The influence of processing parameters is investigated on the structural characteristics of single and mixed oxides produced by spray pyrolysis technique. The films were synthesized by spraying precursor solutions through a noz-zle onto a heated alumina substrate. The precursor consisted separately of aqueous solutions of tin chloride for SnO 2 and zinc chloride for ZnO for single oxide cases, and aqueous solutions of tin chloride and indium nitrate for SnO 2 + In 2 O 3 and zinc chloride and indium nitrate solutions for ZnO + In 2 O 3 for mixed oxide cases. The substrate temperature was varied accordingly for each single and mixed case. The films produced were characterized by X-ray Photoelectron Spectroscopy and Scanning Electron Microscopy. The results indicate that a non-homogenous film is formed at low temperature for both single oxides considered. The temperature has significant effect on the composition of the synthesized films of both single oxides below 450 ℃ . The results for mixed oxides show that the best homogeneous films are obtained for 80 wt% ZnO + 20 wt% In 2 O 3 , and 80 wt% SnO 2 + 20 wt% In 2 O 3 .
KeywordsZinc Oxide FilmTin Oxide FilmMixed Metal OxidesNano-Composite Sen-sorsSpray Pyrolysis
Kruis, F.E., Fissan, H. and Peled, A. (1998) Synthesis of Nanoparticles in the Gas Phase for Electronic, Optical and Magnetic Applications—A Review. Journal of Aerosol Science, 29, 511-535. https://doi.org/10.1016/S0021-8502(97)10032-5
Shaginyan, L.R. (1998) Methods of Production, Structure, and Properties of Film Materials Based on the Carbon—Nitrogen System (Survey). Powder Metallurgy and Metal Ceramics, 37, 648-658. https://doi.org/10.1007/BF02680122
Perednis, D. and Gauckler, L.J. (2005) Thin Film Deposition Using Spray Pyrolysis. Journal of Electroceramics, 14, 103-111. https://doi.org/10.1007/s10832-005-0870-x
Kalantar-Zadeh, K. and Fry, B. (2007) Nanotechnology-Enabled Sensors. Springer, New York, 184-186.
Perednis, D. (2003) Thin Film Deposition by Spray Pyrolysis and the Application in Solid Oxide Fuel Cells, PhD Dissertation, ETH, Zurich.
George, J. (1992) Preparation of Thin Films. CRC Press, New York, 339-342.
Tofield, B.C. (1987) State of the Art and Future Prospects for Solid State Gas Sensors. In: Moseley, P.T. and Tofield, B.C., Eds., Solid State Gas Sensors, Adam Hilger, Bristol, 198-237.
Vigil, O., Cruz, F., Santana, G., Vaillant, L., Morales-Acevedo, A. and Contreras-Puente, G. (2000) Influence of Post-Thermal Annealing on the Properties of Sprayed Cadmium-Zinc Oxide Thin Films. Applied Surface Science, 161, 27-34. https://doi.org/10.1016/S0169-4332(00)00117-3
Nehru, L.C., Umadevi, M. and Sanjeeviraja, C. (2012) Studies on Structural, Optical and Electrical Properties of ZnO Thin Films Prepared by the Spray Pyrolysis Method. International Journal of Materials Engineering, 2, 12-17. https://doi.org/10.5923/j.ijme.20120201.03
Dedova, T. (2007) Chemical Spray Pyrolysis Deposition of Zinc Sulfide Thin Films and Zinc Oxide Nanostructured Layers. PhD Dissertation, Tallinn University of Technology, Estonia.
Zahedi, F., Dariani, R.S. and Rozati, S.M. (2013) Effect of Substrate Temperature on the Properties of ZnO Thin Films Prepared by Spray Pyrolysis. Materials Science in Semiconductor Processing, 16, 245-249. https://doi.org/10.1016/j.mssp.2012.11.005
Korotcenkov, G., Brinzari, V., Schwank, J., DiBattista, M. and Vasiliev, A. (2001) Peculiarities of SnO2 Thin Film Deposition by Spray Pyrolysis for Gas Sensor Application. Sensors and Actuators B: Chemical, 77, 244-252. https://doi.org/10.1016/S0925-4005(01)00741-9
Ikhmayies, S.J. and Ahmad-Bitar, R.N. (2009) Effect of the Substrate Temperature on the Electrical and Structural Properties of Spray-Deposited SnO2: F Thin Films. Materials Science in Semiconductor Processing, 12, 122-125. https://doi.org/10.1016/j.mssp.2009.09.003
Bai, S., Li, D., Han, D., Luo, R., Chen, A. and Chung, C.L. (2010) Preparation, Characterization of WO3-SnO2 Nanocomposites and Their Sensing Properties for NO2. Sensors and Actuators B: Chemical, 150, 749-755. https://doi.org/10.1016/j.snb.2010.08.007
Ilican, S., Caglar, Y., Caglar, M. and Yakuphanoglu, F. (2006) Electrical Conductivity, Optical and Structural Properties of Indium-Doped ZnO Nanofiber Thin Film Deposited by Spray Pyrolysis Method. Physica E: Low-dimensional Systems and Nanostructures, 35, 131-138. https://doi.org/10.1016/j.physe.2006.07.009
Rozati, S.M., Zarenejad, F. and Memarian, N. (2011) Study on Physical Properties of Indium-Doped Zinc Oxide Deposited by Spray Pyrolysis Technique. Thin Solid Films, 520, 1259-1262. https://doi.org/10.1016/j.tsf.2011.04.200
Wienke, J. and Booij, A.S. (2013) Spray Deposition of Oxides at Ambient Atmosphere Part 1: Transparent Conductive Oxides.
Bagheri Khatibani, A. and Rozati, S.M. (2013) Synthesis and Characterization of Amorphous Aluminum Oxide Thin Films Prepared by Spray Pyrolysis: Effects of Substrate Temperature. Journal of Non-Crystalline Solids, 363, 121-133. https://doi.org/10.1016/j.jnoncrysol.2012.12.013
Khatami, S.M.N. and Ilegbusi, O.J. (2011) Modeling of Aerosol Spray Characteristics for Synthesis of Mixed-Oxide Nanocomposite Sensor Film. 2011 International Mechanical Engineering Congress and Exposition, Denver, 11-17 November 2011, 581-589. https://doi.org/10.1115/IMECE2011-62252
Khatami, S.M.N. and Ilegbusi, O.J. (2012) Droplet Evaporation and Chemical Reaction in a Single Multi-Component Droplet to Synthesis Mixed-Oxide Film Using Spray Pyrolysis Method. 2012 International Mechanical Engineering Congress and Exposition, Houston, 9-15 November 2012, 633-638. https://doi.org/10.1115/IMECE2012-86382
Navid Khatami, S.M., Ilegbusi, O.J. and Trakhtenberg, L.I. (2015) Modelling Evaporation and Chemical Reaction in a Multi-Component Droplet from Spray Pyrolysis Synthesis of Mixed Metal-Oxide Nanocomposite Films. International Journal of Mathematical Modelling & Numerical Optimisation, 6, 141-158. https://doi.org/10.1504/IJMMNO.2015.069967
Khatami, S.M.N., Kuruppumullage, D.N. and Ilegbusi, O.J. (2013) Characterization of Metal Oxide Sensor Thin Films Deposited by Spray Pyrolysis. 2013 International Mechanical Engineering Congress and Exposition, San Diego, 15-21 November 2013, V010T11A044. https://doi.org/10.1115/imece2013-65136
Khatami, S.M.N., Ilegbusi, O.J. and Trakhtenberg, L. (2013) Modeling of Aerosol Spray Characteristics for Synthesis of Sensor Thin Film from Solution. Applied Mathematical Modelling, 37, 6389-6399. https://doi.org/10.1016/j.apm.2013.01.009
Patil, G.E., Kajale, D.D., Gaikwad, V.B. and Jain, G.H. (2012) Spray Pyrolysis Deposition of Nanostructured Tin Oxide Thin Films. ISRN Nanotechnology, 2012, Article ID: 275872.
Trakhtenberg, L.I.J., Navid Khatami, S.M., Gerasimov, G.N. and Ilegbusi, O.J. (2015) Effect of Composition and Morphology on Sensor Properties of Aerosol Deposited Nanostructured ZnO+In2O3 Films. Materials Sciences and Applications, 6, 220-227. https://doi.org/10.4236/msa.2015.63026
Zaier, A., Lakfif, F., Kabir, A., Boudjadar, S. and Aida, M.S. (2009) Effects of the Substrate Temperature and Solution Molarity on the Structural Opto-Electric Properties of ZnO Thin Films Deposited by Spray Pyrolysis. Materials Science in Semiconductor Processing, 12, 207-211. https://doi.org/10.1016/j.mssp.2009.12.002
Bagheri-Mohagheghi, M.M. and Shokooh-Saremi, M. (2004) Electrical, Optical and Structural Properties of Li-Doped SnO2 Transparent Conducting Films Deposited by the Spray Pyrolysis Technique: A Carrier-Type Conversion Study. Semiconductor Science and Technology, 19, 764-769. https://doi.org/10.1088/0268-1242/19/6/019
Hu, J. and Gordon, R.G. (1992) Atmospheric Pressure Chemical Vapor Deposition of Gallium Doped Zinc Oxide Thin Films from Diethyl Zinc, Water, and Triethyl Gallium. Journal of Applied Physics, 72, 5381-5392. https://doi.org/10.1063/1.351977
Hu, J. and Gordon, R.G. (1992) Textured Aluminum Doped Zinc Oxide Thin Films from Atmospheric Pressure Chemical-Vapor Deposition. Journal of Applied Physics, 71, 880-890. https://doi.org/10.1063/1.351309
Zunke, I., Heft, A., Schäfer, P., Haidu, F., Lehmann, D., Grünler, B. and Zahn, D.R.T. (2013) Conductive Zinc Oxide Thin Film Coatings by Combustion Chemical Vapour Deposition at Atmospheric Pressure. Thin Solid Films, 532, 50-55. https://doi.org/10.1016/j.tsf.2012.11.151
Ayouchi, R., Martin, F., Leinen, D. and Ramos-Barrado, J.R. (2003) Growth of Pure ZnO Thin Films Prepared by Chemical Spray Pyrolysis on Silicon. Journal of Crystal Growth, 247, 497-504. https://doi.org/10.1016/S0022-0248(02)01917-6
Ghimbeu, C.M., Van Landschoot, R.C., Schoonman, J. and Lumbreras, M. (2007) Preparation and Characterization of SnO2 and Cu-Doped SnO2 Thin Films Using Electrostatic Spray Deposition (ESD). Journal of the European Ceramic Society, 27, 207-213. https://doi.org/10.1016/j.jeurceramsoc.2006.05.092
Chen, Z., Salagaj, T., Jensen, C., Strobl, K., Nakarmi, M. and Shum, K. (2009) ZnO Thin Film Deposition on Sapphire Substrates by Chemical Vapor Deposition. MRS Online Proceeding, 1167, 1167-O07. https://doi.org/10.1557/proc-1167-o07-09
Jiao, B.C., Zhang, X.D., Wei, C.C., Sun, J., Huang, Q. and Zhao, Y. (2011) Effect of Acetic Acid on ZnO: In Transparent Conductive Oxide Prepared by Ultrasonic Spray Pyrolysis. Thin Solid Films, 520, 1323-1329. https://doi.org/10.1016/j.tsf.2011.04.152
Liang, Z., Gao, R., Lan, J.L., Wiranwetchayan, O., Zhang, Q., Li, C. and Cao, G. (2013) Growth of Vertically Aligned ZnO Nanowalls for Inverted Polymer Solar Cells. Solar Energy Materials and Solar Cells, 117, 34-40. https://doi.org/10.1016/j.solmat.2013.05.019
Tucic, A., Marinkovic, Z.V., Mancic, L., Cilense, M. and Milosevic, O. (2003) Pyrosol Preparation and Structural Characterization of SnO2 Thin Films. Journal of Materials Processing Technology, 143, 41-45. https://doi.org/10.1016/S0924-0136(03)00316-9
Patil, P.S., Kawar, R.K., Sadale, S.B. and Chigare, P.S. (2003) Properties of Spray Deposited Tin Oxide Thin Films Derived from Tri-N-Butyltin Acetate. Thin Solid Films, 437, 34-44. https://doi.org/10.1016/S0040-6090(03)00680-1
Smith, A. (2000) Pyrosol Deposition of ZnO and SnO2 Based Thin Films: The Interplay between Solution Chemistry, Growth Rate and Film Morphology. Thin Solid Films, 376, 47-55. https://doi.org/10.1016/S0040-6090(00)01403-6
Badadhe, S.S. and Mulla, I.S. (2009) H2S Gas Sensitive Indium-Doped ZnO Thin Films: Preparation and Characterization. Sensors and Actuators B: Chemical, 143, 164-170. https://doi.org/10.1016/j.snb.2009.08.056
Miki-Yoshida, M., Paraguay-Delgado, F., Estrada-Lopez, W. and Andrade, E. (2000) Structure and Morphology of High Quality Indium-Doped ZnO Films Obtained by Spray Pyrolysis. Thin Solid Films, 376, 99-109. https://doi.org/10.1016/S0040-6090(00)01408-5
Sivalingam, D., Gopalakrishnan, J.B. and Rayappan, J.B.B. (2012) Nanostructured Mixed ZnO and CdO Thin Film for Selective Ethanol Sensing. Materials Letters, 77, 117-120. https://doi.org/10.1016/j.matlet.2012.03.009
Lee, J.H., Lee, S.Y. and Park, B.O. (2006) Fabrication and Characteristics of Transparent Conducting In2O3-ZnO Thin Films by Ultrasonic Spray Pyrolysis. Materials Science and Engineering B, 127, 267-271. https://doi.org/10.1016/j.mseb.2005.10.008
Gupta, S.P. (1985) Measures of Dispersion, Statistical Methods. Sultan Chand and Sons, New Delhi.
Navid Khatami, S.M., Ilegbusi, O.J. and Trakhtenberg, L.I. (2015) Mathematical Modeling and Experimental Validation of Mixed Metal Oxide Thin Film Deposition by Spray Pyrolysis. Materials Sciences and Applications, 6, 68-77. https://doi.org/10.4236/msa.2015.61009