Abstract
A titanium-based heterobimetallic single-source precursor [Y2Ti4(μ3-O)4(μ2-O)3(H2O)(TFA)8(THF)5].3(THF) (1) (where TFA = trifluoroacetato and THF = tetrahydrofuran) was successfully used to fabricate pyrochlore-structured Y2Ti2O7–2TiO2 composite thin films on fluorine-doped tin oxide (FTO) substrates using the aerosol-assisted chemical vapor deposition technique (AACVD). The precursor complex (1), isolated in crystalline form by reacting yttrium (III) acetate monohydrate with titanium (IV) isopropoxide and trifluroacetic acid in THF solution, was characterized by physicochemical methods such as melting point, microanalysis, FT-IR, 1H-NMR, thermogravimetric analyses (TGA/DTG), and single-crystal X-ray diffraction. Thin films prepared at 550 °C were investigated by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), field emission gun-scanning electron microscopy (FESEM), and energy-dispersive X-ray spectroscopy (EDX) which demonstrated the development of mesoporous structured microballs of Y2Ti2O7–2TiO2 with precise stoichiometry. The optical analysis showed that Y2Ti2O7–2TiO2 has a direct optical band gap of 1.8 eV. Photo-oxidation of water via Y2Ti2O7–2TiO2 thin films was carried out under simulated solar irradiation of AM 1.5 G (100 mW cm−2) using three-electrode photoelectrochemical cell in of in three separate 0.5 M electrolyte solutions of NaOH (pH = 13.5), Na2SO4 (pH = 7.2), and citrate buffer (pH = 4). A best photocurrent density of ~ 60 μA cm−2 at + 0.8 V vs. SCE was observed at pH of 13.5. These observations were further validated by electrochemical impedance spectroscopy (EIS) studies in terms of charge transportation and its recombination time.
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The work received financial support from the University of Malaya through FRGS Grant No. FP039-2016 and IPPP Grant No. PG053-2016A.
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CCDC 1576421 contains the supplementary crystallographic data for complex (1). These data can be obtained free of charge via http://www.ccdc.cam.ac.uk/conts/retrieving.html, or from the Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: (+44) 1223–336-033; or e-mail: deposit@ccdc.cam.ac.uk. Crystallographic details, FT-IR and NMR spectra for compound complex 1, XRD stick pattern matching with standard cards, high resolution FESEM images and EDX of thin films are is available in supplementary data.
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Munawar, K., Mansoor, M.A., Olmstead, M.M. et al. Pyrochlore-structured Y2Ti2O7–2TiO2 composite thin films for photovoltaic applications. J Aust Ceram Soc 55, 921–932 (2019). https://doi.org/10.1007/s41779-019-00329-3
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DOI: https://doi.org/10.1007/s41779-019-00329-3