloring: batch adsorption study and process intensification using multivariate data-based optimization. Chem Eng Process 158:108170. https://doi.org/10.1016/j.cep.2020.108170
Smith MW, Dallmeyer I, Johnson TJ, Brauer CS, McEwen JS, Espinal JF, Garcia-Perez M (2016) Structural analysis of char by Raman spectroscopy: improving band assignments through computational calculations from first principles. Carbon 100:678–692. https://doi.org/10.1016/j.carbon.2016.01.031
Tian N, Tian X, Nie Y, Yang C, Zhou Z, Li Y (2018) Biogenic manganese oxide: an efficient peroxymonosulfate activation catalyst for tetracycline and phenol degradation in water. Chem Eng J 352:469–476. https://doi.org/10.1016/j.cej.2018.07.061
Wang C, Qu G, Wang T, Deng F, Liang D (2018) Removal of tetracycline antibiotics from wastewater by pulsed corona discharge plasma coupled with natural soil particles. Chem Eng J 346:159–170. https://doi.org/10.1016/j.cej.2018.03.149
Wang HZ, Guo WQ, Liu BH, Wu QL, Luo HC, Zhao Q, Si QS, Sseguya F, Ren NQ (2019) Edge-nitrogenated biochar for efficient peroxydisulfate activation: an electron transfer mechanism. Water Res 160:405–414. https://doi.org/10.1016/j.watres.2019.05.059
Wang J, Liao Z, Ifthikar J, Shi L, Du Y, Zhu J, Xi S, Chen Z, Chen Z (2017) Treatment of refractory contaminants by sludge-derived biochar/persulfate system via both adsorption and advanced oxidation process. Chemosphere 185:754–763. https://doi.org/10.1016/j.chemosphere.2017.07.084
Wei X, Gao N, Li C, Deng Y, Zhou S, Li L (2016) Zero-valent iron (ZVI) activation of persulfate (PS) for oxidation of bentazon in water. Chem Eng J 285:660–670. https://doi.org/10.1016/j.cej.2015.08.120
Wu Z, Su X, Lin Z, Khan NI, Owens G, Chen Z (2021) Removal of As(V) by iron-based nanoparticles synthesized via the complexation of biomolecules in green tea extracts and an iron salt. Sci Total Environ 764:142883. https://doi.org/10.1016/j.scitotenv.2020.142883
Xiao C, Li H, Zhao Y, Zhang X, Wang X (2020) Green synthesis of iron nanoparticle by tea extract (polyphenols) and its selective removal of cationic dyes. J Environ Manage 275:111262. https://doi.org/10.1016/j.jenvman.2020.111262
Xiong W, Zeng G, Yang Z, Zhou Y, Zhang C, Cheng M, Liu Y, Hu L, Wan J, Zhou C, Xu R, Li X (2018) Adsorption of tetracycline antibiotics from aqueous solutions on nanocomposite multi-walled carbon nanotube functionalized MIL-53(Fe) as new adsorbent. Sci Total Environ 627:235–244. https://doi.org/10.1016/j.scitotenv.2018.01.249
Yang Q, Yang X, Yan Y, Sun C, Wu H, He J, Wang D (2018) Heterogeneous activation of peroxymonosulfate by different ferromanganese oxides for tetracycline degradation: structure dependence and catalytic mechanism. Chem Eng J 348:263–270. https://doi.org/10.1016/j.cej.2018.04.206
Yin R, Guo W, Wang H, Du J, Wu Q, Chang J-S, Ren N (2019) Singlet oxygen-dominated peroxydisulfate activation by sludge-derived biochar for sulfamethoxazole degradation through a nonradical oxidation pathway: performance and mechanism. Chem Eng J 357:589–599. https://doi.org/10.1016/j.cej.2018.09.184
Yoo S, Kelley SS, Tilotta DC, Park S (2018) Structural characterization of loblolly pine derived biochar by X-ray diffraction and electron energy loss spectroscopy. ACS Sustainable Chem Eng 6:2621–2629. https://doi.org/10.1021/acssuschemeng.7b04119
Yu J, Tang L, Pang Y, Zeng G, Wang J, Deng Y, Liu Y, Feng H, Chen S, Ren X (2019) Magnetic nitrogen-doped sludge-derived biochar catalysts for persulfate activation: Internal electron transfer mechanism. Chem Eng J 364:146–159. https://doi.org/10.1016/j.cej.2019.01.163
Zhang H, Tang L, Wang J, Yu J, Feng H, Lu Y, Chen Y, Liu Y, Wang J, Xie Q (2020) Enhanced surface activation process of persulfate by modified bagasse biochar for degradation of phenol in water and soil: active sites and electron transfer mechanism. Colloids Surf A 599:124904. https://doi.org/10.1016/j.colsurfa.2020.124904
Zhang P, Tan X, Liu S, Liu Y, Zeng G, Ye S, Yin Z, Hu X, Liu N (2019) Catalytic degradation of estrogen by persulfate activated with iron-doped graphitic biochar: process variables effects and matrix effects. Chem Eng J 378:122141. https://doi.org/10.1016/j.cej.2019.122141
Zhang Y, Zhou J, Chen X, Wang L, Cai W (2019) Coupling of heterogeneous advanced oxidation processes and photocatalysis in efficient degradation of tetracycline hydrochloride by Fe-based MOFs: synergistic effect and degradation pathway. Chem Eng J 369:745–757. https://doi.org/10.1016/j.cej.2019.03.108
Zhao Q, Mao Q, Zhou Y, Wei J, Liu X, Yang J, Luo L, Zhang J, Chen H, Chen H, Tang L (2017) Metal-free carbon materials-catalyzed sulfate radical-based advanced oxidation processes: a review on heterogeneous catalysts and applications. Chemosphere 189:224–238. https://doi.org/10.1016/j.chemosphere.2017.09.042
Zhu SS, Huang XC, Ma F, Wang L, Duan XG, Wang SB (2018) Catalytic removal of aqueous contaminants on N-doped graphitic biochars: inherent roles of adsorption and nonradical mechanisms. Environ Sci Technol 52:8649–8658. https://doi.org/10.1021/acs.est.8b01817
Funding
This work was provided by the National Natural Science Foundation of China under grants (No.21477050), the International Scientific and Technological Cooperation in Changzhou (CZ20140017), Changzhou Sci&Tech Program (CJ20200077), Natural Science Research Project of Higher Education Institutions in Jiangsu Province (19KJB560008), and Postgraduate Research Innovation Project of Jiangsu Province (KYCX20_2598, KYCX20_2561).
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YZ: conceptualization, investigation, methodology, formal analysis, writing—original draft, and writing—review and editing. SJ: supervision, project administration, writing—review and editing, and funding acquisition. LQ: conceptualization and resources. KX: resources, data curation, and software. XK: resources, data curation, and software. LW: supervision, project administration, and funding acquisition.
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Zhang, Y., Jiang, S., Qiu, L. et al. Performance and mechanism of tea waste biochar in enhancing the removal of tetracycline by peroxodisulfate. Environ Sci Pollut Res 29, 27595–27605 (2022). https://doi.org/10.1007/s11356-021-18285-6
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DOI: https://doi.org/10.1007/s11356-021-18285-6