Abstract
The tetracycline (TC) in water has led to serious concern. Graphitic carbon nitride (g-C3N4) photocatalysts were produced via copolymerization of mono-benzene ring-mediated precursors (urea, melamine, and dicyandiamide) involving salicylic acid (SA) for TC degradation. The SA-modified g-C3N4 samples showed improved visible light absorbance, transfer and separation of photogenerated electrons, and prospective photocatalytic application in TC degradation. As a result, the optimal SA-modified g-C3N4 (2 wt% of SA) using urea (CNU-SA-2) showed 2 times higher TC degradation than that of pristine g-C3N4. The process of TC degradation was evaluated by the reduction of antibacterial activity and extensively studied by varying the types of TC, initial pH values, co-existing anions, and natural organic materials. In addition, the catalyst could be reused for at least four cycles, indicating good reusability. The main active species were revealed to be h+ and ·O2− by scavenging experiments and electron spin resonance. The CNU-SA-2 photocatalyst and TC intermediates during degradation had no adverse impact on zebrafish embryos. This work could provide a design strategy and a perspective on the practical application of g-C3N4-based photocatalysts for the treatment of wastewater containing antibiotics.
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References
Chi X, Liu F, Gao Y, Song J, Guan R, Yuan H (2022) An efficient B/Na co-doped porous g-C3N4 nanosheets photocatalyst with enhanced photocatalytic hydrogen evolution and degradation of tetracycline under visible light. Appl Surf Sci 576:151837
Coledam DA, Aquino JM, Silva BF, Silva AJ, Rocha-Filho RC (2016) Electrochemical mineralization of norfloxacin using distinct boron-doped diamond anodes in a filter-press reactor, with investigations of toxicity and oxidation by-products. Electrochim Acta 213:856–864
Dong H, Guo X, Yang C, Ouyang Z (2018) Synthesis of g-C3N4 by different precursors under burning explosion effect and its photocatalytic degradation for tylosin. Appl Catal B-Environ 230:65–76
Du J, Xu Z, Li H, Yang H, Xu S, Wang J, Jia Y, Ma S, Zhan S (2021) Ag3PO4/g-C3N4 Z-scheme composites with enhanced visible-light-driven disinfection and organic pollutants degradation: uncovering the mechanism. Appl Surf Sci 541:148487
Feng J, Chen T, Liu S, Zhou Q, Ren Y, Lv Y, Fan Z (2016) Improvement of g-C3N4 photocatalytic properties using the Hummers method. J Colloid Interface Sci 479:1–6
Han C-H, Park H-D, Kim S-B, Yargeau V, Choi J-W, Lee S-H, Park J-A (2020) Oxidation of tetracycline and oxytetracycline for the photo-Fenton process: their transformation products and toxicity assessment. Water Res 172:115514
He Y, Peng G, Jiang Y, Zhao M, Wang X, Chen M, Lin S (2020) Environmental hazard potential of nano-photocatalysts determined by nano-bio interactions and exposure conditions. Small 16:e1907690
Jia L, Cheng X, Wang X, Cai H, He P, Ma J, Li L, Ding Y, Fan X (2019) Large-scale preparation of g-C3N4 porous nanotubes with enhanced photocatalytic activity by using salicylic acid and melamine. Ind Eng Chem Res 59:1065–1072
Li Z, Chen H, Liu W (2018) Full-spectrum photocatalytic activity of ZnO/CuO/ZnFe2O4 nanocomposite as a photoFenton-like catalyst. Catalysts 8:557
Li M, Li P, Zhang L, Chen M, Tang J, Qin C, Ling Jie Lee S, Lin S (2022) Facile fabrication of ZnO decorated ZnFe-layered double hydroxides @ biochar nanocomposites for synergistic photodegradation of tetracycline under visible light. Chem Eng J 434:134772
Lin S, Yu T, Yu Z, Hu X, Yin D (2018) Nanomaterials safer-by-design: an environmental safety perspective. Adv Mater 30:1705691
Lin B, Li S, Peng Y, Chen Z, Wang X (2021) MOF-derived core/shell C-TiO2/CoTiO3 type II heterojunction for efficient photocatalytic removal of antibiotics. J Hazard Mater 406:124675
Liu N, Lu N, Su Y, Wang P, Quan X (2019a) Fabrication of g-C3N4/Ti3C2 composite and its visible-light photocatalytic capability for ciprofloxacin degradation. Sep Purif Technol 211:782–789
Liu S, Wang S, Jiang Y, Zhao Z, Jiang G, Sun Z (2019b) Synthesis of Fe2O3 loaded porous g-C3N4 photocatalyst for photocatalytic reduction of dinitrogen to ammonia. Chem Eng J 373:572–579
Liu Y, Wang X, Sun Q, Yuan M, Sun Z, Xia S, Zhao J (2022) Enhanced visible light photo-Fenton-like degradation of tetracyclines by expanded perlite supported FeMo3Ox/g-C3N4 floating Z-scheme catalyst. J Hazard Mater 424:127387
Luo Z, Song Y, Wang M, Zheng X, Qu L, Wang J, Wu X, Wu Z (2020) Comparison of g-C3N4 synthesized by different precursors in remediation of phenanthrene contaminated soil and ecotoxicity. J Photoch Photobio A 389:112241
Osin OA, Yu T, Cai X, Jiang Y, Peng G, Cheng X, Li R, Qin Y, Lin S (2018) Photocatalytic degradation of 4-nitrophenol by C, N-TiO2: degradation efficiency vs. embryonic toxicity of the resulting compounds. Front Chem 6:192
Qin Y, Lu J, Zhao X, Lin X, Hao Y, Huo P, Meng M, Yan Y (2021) Nitrogen defect engineering and π-conjugation structure decorated g-C3N4 with highly enhanced visible-light photocatalytic hydrogen evolution and mechanism insight. Chem Eng J 425:131844
Sharma A, Saneja A (2022) Zebrafish as a powerful alternative model organism for preclinical investigation of nanomedicines. Drug Discov Today 27:1513–1522
Shi Y, Li J, Wan D, Huang J, Liu Y (2020) Peroxymonosulfate-enhanced photocatalysis by carbonyl-modified g-C3N4 for effective degradation of the tetracycline hydrochloride. Sci Total Environ 749:142313
Sun H, Guo F, Pan J, Huang W, Wang K, Shi W (2021) One-pot thermal polymerization route to prepare N-deficient modified g-C3N4 for the degradation of tetracycline by the synergistic effect of photocatalysis and persulfate-based advanced oxidation process. Chem Eng J 406:126844
Tang J, Wang J, Tang L, Feng C, Zhu X, Yi Y, Feng H, Yu J, Ren X (2022) Preparation of floating porous g-C3N4 photocatalyst via a facile one-pot method for efficient photocatalytic elimination of tetracycline under visible light irradiation. Chem Eng J 430:132669
Watkinson A, Murby E, Costanzo S (2007) Removal of antibiotics in conventional and advanced wastewater treatment: implications for environmental discharge and wastewater recycling. Water Res 41:4164–4176
Wei R, Ge F, Chen M, Huang S, Wang R (2010) Pollution of tetracyclines from livestock and poultry farms in aquatic environment in Jiangsu Province, China. J Agro-Environ Sci 29:1205
Xia P, Zhu B, Yu J, Cao S, Jaroniec M (2017) Ultra-thin nanosheet assemblies of graphitic carbon nitride for enhanced photocatalytic CO 2 reduction. J Mater Chem A 5:3230–3238
Xu L, Zhang H, Xiong P, Zhu Q, Liao C, Jiang G (2021) Occurrence, fate, and risk assessment of typical tetracycline antibiotics in the aquatic environment: a review. Sci Total Environ 753:141975
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
Yu Y, Wu K, Xu W, Chen D, Fang J, Zhu X, Sun J, Liang Y, Hu X, Li R (2021) Adsorption-photocatalysis synergistic removal of contaminants under antibiotic and Cr (VI) coexistence environment using non-metal g-C3N4 based nanomaterial obtained by supramolecular self-assembly method. J Hazard Mater 404:124171
Zhang J, Zhang G, Chen X, Lin S, Mohlmann L, Dolega G, Lipner G, Antonietti M, Blechert S, Wang X (2012) Co-monomer control of carbon nitride semiconductors to optimize hydrogen evolution with visible light. Angew Chem Int Ed Eng 51:3183–3187
Zhang Q, Jiang L, Wang J, Zhu Y, Pu Y, Dai W (2020) Photocatalytic degradation of tetracycline antibiotics using three-dimensional network structure perylene diimide supramolecular organic photocatalyst under visible-light irradiation. Appl Catal B-Environ 277:119122
Zhao T, Zheng M, Fu C, Li G, Xiong Y, Qiu W, Zhang T, Zhang J, Zheng C (2020) Effect of low-level H2O2 and Fe(II) on the UV treatment of tetracycline antibiotics and the toxicity of reaction solutions to zebrafish embryos. Chem Eng J 394:125021
Zhao G, Ding J, Zhou F, Chen X, Wei L, Gao Q, Wang K, Zhao Q (2021) Construction of a visible-light-driven magnetic dual Z-scheme BiVO4/g-C3N4/NiFe2O4 photocatalyst for effective removal of ofloxacin: mechanisms and degradation pathway. Chem Eng J 405:126704
Zhou C, Huang D, Xu P, Zeng G, Huang J, Shi T, Lai C, Zhang C, Cheng M, Lu Y, Duan A, Xiong W, Zhou M (2019a) Efficient visible light driven degradation of sulfamethazine and tetracycline by salicylic acid modified polymeric carbon nitride via charge transfer. Chem Eng J 370:1077–1086
Zhou C, Zeng Z, Zeng G, Huang D, Xiao R, Cheng M, Zhang C, Xiong W, Lai C, Yang Y, Wang W, Yi H, Li B (2019b) Visible-light-driven photocatalytic degradation of sulfamethazine by surface engineering of carbon nitride: properties, degradation pathway and mechanisms. J Hazard Mater 380:120815
Zhu A, Qiao L, Tan P, Pan J (2020) Interfaces of graphitic carbon nitride-based composite photocatalysts. Inorg Chem Front 7:4754–4793
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This work has received the finical support from the National Natural Science Foundation of China (No. 21777116) and the Fundamental Research Funds for the Central Universities.
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Mengmeng Chen: conceptualization, data curation, investigation, methodology, writing—review and editing. Mengxue Li: writing—review and editing. Peng Li: writing—review and editing. Stephanie Ling Jie Lee: writing—review and editing. Juanjuan Tang: data curation. Qian Li: data curation. Sijie Lin: project design, supervision, writing—review and editing, project administration, funding acquisition.
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Chen, M., Li, M., Li, P. et al. Enhanced visible light-driven photodegradation of tetracycline by salicylic acid-modified graphitic carbon nitride and toxicity assessment. Environ Sci Pollut Res 29, 90768–90778 (2022). https://doi.org/10.1007/s11356-022-22000-4
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DOI: https://doi.org/10.1007/s11356-022-22000-4