Abstract
In the present work, Er-doped BiFeO3 (BFO) nanoparticles (Bi(1−x)ErxFeO3, where x = 0.00, 0.01, 0.03, 0.05) containing different concentrations of Er dopants were successfully prepared through a facile sol gel method. The crystalline structure, morphological features, and chemical compositions of the obtained samples were examined by a variety of characterization techniques, and these samples were then used as photocatalysts for the photocatalytic removal of tetracycline hydrochloride (TC) upon visible light. The Er doping could significantly improve the optical absorption capability of the BFO especially in visible light range, and could also boost the photocatalytic activity of the BFO for TC removal. Among all the prepared photocatalysts, the Er3%-BFO sample yielded the highest photocatalytic efficiency of 75.8% for TC removal, which was nearly 2.78 times that of pure BFO. On the basis of the photocurrent response, electrochemical impedance spectra, and photoluminescence emission results, the contributions made on the significantly boosted photocatalytic activities of Er-doped BFO could be reflected on the following aspects: (i) the improved spectral absorption especially in visible light region, (ii) the promotion of photoinduced charge separation and migration, and (iii) the suppressed recombination probability of photogenerated electron–hole pairs. The present work demonstrates the feasibility of employing rare earth doping to develop highly efficient BFO-based photocatalysts for the photocatalytic removal of antibiotics.
Highlights
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Effective Er doping into BiFeO3 (BFO) nanoparticles was obtained by a facile sol–gel route.
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The optical absorption properties of BFO nanoparticles was improved by Er doping.
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Er-doped BFO nanoparticles showed superior photocatalytic activities for TC removal.
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The possible photocatalytic mechanism of Er-doped BFO nanoparticles was discussed.
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References
Homem V, Santos L (2011) Degradation and removal methods of antibiotics from aqueous matrices—a review. J Environ Manag 92:2304–2347
Bagheri S, Termehyousefi A (2017) Photocatalytic pathway toward degradation of environmental pharmaceutical pollutants: structure, kinetics and mechanism approach. Catal Sci Technol 7:4548–4569
Chong MN, Jin B, Chow CW, Saint C (2010) Recent developments in photocatalytic water treatment technology, a review. Water Res 44:2997–3027
He HY (2016) Facile synthesis of ultrafine CuS nanocrystalline/TiO2:Fe nanotubes hybrids and their photocatalytic and Fenton-like photocatalytic activities in the dye degradation. Microporous Mesoporous Mater 227:31–38
He HY (2017) Facile synthesis of Bi2S3 nanocrystalline-modified TiO2:Fe nanotubes hybrids and their photocatalytic activities in dye degradation. Part Sci Technol 35:410–417
He HY, Tian CY (2016) Rapid photo- and photo-Fenton-like catalytic removals of malachite green in aqueous solution on undoped and doped TiO2 nanotubes. Desalin Water Treat 57:14622–14631
Pan FM, Zhang B, Cai WH (2017) The effect of hydrophilicity/hydrophobicity of TiO2–SiO2 composite aerogels in the epoxidation reaction. Catal Commun 98:121–125
Xiang C, Guo RH, Lan JW, Jiang SX, Wang C, Du ZF, Cheng C (2018) Self-assembling porous 3D titanium dioxide-reduced graphene oxide aerogel for the tunable absorption of oleic acid and RhodamineB dye. J Alloys Compd 735:246–252
Cho CM, Noh JH, Cho IS, An JS, Hong KS, Kim JY (2008) Low-temperature hydrothermal synthesis of pure BiFeO3 nanopowders using triethanolamine and their applications as visible-light photocatalysts. J Am Ceram Soc 91:3753–3755
Joshi UA, Jang JS, Borse PH, Lee JS (2008) Microwave synthesis of single-crystalline perovskite BiFeO3 nanocubes for photoelectrode and photocatalytic applications. Appl Phys Lett 92:242106
Huo YN, Jin Y, Zhang Y (2010) Citric acid assisted solvothermal synthesis of BiFeO3 microspheres with high visible-light photocatalytic activity. J Mol Catal A Chem 331:15–20
Li ZX, Shen Y, Yang C, Lei YC, Guan YH, Lin YH, Liu DB, Nan W (2013) Significant enhancement in the visible light photocatalytic properties of BiFeO3–graphene nanohybrids. J Mater Chem A 1:823–829
Fei LF, Yuan JK, Hu YM, Wu CZ, Wang JL, Wang Y (2011) Visible light responsive perovskite BiFeO3 pills and rods with dominant {111}(c) facets. Cryst Growth Des 11:1049–1053
Guo RQ, Fang L, Dong W, Zheng FG, Shen MG (2010) Enhanced photocatalytic activity and ferromagnetism in gd doped BiFeO3 nanoparticles. J Phys Chem C 114:21390–21396
Niu F, Chen D, Qin LS, Gao T, Zhang N, Wang S, Chen Z, Wang JY, Sun XG, Huang YX (2015) Synthesis of Pt/BiFeO3 heterostructured photocatalysts for highly efficient visible-light photocatalytic performances. Sol Energy Mater Sol Cells 143:386–396
Niu F, Chen D, Qin L, Zhang N, Wang JY, Chen Z, Huang YX (2015) Facile synthesis of highly efficient p–n heterojunction CuO/BiFeO3 composite photocatalysts with enhanced visible-light photocatalytic activity. ChemCatChem 7:3279–3289
Mohan S, Subramanian B, Bhaumik I, Gupta PK, Jaisankar SN (2014) Nanostructured Bi(1−x)Gd(x)FeO3—a multiferroic photocatalyst on its sunlight driven photocatalytic activity. RSC Adv 4:16871–16878
Pei YL, Zhang C (2013) Effect of ion doping in different sites on the morphology and photocatalytic activity of BiFeO3 microcrystals. J Alloys Compd 570:57–60
Bingham S, Daoud WA (2011) Recent advances in making nano-sized TiO2 visible-light active through rare-earth metal doping J Mater Chem 21:2041–2050
Weber AS, Grady AM, Koodali RT (2012) Lanthanide modified semiconductor photocatalysts. Catal Sci Technol 2:683–693
Ranjit KT, Willner I, Bossmann SH, Braun AM (2001) Lanthanide oxide-doped titanium dioxide photocatalysts: novel photocatalysts for the enhanced degradation of p-chlorophenoxyacetic acid. Environ Sci Technol 35:1544–1549
Yang Y, Zhang CC, Xu Y, Wang HY, Li X, Wang C (2010) Electrospun Er:TiO2 nanofibrous films as efficient photocatalysts under solar simulated light. Mater Lett 64:147–150
Bharathkumar S, Sakar M, Ponpandian N, Balakumar S (2018) Dual oxidation state induced oxygen vacancies in Pr substituted BiFeO3 compounds: an effective material activation strategy to enhance the magnetic and visible light-driven photocatalytic properties. Mater Res Bull 101:107–115
Chen ZW, Wu YP, Wang X, Jin WL, Zhu CB (2015) Ferromagnetism and enhanced photocatalytic activity in Nd doped BiFeO3 nanopowders. J Mater Sci Mater Electron 26:9929–9940
Hu ZJ, Chen D, Wang S, Zhang N, Qin LS, Huang YX (2017) Facile synthesis of Sm-doped BiFeO3 nanoparticles for enhanced visible light photocatalytic performance. Mater Sci Eng B Adv Funct Solid-State Mater 220:1–12
Sakar M, Balakumar S, Saravanan P, Bharathkumar S (2015) Compliments of confinements: substitution and dimension induced magnetic origin and band-bending mediated photocatalytic enhancements in Bi1−xDyxFeO3 particulate and fiber nanostructures. Nanoscale 7:10667–10679
Obregóna S, Colón G (2012) Evidence of upconversion luminescence contribution to the improved photoactivity of erbium doped TiO2 systems. Chem Commun 48:7865–7867
Wang T, Song SH, Xu T, Wang M (2016) Maltose-assisted sol–gel synthesis, structural, magnetic and optical properties of multiferroic BiFeO3 nanopowders. J Sol-Gel Sci Technol 80:675–682
Chen C, Cheng JR, Yu SW, Che LJ, Meng ZY (2006) Hydrothermal synthesis of perovskite bismuth ferrite crystallites. J Cryst Growth 291:135–139
Maurya D, Thota H, Nalwa KS, Garg A (2009) BiFeO3 ceramics synthesized by mechanical activation assisted versus conventional solid-state-reaction process: a comparative study. J Alloys Compd 477:780–784
Wang YP, Zhou L, Zhang MF, Chen XY, Liu JM, Liu ZG (2004) Room-temperature saturated ferroelectric polarization in BiFeO3 ceramics synthesized by rapid liquid phase sintering. Appl Phys Lett 84:1731–1733
Shokrollahi H (2013) Magnetic, electrical and structural characterization of BiFeO3 nanoparticles synthesized by co-precipitation. Powder Technol 235:953–958
Das N, Majumdar R, Sen A, Maiti HS (2007) Nanosized bismuth ferrite powder prepared through sonochemical and microemulsion techniques. Mater Lett 61:2100–2104
Gao T, Chen Z, Zhu YX, Niu F, Huang QL, Qin LS, Sun XG, Huang YX (2014) Synthesis of BiFeO3 nanoparticles for the visible-light induced photocatalytic property. Mater Res Bull 59:6–12
Zhang N, Chen D, Niu F, Wang S, Qin LS, Huang YX (2016) Enhanced visible light photocatalytic activity of Gd-doped BiFeO3 nanoparticles and mechanism insight Sci Rep 6:26467
Xing WY, Ma Y, Ma Z, Bai YL, Chen JY, Zhao SF (2014) Improved ferroelectric and leakage current properties of Er-doped BiFeO3 thin films derived from structural transformation. Smart Mater Struct 23:085030
Yang YC, Zhang T, Le L, Ruan XF, Fang PF, Pan CX, Xiong R, Shi J, Wei JH (2014) Quick and facile preparation of visible light-driven TiO2 photocatalyst with high absorption and photocatalytic activity. Sci Rep 4:7045–7052
Yu CL, Yang K, Xie Y, Fan QZ, Yu JC, Shu Q, Wang CY (2013) Novel hollow Pt-ZnO nanocomposite microspheres with hierarchical structure and enhanced photocatalytic activity and stability. Nanoscale 5:2142–2151
Zhao YK, Liu YD, Du XQ, Han RX, Ding Y (2014) Hexagonal assembly of Co3V2O8 nanoparticles acting as an efficient catalyst for visible light-driven water oxidation. J Mater Chem A 2:19308–19314
Mao CY, Li WJ, Wu F, Dou YY, Fang L, Ruan HB, Kong CY (2015) Effect of Er doping on microstructure and optical properties of ZnO thin films prepared by sol–gel method. J Mater Sci Mater Electron 26:8732–8739
Maneeshya LV, Thomas PV, Joy K (2015) Effects of site substitutions and concentration on the structural, optical and visible photoluminescence properties of Er doped BaTiO3 thin films prepared by RF magnetron sputtering. Opt Mater 46:304–309
Clementi C, Miliani C, Verri G, Sotiropoulou S, Romani A, Brunetti BG, Sgamellotti A (2009) Application of the Kubelka–Munk correction for self-adsorption of fluorescence emission in carmine lake paint layers. Appl Spectrosc 63:1323–1329
Tao R, Shao CL, Li XH, Li XW, Liu S, Yang S, Zhao CC, Liu YC (2018) Bi2MoO6/BiFeO3 heterojunction nanofibers: enhanced photocatalytic activity, charge separation mechanism and magnetic separability. J Colloid Interface Sci 529:404–414
Gong YY, Wu YJ, Xu Y, Li L, Li C, Liu XJ, Niu LY (2018) All-solid-state Z-scheme CdTe/TiO2 heterostructure photocatalysts with enhanced visible-light photocatalytic degradation of antibiotic waste water. Chem Eng J 350:257–267
Jiang YH, Jing X, Zhu K, Peng ZY, Zhang JM, Liu Y, Zhang WL, Ni L, Liu ZC (2018) Ta3N5 nanoparticles/TiO2 hollow sphere (0D/3D) heterojunction: facile synthesis and enhanced photocatalytic activities of levofloxacin degradation and H2 evolution. Dalton Trans 47:13113–13125
Shen XF, Song LL, Luo L, Zhang Y, Zhu B, Liu JS, Chen ZG, Zhang LS (2018) Preparation of TiO2/C3N4 heterojunctions on carbon-fiber cloth as efficient filter-membrane-shaped photocatalyst for removing various pollutants from the flowing wastewater. J Colloid Interface Sci 532:798–807
He L, Dong YN, Zhang YN, Jia QM, Shan SY, Zhang YQ (2019) A novel magnetic MIL-101(Fe)/TiO2 composite for photo degradation of tetracycline under solar light. J Hazard Mater 361:85–94
Shi YY, Yang ZW, Wang B, An H, Chen ZZ, Cui H (2016) Adsorption and photocatalytic degradation of tetracycline hydrochloride using a palygorskite-supported Cu2O–TiO2 composite. Appl Clay Sci 119:311–320
Ma SS, Li R, Lv CP, Xu W, Gou XL (2011) Facile synthesis of ZnO nanorod arrays and hierarchical nanostructures for photocatalysis and gas sensor applications. J Hazard Mater 192:730–740
Akpan UG, Hameed BH (2010) The advancements in sol–gel method of doped-TiO2 photocatalysts. Appl Catal A Gen 375:1–11
Minero C, Mariella G, Maurino V, Vione D, Pelizzetti E (2000) Photocatalytic transformation of organic compounds in the presence of inorganic ions. 2. Competitive reactions of phenol and alcohols and titanium dioxide–fluoride system. Langmuir 16:8964–8972
Tian Y, Chang B, Lu J, Fu J, Xi F, Dong X (2013) Hydrothermal synthesis of graphitic carbon nitride–Bi2WO6 heterojunctions with enhanced visible light photocatalytic activities. ACS Appl Mater Interfaces 5:7079–7085
Li WJ, Li DZ, Lin YM, Wang PX, Chen W, Fu XZ, Shao Y (2012) Evidence for the active species involved in the photodegradation process of methyl orange on TiO2. J Phys Chem C 116:3552–3560
Kim HG, Borse PH, Choi W, Lee JS (2010) Photocatalytic nanodiodes for visible-light photocatalysis. Angew Chem Int Ed 117:4661–4665
Hong SJ, Lee S, Jang JS, Lee JS (2011) Heterojunction BiVO4/WO3 electrodes for enhanced photoactivity of water oxidation. Energy Environ Sci 4:1781–1787
Shiraishi Y, Takeshita S, Isobe T (2015) Two photoenergy conversion modes of YVO4:Eu3+ nanoparticles: photoluminescence and photocatalytic activity. J Phys Chem C 119:13502–13508
Bhethanabotla VC, Russell DR, Kuhn JN (2017) Assessment of mechanisms for enhanced performance of Yb/Er/titania photocatalysts for organic degradation: role of rare earth elements in the titania phase. Appl Catal B Environ 202:156–164
Tobaldi DM, Ferreira RAS, Pullar RC, Seabra MP, Carlos LD, Labrincha JA (2015) Nano-titania doped with europium and neodymium showing simultaneous photoluminescent and photocatalytic behaviour. J Mater Chem C 3:4970–4986
Chang MQ, Zou HF, Song YH, Chen J, Cui L, Sheng Y, Zheng KY (2019) Photoluminescence and photodegradation properties of SiO2@TiO2:Sm3+ with different coating effects. J Phys Chem Solids 124:100–110
Acknowledgements
The authors are grateful for the financial support from the Zhejiang Provincial Natural Science Foundation of China (No. LY17E020009), National Natural Science Foundation of China (Nos. 51872271 and 51572250), the National Key Research and Development Program of China (No. 2017YFF0204701), CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, China (No. 2013DP173231), Zhejiang Provincial Key Lab for Chem & Bio Processing Technology of Farm Products (No. 2016KF0002).
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Zhou, J., Jiang, L., Chen, D. et al. Facile synthesis of Er-doped BiFeO3 nanoparticles for enhanced visible light photocatalytic degradation of tetracycline hydrochloride. J Sol-Gel Sci Technol 90, 535–546 (2019). https://doi.org/10.1007/s10971-019-04932-5
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DOI: https://doi.org/10.1007/s10971-019-04932-5