Abstract
An effective catalyst of MIL-101(Fe)/TiO2 composite was synthesized by solvothermal method. The resultant MIL-101(Fe)/TiO2 was used for advanced oxidation degradation of tetracycline (TC) for the first time. The results indicated that the MIL-101(Fe)/TiO2 showed higher TC degradation efficiency than pure MIL-101(Fe) or TiO2 with the persulfate. Using 1 g L−1 MIL-101(Fe)/TiO2 and persulfate at pH 7, 90.15% degradation rate was achieved under xenon lamp irradiation in 5 min for 20 mg L−1 TC. TiO2 introduced in the composite played an important role in the degradation process, in which TiO2 had a synergetic effect with Fe3+ to generate Fe2+, Ti3+ and radicals. Fe2+ reacted with persulfate to produce Fe3+ and a number of ·OH to degrade TC. This reaction process was so fast that MIL-101(Fe)/TiO2 with persulfate could degrade TC fairly rapidly. A novel TiO2-based metal–organic frameworks (MOFs) composite was more efficient for degrading pharmaceutical wastewater.
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C. Liu, G. Wu, J. Chen, K. Huang, W. Shi, Fabrication of a visible-light-driven photocatalyst and degradation of tetracycline based on the photoinduced interfacial charge transfer of SrTi3/Fe2O3 nanowires. New J. Chem. 40, 5198–5208 (2016)
Y.-Y. Chen, Y.-L. Ma, J. Yang, L.-Q. Wang, J.-M. Lv, C.-J. Ren, Aqueous tetracycline degradation by H2O2 alone: removal and transformation pathway. Chem. Eng. J. 307, 15–23 (2017)
H. Liu, G. Zhang, C. Liu, L. Li, M. Xiang, Characteristics of chloramphenicol and tetracyclines in municipal sewage and Nanming River of Guiyang City, China. Huan jing ke xue Huanjing kexue 30, 687–692 (2009)
Y. Jiang, M. Li, C. Guo, D. An, J. Xu, Y. Zhang, B. Xi, Distribution and ecological risk of antibiotics in a typical effluent–receiving river (Wangyang River) in north China. Chemosphere 112, 267–274 (2014)
A. Selvam, K. Kwok, Y. Chen, A. Cheung, K.S. Leung, J.W. Wong, Influence of livestock activities on residue antibiotic levels of rivers in Hong Kong. Environ. Sci. Pollut. Res. 24, 9058–9066 (2017)
S.-Z. Li, X.-Y. Li, D.-Z. Wang, Membrane (RO-UF) filtration for antibiotic wastewater treatment and recovery of antibiotics. Sep. Purif. Technol. 34, 109–114 (2004)
J. Radjenović, M. Petrović, F. Ventura, D. Barceló, Rejection of pharmaceuticals in nanofiltration and reverse osmosis membrane drinking water treatment. Water Res. 42, 3601–3610 (2008)
K. Košutić, D. Dolar, D. Ašperger, B. Kunst, Removal of antibiotics from a model wastewater by RO/NF membranes. Sep. Purif. Technol. 53, 244–249 (2007)
V. Homem, L. Santos, Degradation and removal methods of antibiotics from aqueous matrices–a review. J. Environ. Manag. 92, 2304–2347 (2011)
K.-J. Choi, S.-G. Kim, S.-H. Kim, Removal of antibiotics by coagulation and granular activated carbon filtration. J. Hazard. Mater. 151, 38–43 (2008)
J.L. Rowsell, O.M. Yaghi, Metal–organic frameworks: a new class of porous materials. Microporous Mesoporous Mater. 73, 3–14 (2004)
Y. Belmabkhout, R.S. Pillai, D. Alezi, O. Shekhah, P.M. Bhatt, Z. Chen, K. Adil, S. Vaesen, G. De Weireld, M. Pang, Metal–organic frameworks to satisfy gas upgrading demands: fine-tuning the soc-MOF platform for the operative removal of H 2 S. J. Mater. Chem. A 5, 3293–3303 (2017)
T. Hu, H. Lv, S. Shan, Q. Jia, H. Su, N. Tian, S. He, Porous structured MIL-101 synthesized with different mineralizers for adsorptive removal of oxytetracycline from aqueous solution. RSC Adv. 6, 73741–73747 (2016)
T. Hu, Q. Jia, S. He, S. Shan, H. Su, Y. Zhi, L. He, Novel functionalized metal-organic framework MIL-101 adsorbent for capturing oxytetracycline. J. Alloys Compd. 727, 114–122 (2017)
N. Tian, Q. Jia, H. Su, Y. Zhi, A. Ma, J. Wu, S. Shan, The synthesis of mesostructured NH2-MIL-101 (Cr) and kinetic and thermodynamic study in tetracycline aqueous solutions. J. Porous Mater. 23, 1269–1278 (2016)
K. Rajeshwar, J.G. Ibanez, Environmental Electrochemistry: Fundamentals and Applications in Pollution Sensors and Abatement (Elsevier, San Diego, 1997)
M. Miyata, I. Ihara, G. Yoshid, K. Toyod, K. Umetsu, Electrochemical oxidation of tetracycline antibiotics using a Ti/IrO2 anode for wastewater treatment of animal husbandry. Water Sci. Technol. 63, 456–461 (2011)
M. Panizza, G. Cerisola, Direct and mediated anodic oxidation of organic pollutants. Chem. Rev. 109, 6541–6569 (2009)
L. Hou, L. Wang, S. Royer, H. Zhang, Ultrasound-assisted heterogeneous Fenton-like degradation of tetracycline over a magnetite catalyst. J. Hazard. Mater. 302, 458–467 (2016)
S. Yang, P. Wang, X. Yang, L. Shan, W. Zhang, X. Shao, R. Niu, Degradation efficiencies of azo dye Acid Orange 7 by the interaction of heat, UV and anions with common oxidants: persulfate, peroxymonosulfate and hydrogen peroxide. J. Hazard. Mater. 179, 552–558 (2010)
C. Tan, N. Gao, Y. Deng, W. Rong, S. Zhou, N. Lu, Degradation of antipyrine by heat activated persulfate. Sep. Purif. Technol. 109, 122–128 (2013)
Y. Lei, C.-S. Chen, Y.-J. Tu, Y.-H. Huang, H. Zhang, Heterogeneous degradation of organic pollutants by persulfate activated by CuO-Fe3O4: mechanism, stability, and effects of pH and bicarbonate ions. Environ. Sci. Technol. 49, 6838–6845 (2015)
P. Villegas-Guzman, J. Silva-Agredo, O. Florez, A.L. Giraldo-Aguirre, C. Pulgarin, R.A. Torres-Palma, Selecting the best AOP for isoxazolyl penicillins degradation as a function of water characteristics: effects of pH, chemical nature of additives and pollutant concentration. J. Environ. Manag. 190, 72–79 (2017)
L.W. Matzek, K.E. Carter, Sustained persulfate activation using solid iron: kinetics and application to ciprofloxacin degradation. Chem. Eng. J. 307, 650–660 (2017)
G.P. Anipsitakis, D.D. Dionysiou, Radical generation by the interaction of transition metals with common oxidants. Environ. Sci. Technol. 38, 3705–3712 (2004)
L. Bu, S. Zhou, Z. Shi, C. Bi, S. Zhu, N. Gao, Iron electrode as efficient persulfate activator for oxcarbazepine degradation: performance, mechanism, and kinetic modeling. Sep. Purif. Technol. 178, 66–74 (2017)
Y. Gao, S. Li, Y. Li, L. Yao, H. Zhang, Accelerated photocatalytic degradation of organic pollutant over metal-organic framework MIL-53 (Fe) under visible LED light mediated by persulfate. Appl. Catal. B 202, 165–174 (2017)
X. Li, W. Guo, Z. Liu, R. Wang, H. Liu, Fe-based MOFs for efficient adsorption and degradation of acid orange 7 in aqueous solution via persulfate activation. Appl. Surf. Sci. 369, 130–136 (2016)
G. Férey, C. Mellot-Draznieks, C. Serre, F. Millange, J. Dutour, S. Surblé, I. Margiolaki, A chromium terephthalate-based solid with unusually large pore volumes and surface area. Science 309, 2040–2042 (2005)
Y.K. Seo, J.W. Yoon, J.S. Lee, Y.K. Hwang, C.H. Jun, J.S. Chang, S. Wuttke, P. Bazin, A. Vimont, M. Daturi, Energy-efficient dehumidification over hierachically porous metal-organic frameworks as advanced water adsorbents. Adv. Mater. 24, 806–810 (2012)
K.-Y.A. Lin, H.-A. Chang, C.-J. Hsu, Iron-based metal organic framework, MIL-88A, as a heterogeneous persulfate catalyst for decolorization of Rhodamine B in water. RSC Adv. 5, 32520–32530 (2015)
S. Rodriguez, L. Vasquez, D. Costa, A. Romero, A. Santos, Oxidation of Orange G by persulfate activated by Fe(II), Fe(III) and zero valent iron (ZVI). Chemosphere 101, 86–92 (2014)
D. Han, J. Wan, Y. Ma, Y. Wang, Y. Li, D. Li, Z. Guan, New insights into the role of organic chelating agents in Fe(II) activated persulfate processes. Chem. Eng. J. 269, 425–433 (2015)
J.J.M. Vequizo, H. Matsunaga, T. Ishiku, S. Kamimura, T. Ohno, A. Yamakata, Trapping-induced enhancement of photocatalytic activity on brookite TiO2 powders: comparison with anatase and rutile TiO2 powders. ACS Catal. 7, 2644–2651 (2017)
R.C. Gilson, K.C. Black, D.D. Lane, S. Achilefu, Hybrid TiO2–Ruthenium Nano-photosensitizer Synergistically Produces Reactive Oxygen Species in both Hypoxic and Normoxic Conditions. Angew. Chem. Int. Ed. 56, 10717–10720 (2017)
T. Tong, J. Zhang, B. Tian, F. Chen, D. He, Preparation of Fe3+-doped TiO2 catalysts by controlled hydrolysis of titanium alkoxide and study on their photocatalytic activity for methyl orange degradation. J. Hazard. Mater. 155, 572–579 (2008)
I.Y. Skobelev, A.B. Sorokin, K.A. Kovalenko, V.P. Fedin, O.A. Kholdeeva, Solvent-free allylic oxidation of alkenes with O2 mediated by Fe-and Cr-MIL-101. J. Catal. 298, 61–69 (2013)
S. Bauer, C. Serre, T. Devic, P. Horcajada, J. Marrot, G. Ferey, N. Stock, High-throughput assisted rationalization of the formation of metal organic frameworks in the iron (III) aminoterephthalate solvothermal system. Inorg. Chem. 47, 7568–7576 (2008)
M. Hartmann, M. Fischer, Amino-functionalized basic catalysts with MIL-101 structure. Microporous Mesoporous Mater. 164, 38–43 (2012)
F. Cui, Q. Deng, L. Sun, Prussian blue modified metal–organic framework MIL-101 (Fe) with intrinsic peroxidase-like catalytic activity as a colorimetric biosensing platform. RSC Adv. 5, 98215–98221 (2015)
J. Tang, M. Yang, M. Yang, J. Wang, W. Dong, G. Wang, Heterogeneous Fe-MIL-101 catalysts for efficient one-pot four-component coupling synthesis of highly substituted pyrroles. New J. Chem. 39, 4919–4923 (2015)
L. He, Y. Dong, Y. Zheng, Q. Jia, S. Shan, Y. Zhang, A novel magnetic MIL-101 (Fe)/TiO2 composite for photo degradation of tetracycline under solar light. J. Hazard. Mater. 361, 85–94 (2019)
A. Murashkevich, A. Lavitskaya, T. Barannikova, I. Zharskii, Infrared absorption spectra and structure of TiO2-SiO2 composites. J. Appl. Spectrosc. 75, 730–734 (2008)
T. Bezrodna, G. Puchkovska, V. Shymanovska, J. Baran, H. Ratajczak, IR-analysis of H-bonded H2O on the pure TiO2 surface. J. Mol. Struct. 700, 175–181 (2004)
X. Yue, W. Guo, X. Li, H. Zhou, R. Wang, Core-shell Fe3O4@ MIL-101 (Fe) composites as heterogeneous catalysts of persulfate activation for the removal of Acid Orange 7. Environ. Sci. Pollut. Res. 23, 15218–15226 (2016)
G. Srinivas, W. Travis, J. Ford, H. Wu, Z.-X. Guo, T. Yildirim, Nanoconfined ammonia borane in a flexible metal–organic framework Fe–MIL-53: clean hydrogen release with fast kinetics. J. Mater. Chem. A 1, 4167–4172 (2013)
J.-J. Du, Y.-P. Yuan, J.-X. Sun, F.-M. Peng, X. Jiang, L.-G. Qiu, A.-J. Xie, Y.-H. Shen, J.-F. Zhu, New photocatalysts based on MIL-53 metal–organic frameworks for the decolorization of methylene blue dye. J. Hazard. Mater. 190, 945–951 (2011)
H. Lv, H. Zhao, T. Cao, L. Qian, Y. Wang, G. Zhao, Efficient degradation of high concentration azo-dye wastewater by heterogeneous Fenton process with iron-based metal-organic framework. J. Mol. Catal. A 400, 81–89 (2015)
K. Yokota, K. Nakamura, T. Kasuya, S. Tamura, T. Sugimoto, K. Akamatsu, K. Nakao, F. Miyashita, Compositional structure of dual TiNO layers deposited on SUS 304 by an IBAD technique. Surf. Coat. Technol. 158, 568–572 (2002)
R. Li, X. Jin, M. Megharaj, R. Naidu, Z. Chen, Heterogeneous Fenton oxidation of 2, 4-dichlorophenol using iron-based nanoparticles and persulfate system. Chem. Eng. J. 264, 587–594 (2015)
S. Wang, N. Zhou, Removal of carbamazepine from aqueous solution using sono-activated persulfate process. Ultrason. Sonochem. 29, 156–162 (2016)
A.J. Jafari, B. Kakavandi, N. Jaafarzadeh, R.R. Kalantary, M. Ahmadi, A.A. Babaei, Fenton-like catalytic oxidation of tetracycline by AC@ Fe3O4 as a heterogeneous persulfate activator: adsorption and degradation studies. J. Ind. Eng. Chem. 45, 323–333 (2017)
I. Arslan-Alaton, G. Tureli, T. Olmez-Hanci, Treatment of azo dye production wastewaters using Photo-Fenton-like advanced oxidation processes: optimization by response surface methodology. J. Photochem. Photobiol., A 202, 142–153 (2009)
A.K. Verma, R.R. Dash, P. Bhunia, A review on chemical coagulation/flocculation technologies for removal of colour from textile wastewaters. J. Environ. Manag. 93, 154–168 (2012)
Y. Su, Z. Wu, Y. Wu, J. Yu, L. Sun, C. Lin, Acid Orange II degradation through a heterogeneous Fenton-like reaction using Fe–TiO2 nanotube arrays as a photocatalyst. J. Mater. Chem. A 3, 8537–8544 (2015)
C. Liang, C.J. Bruell, M.C. Marley, K.L. Sperry, Persulfate oxidation for in situ remediation of TCE. I. Activated by ferrous ion with and without a persulfate–thiosulfate redox couple. Chemosphere 55, 1213–1223 (2004)
Y. Ji, Y. Shi, W. Dong, X. Wen, M. Jiang, J. Lu, Thermo-activated persulfate oxidation system for tetracycline antibiotics degradation in aqueous solution. Chem. Eng. J. 298, 225–233 (2016)
S. Nasseri, A.H. Mahvi, M. Seyedsalehi, K. Yaghmaeian, R. Nabizadeh, M. Alimohammadi, G.H. Safari, 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 (2017)
M. Liu, L.-A. Hou, Q. Li, X. Hu, S. Yu, Heterogeneous degradation of tetracycline by magnetic Ag/AgCl/modified zeolite X–persulfate system under visible light. RSC Adv. 6, 35216–35227 (2016)
J. Liu, S. Zhong, Y. Song, B. Wang, F. Zhang, Degradation of tetracycline hydrochloride by electro-activated persulfate oxidation. J. Electroanal. Chem. 809, 74–79 (2018)
G.H. Safari, S. Nasseri, A.H. Mahvi, K. Yaghmaeian, R. Nabizadeh, M. Alimohammadi, Optimization of sonochemical degradation of tetracycline in aqueous solution using sono-activated persulfate process. J. Environ. Health Sci. Eng. 13, 76 (2015)
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This work was financially supported by National Natural Science Foundation of China (Grant Nos. 51364023, 21766016 and 21566014) and Talent Reserve Project in Yunnan (Grant No. 2015HB014).
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He, L., Zhang, Y., Zheng, Y. et al. Degradation of tetracycline by a novel MIL-101(Fe)/TiO2 composite with persulfate. J Porous Mater 26, 1839–1850 (2019). https://doi.org/10.1007/s10934-019-00778-y
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DOI: https://doi.org/10.1007/s10934-019-00778-y