Adsorption and degradation of some psychiatric drugs by sol-gel synthesized titania-based photocatalysts: influence of tungsten and sodium content
Abstract
Mesoporous anatase nanopowders were doped with 0.05−0.5 mol% of W6+, in order to obtain more efficient photocatalyst than TiO2 Degussa P25 in the degradation of amitriptyline (AMI) under simulated solar irradiation (SSI). Dominant XRPD peaks were ascribed to anatase phase, with additional peaks which could correspond to brookite, TiO2 bronze and sodium titanate, Na2Ti9O19. The Raman scattering measurements have confirmed anatase as dominant phase, with broad Raman feature at ~270 cm−1 possibly related to Ti–O–Na stretching vibration. All W-doped nanopowders have shown enhanced adsorption and higher efficiency in photodegradation of AMI in comparison to TiO2 Degussa P25 under the same conditions. The catalyst doped with 0.4 mol% of W6+, which has shown the highest efficiency in degradation of AMI under SSI, has also been tested in degradation of alprazolam (ALP). The effect of substrate type (AMI and ALP), catalyst loading, and initial substrate concentration on photocatalytic degradation using SSI was examined. The identification of the species responsible for the photocatalytic degradation of AMI and ALP by the catalyst doped with 0.4 mol% of W6+ was performed in the presence of various scavengers under SSI. The major role in degradation of AMI may be attributed to hydroxyl radicals, whereas superoxide anion radicals, singlet molecular oxygen and hydroxyl radicals contribute to degradation of ALP.
Highlights
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Influence of W and Na content on the properties of TiO2 catalysts synthesized by sol-gel method.
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Powders characterized by XRPD, SEM, EDS, BET, Raman, and UV-vis spectroscopy.
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Adsorption and photodegradation of amitriptyline and alprazolam under simulated solar irradiation.
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Optimal synthesis and W-doping conditions for photocatalytic degradation of amitriptyline found.
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Various scavengers used to identify mechanisms of photodegradation of amitriptyline and alprazolam.
Keywords
Sol-gel synthesis Doped titania nanopowders XRPD Raman spectroscopy Adsorption and photocatalytic degradation Psychiatric drugsNotes
Acknowledgements
This work was financially supported by the Ministry of Education, Science and Technological Development (Republic of Serbia), under the Projects No. III45018, ON172042, and III45015, as well as SASA project F–134. Besides, authors thank MSc Maria Uzelac and MSc Marta Kolesar for the technical assistance.
Compliance with ethical standards
Conflict of interest
The authors declare that they have no conflict of interest.
Supplementary material
References
- 1.Ratova M, West GT, Kelly PJ (2013) Optimization studies of photocatalytic tungsten-doped titania coatings deposited by reactive magnetron co-sputtering. Coatings 3:194–207CrossRefGoogle Scholar
- 2.Doeff MM, Cabana J, Shirpour M (2014) Titanate anodes for sodium ion batteries. J Inorg Organomet Polym 24:5–14CrossRefGoogle Scholar
- 3.Kolen’ko YV, Kovnir KA, Gavrilov AI, Garshev AV, Frantti J, Lebedev OI, Churagulov BR, Van Tendeloo OG, Yoshimura M (2006) Hydrothermal synthesis and characterization of nanorods of various titanates and titanium dioxide. J Phys Chem B 110:4030–4038CrossRefGoogle Scholar
- 4.Ahmed S, Rasul MG, Martens WN, Brown R, Hashib MA (2010) Heterogeneous photocatalytic degradation of phenols in wastewater: a review on current status and developments. Desalination 261:3–18CrossRefGoogle Scholar
- 5.Jones OAH, Voulvoulis N, Lester JN (2006) Partitioning behavior of five pharmaceutical compounds to activated sludge and river sediment. Arch Environ Contam Toxicol 50:297–305CrossRefGoogle Scholar
- 6.Calisto V, Esteves VI (2009) Psychiatric pharmaceuticals in the environment. Chemosphere 77:1257–1274CrossRefGoogle Scholar
- 7.Bottoni P, Caroli S, Barra Caracciolo A (2010) Pharmaceuticals as priority water contaminants. Toxicol Environ Chem 92:549–565CrossRefGoogle Scholar
- 8.Fernández-Navarro JJ, Ruiz-Ángel MJ, García-Álvarez-Coque MC (2012) Reversed-phase liquid chromatography without organic solvent for determination of tricyclic antidepressants. J Sep Sci 35:1303–1309CrossRefGoogle Scholar
- 9.Viola G, Miolo G, Vedaldi D, Dall’Acqua F (2000) In vitro studies of the phototoxic potential of the antidepressant drugs amitriptyline and imipramine. Farmaco 55:211–218CrossRefGoogle Scholar
- 10.Vosough M, Iravani NJ (2016) Matrix-free analysis of selected benzodiazepines in human serum samples using alternating trilinear decomposition modeling of fast liquid chromatography diode array detection data. Talanta 148:454–462CrossRefGoogle Scholar
- 11.Cabrera CG, Waisbaum RG, Nudelman NS (2005) Kinetic and mechanistic studies on the hydrolysis and photodegradation of diazepam and alprazolam. J Phys Org Chem 18:156–161CrossRefGoogle Scholar
- 12.Soboleva NM, Nosovich AA, Goncharuk VV (2007) The heterogenic photocatalysis in water treatment processes. J Water Chem Technol 29:72–89CrossRefGoogle Scholar
- 13.Abramović B, Šojić D (2010) In: Urbonienė IA (ed) Desalination: methods, costs and technology, Chapter: TiO2-Assisted photocatalytic degradation of herbicides in aqueous solution: a review. Nova Science Publishers Inc., New YorkGoogle Scholar
- 14.Zhang L, Li Y, Xie H, Wang H, Zhang Q (2015) Efficient mineralization of toluene by W-doped TiO2 nanofibers under visible light irradiation. J Nanosci Nanotechnol 15:2944–2951CrossRefGoogle Scholar
- 15.Xie Z, Wang Y, Wang P, Zhang L (2014) W-doped TiO2 preparation and photocatalytic degradation of guaiacol. Appl Mech Mater 513−514:33–36CrossRefGoogle Scholar
- 16.Couselo N, Garcıa Einschlag FS, Candal RJ, Jobbagy M (2008) Tungsten-doped TiO2 vs pure TiO2 photocatalysts: effects on photobleaching kinetics and mechanism. J Phys Chem C 112:1094–1100CrossRefGoogle Scholar
- 17.Michalow KA, Vital A, Heel A, Graule T, Reifler FA, Ritter A, Zakrzewska K, Rekas M (2008) Photocatalytic activity of W-doped TiO2 nanopowders. J Adv Oxid Technol 11:56–64Google Scholar
- 18.Tian H, Ma J, Li K, Li J (2008) Photocatalytic degradation of methyl orange with W-doped TiO2 synthesized by a hydrothermal method. Mat. Chem Phys 112:47–51Google Scholar
- 19.Sathasivam S, Bhachu DS, Lu Y, Chadwick N, Althabaiti SA, Alyoubi AO, Basahel SN, Carmalt CJ, Parkin IP (2015) Tungsten doped TiO2 with enhanced photocatalytic and optoelectrical properties via aerosol assisted chemical vapor deposition. Sci Rep 5(1-5):10952CrossRefGoogle Scholar
- 20.Mayoufi A, Nsib MF, Houas A (2014) Doping level effect on visible-light irradiation W-doped TiO2–anatase photocatalysts for congo red photodegradation. C R Chim 17:818–823CrossRefGoogle Scholar
- 21.Golubović A, Šćepanović M, Kremenović A, Aškrabić A, Berec V, Dohčević-Mitrović Z, Popović ZV (2009) Raman study of the variation in anatase structure of TiO2 nanopowders due to the changes of sol-gel synthesis conditions. J Sol-Gel Sci Technol 49(3):311–319CrossRefGoogle Scholar
- 22.Šćepanović M, Abramović B, Golubović A, Kler S, Grujić-Brojčin M, Dohčević-Mitrović Z, Babić B, Matović B, Popović ZV (2012) Photocatalytic degradation of metoprolol in water suspension of TiO2 nanopowders prepared using sol-gel route. J Sol-Gel Sci Technol 52:390–402Google Scholar
- 23.Golubović A, Abramović B, Šćepanović M, Grujić-Brojčin M, Armaković S, Veljković I, Babić B, Dohčević-Mitrović Z, Popović ZV (2013) Improved efficiency of sol–gel synthesized mesoporous anatase nanopowders in photocatalytic degradation of metoprolol. Mater Res Bull 48:1363–1371CrossRefGoogle Scholar
- 24.Rietveld HM (1969) A profile refinement method for nuclear and magnetic structures. J Appl Crystallogr 2:65–71CrossRefGoogle Scholar
- 25.Rodriguez-Carvajal J (1993) Recent advances in magnetic structure determination by neutron powder diffraction. Phys B 192:55–69CrossRefGoogle Scholar
- 26.Rodríguez-Carvajal J (2001) Recent developments of the Program FULLPROF, in commission on. Powder Diffr (IUCr), Newsl 26:12–19. http://journals.iucr.org/iucr-top/comm/cpd/Newsletters/ Google Scholar
- 27.Rodriguez-Carvajal J (2016) FullProf computer program (https://www.ill.eu/sites/fullprof/)
- 28.Thompson P, Cox DE, Hastings JM (1987) Rietveld refinement of Debye-Scherrer synchrotron X-ray data from Al2O3. J Appl Cryst 20:79–83CrossRefGoogle Scholar
- 29.Brunauer S, Emmett PH, Teller E (1938) Adsorption of gases in multimolecular layers. J Am Chem Soc 60:309–319CrossRefGoogle Scholar
- 30.Gregg SJ, Sing KSW (1982) Adsorption, Surface Area and Porosity. Academic Press, LondonGoogle Scholar
- 31.Rouquerol F, Rouquerol J, Sing K (1999) Adsorption by powders and porous solids, Academic Press, LondonGoogle Scholar
- 32.Barret EP, Joyner LG, Halenda PP (1951) The determination of pore volume and area distributions in porous substances I Computations from nitrogen isotherms. J Am Chem Soc 73:373–380CrossRefGoogle Scholar
- 33.Ivetić TB, Finčur NL, Abramović BF, Dimitrievska M, Štrbac GR, Čajko KO, Miljević BB, Đačanin LjR, Lukić-Petrović SR (2016) Environmentally friendly photoactive heterojunction zinc tin oxide nanoparticles. Ceram Int 42:3575–3583CrossRefGoogle Scholar
- 34.Tomić N, Grujić-Brojčin M, Finčur N, Abramović B, Simović B, Krstić J, Matović B, Šćepanović M (2015) Photocatalytic degradation of alprazolam in water suspension of brookite type TiO2 nanopowders prepared using hydrothermal route. Mat. Chem Phys 163:518–528Google Scholar
- 35.Ivetić TB, Dimitrievska MR, Finčur NL, Đačani LJR, Guth IO, Abramović BF, Lukić-Petrović SR (2014) Effect of annealing temperature on structural and optical properties of Mg-doped ZnO nanoparticles and their photocatalytic efficiency in alprazolam degradation. Ceram Int 40:1545–1552CrossRefGoogle Scholar
- 36.Howard CJ, Sabine TM, Dickson F (1991) Structural and thermal parameters for rutile and anatase. Acta Crystallogr B: Struct Sci 47:462–468CrossRefGoogle Scholar
- 37.Feist TP, Davies PK (1992) The soft chemical synthesis of TiO2 (B) from layered titanates. J Solid State Chem 101:275–295CrossRefGoogle Scholar
- 38.Pauling L, Sturdivant JH (1928) The crystal structure of brookite. Z fuer Krist, Krist, Krist, Krist 68(1-6):239–256Google Scholar
- 39.Theobald FR, Catlow CRA, Cormack AN (1984) Lattice energy minimization as a complementary technique to refine structures obtained by high-resolution electron. J Solid State Chem 52:80–90CrossRefGoogle Scholar
- 40.Abrahams SC, Bernstein JL (1965) Accuracy of an automatic diffractometer. Measurement of the sodium chloride structure factors. Acta Crystallogr 18:926–932CrossRefGoogle Scholar
- 41.Morgan DL, Liu H-W, Frost RL, Waclawik ER (2010) Implications of precursor chemistry on the alkaline hydrothermal synthesis of titania/titanate nanostructures. J Phys Chem C 114:101–110CrossRefGoogle Scholar
- 42.Rouquerol J, Avnir D, Fairbridge CW, Everett DH, Haynes JH, Pemicone N, Ramsay JDF, Sing KSW, Unger KK (1994) Recommendations for the characterization of porous solids (Technical Report). Pure Appl Chem 66:1739–1758CrossRefGoogle Scholar
- 43.Ohsaka T, Izumi F, Fujiki Y (1978) Raman spectrum of anatase, TiO2. J Raman Spectrosc 7:321–324CrossRefGoogle Scholar
- 44.Stengl V, Králová D (2011) Photoactivity of brookite–rutile TiO2 nanocrystalline mixtures obtained by heat treatment of hydrothermally prepared brookite. Mat Chem Phys 129:794–801CrossRefGoogle Scholar
- 45.Iliev MN, Hadjiev VG, Litvinchuk AP (2013) Raman and infrared spectra of brookite (TiO2): experiment and theory. Vib Spectrosc 64:148–152CrossRefGoogle Scholar
- 46.Zhang Y, Guo L, Yang S (2015) Novel sodium/lithium-ion anode material based on ultrathin Na2Ti2O4(OH)2 nanosheet. Nanoscale 7:14618–14626CrossRefGoogle Scholar
- 47.Bhat SSM, Babu B, Feygenson M, Neuefeind JC, Shaijumon MM (2018) Nanostructured Na2Ti9O19 for hybrid sodium-ion capacitors with excellent rate capability. ACS Appl Mater Interfaces 10:437–447CrossRefGoogle Scholar
- 48.Etacheri V, Yourey JE, Bartlett BM (2014) Chemically bonded TiO2 - bronze nanosheet/reduced graphene oxide hybrid for high-power lithium ion batteries. ACS Nano 8:1491–1499CrossRefGoogle Scholar
- 49.Muneer M, Bahnemann D (2002) Semiconductor-mediated photocatalyzed degradation of two selected pesticide derivatives, terbacil and 2,4,5-tribromoimidazole, in aqueous suspension. Appl Catal B: Environ 36:95–111CrossRefGoogle Scholar
- 50.Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ (2008) Multiresidue methods for the analysis of pharmaceuticals, personal care products and illicit drugs in surface water and wastewater by solid-phase extraction and ultra performance liquid chromatography–electrospray tandem mass spectrometry. Anal Bioanal– Chem 391:1293–1308CrossRefGoogle Scholar
- 51.Lajeunesse A, Gagnon C, Sauvé S (2008) Determination of basic antidepressants and their N-Desmethyl metabolites in raw sewage and wastewater using solid-phase extraction and liquid chromatography–tandem mass spectrometry. Anal Chem 80:5325–5333CrossRefGoogle Scholar
- 52.Sornalingam K, McDonagh A, Zhou JL (2016) Photodegradation of estrogenic endocrine disrupting steroidal hormones in aqueous systems: progress and future challenges. Sci Total Environ 550:209–224CrossRefGoogle Scholar
- 53.Sarkar S, Das R, Choi H, Bhattacharjee C (2014) Involvement of process parameters and various modes of application of TiO2 nanoparticles in heterogeneous photocatalysis of pharmaceutical wastes–a short review. RSC Adv 4:57250–57266CrossRefGoogle Scholar
- 54.Loftsson T, Guðmundsdóttir H, Sigurjónsdóttir JF, Sigurðsson HH, Sigfússon SD, Másson M, Stefánsson E (2001) Cyclodextrin solubilization of benzodiazepines: formulation of midazolam nasal spray. Int J Pharm 212:29–40CrossRefGoogle Scholar
- 55.Sin J-C, Lam S-M, Lee K-T, Mohamed AR (2013) Self-assembly fabrication of ZnO hierarchical micro/nanospheres for enhanced photocatalytic degradation of endocrine-disrupting chemicals. Mat Sci Semicond Process 16:1542–1550CrossRefGoogle Scholar
- 56.Zhao C, Pelaez M, Duan X, Deng H, O’Shea K, Fatta-Kassinos D, Dionysiou DD (2013) Role of pH on photolytic and photocatalytic degradation of antibiotic oxytetracycline in aqueous solution under visible/solar light: kinetics and mechanism studies. Appl Catal B: Environ 134−135:83–92CrossRefGoogle Scholar
- 57.Chen Y, Yang S, Wang K, Lou L (2005) Role of primary active species and TiO2 surface characteristic in UV-illuminated photodegradation of Acid Orange 7. J Photochem Photobiol A 172:47–54CrossRefGoogle Scholar
- 58.Lu Q, Zhang Y, Liu S (2015) Graphene quantum dots enhanced photocatalytic activity of zinc porphyrin toward the degradation of methylene blue under visible-light irradiation. J Mat Chem A3:8552–8558CrossRefGoogle Scholar
- 59.Calza P, Pelizzetti E (2001) Photocatalytic transformation of organic compounds in the presence of inorganic ions. Pure Appl Chem 73:1839–1848CrossRefGoogle Scholar
- 60.Benalioua B, Mansour M, Bentouami A, Boury B, Elandaloussi EH (2015) The layered double hydroxide route to Bi–Zn co-doped TiO2 with high photocatalytic activity under visible light. J Hazard Mater 288:158–167CrossRefGoogle Scholar
- 61.Zou Y, Gong Y, Lin B, Mellott NP (2016) Photodegradation of methylene blue in the visible spectrum: an efficient W6+ ion doped anatase titania photocatalyst via a solvothermal method. Vacuum 126:63–69CrossRefGoogle Scholar
- 62.Prabhu S, Nithya A, Chandra Mohan S, Jothivenkatachalam K (2014) Synthesis, surface acidity and photocatalytic activity of WO3/TiO2 nanocomposites – an overview. Mat Sci Forum 781:63–78CrossRefGoogle Scholar
- 63.Herrmann J-M, Guillard C (2000) Photocatalytic degradation of pesticides in agricultural used waters. Cr Acad Sci II C 3:417–422Google Scholar
- 64.Xie H, Li N, Liu B, Yang J, Zhao X (2016) Role of sodium Ion on TiO2 photocatalyst: influencing crystallographic properties or serving as the recombination center of charge carriers? J Phys Chem C 120:10390–10399CrossRefGoogle Scholar
- 65.Nam H-J, Amemiya T, Murabayashi M, Itoh K (2005) The influence of Na+ on the crystallite size of TiO2 and the photocatalytic activity. Res Chem Intermed 31(4–6):365–370CrossRefGoogle Scholar
- 66.Yang G, Yan Z, Xiao T, Yang B (2013) Low-temperature synthesis of alkalis doped TiO2 photocatalysts and their photocatalytic performance for degradation of methyl orange. J Alloy Compd 580:15–22CrossRefGoogle Scholar
- 67.Masae M, Pitsuwan P, Pholthawon C, Pawanwatcharakorn N (2015) Synthesis of Na doped TiO2 nano photocatalysts film on its photoactivity and hydrophilicity. Thammasat Int J Sci Technol 2:63–71Google Scholar
- 68.Finčur NL, Krstić JB, Šibul FS, Šojić DV, Despotović VN, Banić ND, Agbaba JR, Abramović BF (2017) Removal of alprazolam from aqueous solutions by heterogeneous photocatalysis: Influencing factors, intermediates, and products. Chem Eng J 307:1105–1115CrossRefGoogle Scholar
- 69.Labaran BA, Vohra MS (2014) Photocatalytic removal of selenite and selenate species: effect of EDTA and other process. Environ Technol 35:1091–1100CrossRefGoogle Scholar
- 70.Devi LG, Kavitha R (2014) Enhanced photocatalytic activity of sulfur doped TiO2 for the decomposition of phenol: a new insight into the bulk and surface modification. Mat Chem Phys 143:1300–1308CrossRefGoogle Scholar
- 71.Pastrana-Martínez LM, Morales-Torres S, Kontos AG, Moustakas NG, Faria JL, Doña-Rodrígez JM, Falaras P, Silva AMT (2013) TiO2, surface modified TiO2 and graphene oxide-TiO2 photocatalysts for degradation of water pollutants under near-UV/Vis and visible light. Chem Eng J 224:17–23CrossRefGoogle Scholar
- 72.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 on a titanium dioxide–fluoride system. Langmuir 15:8964–8972CrossRefGoogle Scholar