Abstract
Acetaminophen (AP) is a widely used antipyretic analgesic belonging to the class of PPCPs, which is difficult to be effectively degraded by traditional water treatment processes. However, photocatalytic technology may be an effective approach. Herein, B-doped TiO2 photocatalytic materials were synthesized by sol–gel method, calcinated at 600℃ for 2 h, investigated by XRD, TEM, XPS, and other characterization methods. The photocatalytic efficiency and factors affecting the photocatalytic activity were assessed by degradation of AP under 365 nm UV light. Compared with undoped TiO2, 4%B-TiO2 nanopowder has smaller grain size, higher porosity, and lower bandgap energy of 3.11 eV. Scavenging experiments and ESR results show that •OH is the principal active species. Hence, the degradation efficiency of AP is as high as 98.8% in 30 min when adopting 10-mg/L AP initial concentration and 1-g/L 4%B-TiO2 loading, owing to efficient •OH generated by B-TiO2.
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References
Abdelaal MY, Mohamed RM (2013) Novel Pd/TiO2 nanocomposite prepared by modified sol–gel method for photocatalytic degradation of methylene blue dye under visible light irradiation. J Alloy Compd 576:201–207
Akpan UG, Hameed BH (2010) The advancements in sol–gel method of doped-TiO2 photocatalysts. Appl Catal A 375:1–11
Almeida F, Nunes B (2019) Effects of acetaminophen in oxidative stress and neurotoxicity biomarkers of the gastropod Phorcus lineatus. Environ Sci Pollut Res Int 26:9823–9831
BilginSimsek E (2017) Solvothermal synthesized boron doped TiO2 catalysts: photocatalytic degradation of endocrine disrupting compounds and pharmaceuticals under visible light irradiation. Appl Catal B 200:309–322
Cai H, Zhang D, Ma X, Ma Z (2022) A novel ZnO/biochar composite catalysts for visible light degradation of metronidazole. Sep Purif Technol 288:120633
Chen X, Peng X, Jiang L, Yuan X, Zhang J, Yu H (2020) Terephthalate acid decorated TiO2 for visible light driven photocatalysis mediated via ligand-to-metal charge transfer (LMCT). Colloids Surf A 603:125188
Fan G, Ning R, Yan Z, Luo J, Du B, Zhan J, Liu L, Zhang J (2021) Double photoelectron-transfer mechanism in Ag-AgCl/WO3/g-C3N4 photocatalyst with enhanced visible-light photocatalytic activity for trimethoprim degradation. J Hazard Mater 403:123964
Ganesh I (2018) Surface, structural, energy band-gap, and photocatalytic features of an emulsion-derived B-doped TiO2 nano-powder. Molecular Catalysis 451:51–65
Hasan N, Moon G-h, Park J, Park J, Kim J (2018) Visible light-induced degradation of sulfa drugs on pure TiO2 through ligand-to-metal charge transfer. Sep Purif Technol 203:242–250
Jin X, Wu Y, Lin Z, Liang D, Wang F, Zheng X, Liu H, Lv W, Liu G (2022) Plasmonic Ag nanoparticles decorated copper-phenylacetylide polymer for visible-light-driven photocatalytic reduction of Cr(VI) and degradation of PPCPs: performance, kinetics, and mechanism. J Hazard Mater 425:127599
Koysuren O, Koysuren HN (2019) Photocatalytic activities of boron doped titanium dioxide nanoparticles and its composite with polyaniline. J Macromol Sci Part B Phys 59:182–195
Kumar S, Khanchandani S, Thirumal M, Ganguli AK (2014) Achieving enhanced visible-light-driven photocatalysis using type-II NaNbO3/CdS core/shell heterostructures. ACS Appl Mater Interfaces 6:13221–13233
Leyva E, Moctezuma E, Baines KM, Noriega S, Zarazua E (2018) A review on chemical advanced oxidation processes for pharmaceuticals with paracetamol as a model compound. Reaction conditions, intermediates and total mechanism. Curr Org Chem 22:2–17
Li H, Zhang W, Liu Y (2020) HZSM-5 zeolite supported boron-doped TiO2 for photocatalytic degradation of ofloxacin. J Market Res 9:2557–2567
Li W (2015) Influence of electronic structures of doped TiO2 on their photocatalysis. Physica Status Solidi (RRL) - Rapid Res Lett 9:10–27
Liu J, Zou Y, Cruz D, Savateev A, Antonietti M, Vile G (2021a) Ligand-metal charge transfer induced via adjustment of textural properties controls the performance of single-atom catalysts during photocatalytic degradation. ACS Appl Mater Interfaces 13:25858–25867
Liu X, Zhu L, Wang X, Meng X (2020a) Photocatalytic degradation of wastewater by molecularly imprinted Ag2S-TiO2 with high-selectively. Sci Rep 10:1192
Liu X, Zhu L, Wang X, Meng X (2020b) One-step synthesis of Ag2S-TiO2 and its photocatalytic degradation of ethyl paraben wastewater. Environ Sci Pollut Res Int 27:13590–13598
Liu X, Zhu L, Wang X, Meng X, Zhong L (2020c) The photocatalytic selectivity between molecularly imprinted TiO2 and target contaminants. J Nanopart Res 22:300
Liu X, Xu C, Zhu L, Xie S, Shen S, Wang X (2021b) One-step facile synthesis of shell-pearl structured photocatalysts for efficient removal of selected PPCPs from wastewater. J Environ Chem Eng 9:106758
Liu X, Zhou J, Liu D, Li L, Liu W, Liu S, Feng C (2021c) Construction of Z-scheme CuFe2O4/MnO2 photocatalyst and activating peroxymonosulfate for phenol degradation: synergistic effect, degradation pathways, and mechanism. Environ Res 200:111736
Liu X, Shen S, Xu C, Li X, Zhu L, Wang X (2022a) Studying photocatalytic dye degradation with bismuth nitrate–derived catalysts using paper microzones method. Mater Today Chem 23:100667
Liu X, Xu C, Xiao C, Tang Y, Chen X, Chen Y, Si Y, Zhu L, Wang X (2022b) Insights into the evaluation of photocatalytic quenching experimental results by degrading a dye. Res Chem Intermed 48:2915–2932
Liu X, Xu C, Zhu L, Wang X (2022c) Molecular imprinting produces high photoelectric effect facilitating the efficient photocatalytic degradation of salicylic acid by TiO2. React Kinet Mech Catal 135:529–537
Liu Y, Xia P, Li L, Wang X, Meng J, Yang Y, Guo Y (2020d) In-situ route for the graphitized carbon/TiO2 composite photocatalysts with enhanced removal efficiency to emerging phenolic pollutants. Chin J Catal 41:1378–1392
Loddo V, Bellardita M, Camera-Roda G, Parrino F, Palmisano L (2018) Heterogeneous photocatalysis. Current trends and future developments on (Bio-) membranes, pp. 1–43. Elsevier
Meng Y, Hong Y, Huang C, Shi W (2017) Fabrication of novel Z-scheme InVO4/CdS heterojunctions with efficiently enhanced visible light photocatalytic activity. CrystEngComm 19:982–993
Mostafa MMH, Zhang L, Zhu L, Wang X, Tao X, Liu X, Manickam S (2021) Photocatalytic degradation of ethyl paraben wastewater by mixed crystal molecularly imprinted TiO2. E3S Web Conf 261:02025
Phong Vo HN, Le GK, Hong Nguyen TM, Bui XT, Nguyen KH, Rene ER, Vo TDH, Thanh Cao ND, Mohan R (2019) Acetaminophen micropollutant: historical and current occurrences, toxicity, removal strategies and transformation pathways in different environments. Chemosphere 236:124391
Qin C, Tang J, Qiao R, Lin S (2022) Tetracycline sensitizes TiO2 for visible light photocatalytic degradation via ligand-to-metal charge transfer. Chin Chem Lett 33:5218–5222
Rabhi S, Mahtout L, Bououdina M, Khezami L, Belkacemi H, Kerrami A, Sakher E (2021) Tuning the photocatalytic activity of TiO2 by Ag loading: experimental and modelling studies for the degradation of amlodipine besylate drug. Ceram Int 47:21509–21521
Sin J-C, Lam S-M, Zeng H, Lin H, Li H, Tham K-O, Mohamed AR, Lim J-W, Qin Z (2021) Magnetic NiFe2O4 nanoparticles decorated on N-doped BiOBr nanosheets for expeditious visible light photocatalytic phenol degradation and hexavalent chromium reduction via a Z-scheme heterojunction mechanism. Appl Surf Sci 559:149966
Solis-Casados DA, Escobar-Alarcón L, Natividad R, Romero R (2018) Advanced Oxidation Processes II: removal of pharmaceuticals by photocatalysis, ecopharmacovigilance. The Handbook of Environmental Chemistry, Springer, pp. 143–155
Tao X, Zhu L, Wang X, Chen X, Liu X (2022) Preparation of Zr/Y co-doped TiO2 photocatalyst and degradation performance of hydroquinone. Environ Sci Pollut Res Int 29:40854–40864
Varma KS, Tayade RJ, Shah KJ, Joshi PA, Shukla AD, Gandhi VG (2020) Photocatalytic degradation of pharmaceutical and pesticide compounds (PPCs) using doped TiO2 nanomaterials: a review. Water-Energy Nexus 3:46–61
Vile G, Sharma P, Nachtegaal M, Tollini F, Moscatelli D, Sroka-Bartnicka A, Tomanec O, Petr M, Filip J, Pieta IS, Zboril R, Gawande MB (2021) An earth-abundant Ni-based single-atom catalyst for selective photodegradation of pollutants. Solar Rrl 5(7). https://doi.org/10.1002/solr.202100176
Vilé G (2021) Photocatalytic materials and light-driven continuous processes to remove emerging pharmaceutical pollutants from water and selectively close the carbon cycle. Catal Sci Technol 11:43–61
Wang L, Wang Y, Li X, He T, Wang R, Zhao Y, Song H, Wang H (2021) 3D/2D Fe2O3/g-C3N4 Z-scheme heterojunction catalysts for fast, effective and stable photo Fenton degradation of azo dyes. J Environ Chem Eng 9:105907
Xia L, Yang Y, Cao Y, Liu B, Li X, Chen X, Song H, Zhang X, Gao B, Fu J (2019) Porous N-doped TiO2 nanotubes arrays by reverse oxidation of TiN and their visible-light photocatalytic activity. Surf Coat Technol 365:237–241
Yadav V, Verma P, Sharma H, Tripathy S, Saini VK (2020) Photodegradation of 4-nitrophenol over B-doped TiO2 nanostructure: effect of dopant concentration, kinetics, and mechanism. Environ Sci Pollut Res Int 27:10966–10980
Yang L, Zhao Y, Liu Y, Zhang W (2019) Sol–gel synthesis of B-TiO2(20%)/HZSM-5 composite photocatalyst for azophloxine degradation. J Sol-Gel Sci Technol 93:371–379
Ye C, Zhang W, Liu Y (2020) Supporting B-TiO2 on iM16K glass bubbles to prepare B–TiO2(x%)/iM16K hollow spheres for ofloxacin degradation. Ceram Int 46:10545–10554
Zhang F, Zhao L, Chen H, He Y, Tian P, Zeng X (2019) Synthesis of mesoporous Fe/h-CeO2 hollow micro-spheres with enhanced visible light photocatalytic activity. Mater Res Express 6:099516
Zhang M, Lin X, Yi Z, Xu X, Yang J, Zhu M (2023) Enhanced reactive oxidation species generation by ligand-to-metal-charge transfer between oxygen vacancy-rich ZnO mesocrystal with ciprofloxacin pollutants. Appl Catal B 321:122033
Zhang W, Liu Y, Xin H (2018) Sol-gel preparation of hollow spherical x%B-TiO2 photocatalyst: The effect of boron content on RBR X-3B decoloration. Curr Nanosci 14:209–215
Zhang Y, Cheng Y, Qi H (2022) Synergistic degradation of organic pollutants on CoFe2O4/rGO nanocomposites by peroxymonosulfate activation under LED irradiation. Appl Surf Sci 579:152151
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This work is supported by the National Natural Science Foundation of China (51672196). This article is also supported by the Graduate Innovation and Entrepreneurship Fund Project of Wuhan University of Science and Technology (JCX2021016).
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Caofan Xiao conceived, designed the experiments, and wrote the manuscript. Xueqi Chen and Xiumei Tao provided suggestions for the study. Xian Liu supervised the progress of experiments, provided suggestions, and reviewed papers. Xun Wang provided suggestions and financial support. Lei Zhu reviewed the first draft. All authors discussed the results and contributed to the final manuscript.
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Xiao, C., Chen, X., Tao, X. et al. In situ generation of hydroxyl radicals by B-doped TiO2 for efficient photocatalytic degradation of acetaminophen in wastewater. Environ Sci Pollut Res 30, 46997–47011 (2023). https://doi.org/10.1007/s11356-023-25390-1
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DOI: https://doi.org/10.1007/s11356-023-25390-1