Abstract
Nanocrystalline lead zirconate titanate (PZT) powders were synthesized via a modified Pechini method. The effect of heat treatment temperature on the microstructural properties was studied using X-ray powder diffraction. The explored temperatures were identified from the TGA/DSC measurement and it is found that the crystallization starts from 550 °C. Rietveld refinement was applied to study structural changes and to quantitatively assess the fractional content of lead monoxide, identified in nano-PZT powders. Lebail method was carried out to the XRD pattern to accurately determine the peak broadening and position. Size-Strain Plot and various Williamson-Hall methods were used to calculate the lattice microstrain and crystallite size. The minimum strain was noticed in the pure tetragonal-PZT sample. TEM technique was also employed to study nanopowders and to confirm the formation of small-sized particles. The energy band gap was determined by diffused reflectance measurements and found to range from 3.17 to 3.29 eV.
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Abd El-Sadek MS, Wasly HS, Batoo KM (2019) X-ray peak profile analysis and optical properties of CdS nanoparticles synthesized via the hydrothermal method. Appl Phys A 125:283. https://doi.org/10.1007/s00339-019-2576-y
Anil A, Vani K, Kumar V (2018) Role of defect structures in stabilization of ferroelectric phase in tin-substituted lead zirconate titanate. J Am Ceram Soc 101:3377–3382. https://doi.org/10.1111/jace.15482
Arya PR, Jha P, Ganguli AK (2003) Synthesis, characterization and dielectric properties of nanometer-sized barium strontium titanates prepared by the polymeric citrate precursor method. J Mater Chem 13:415–423. https://doi.org/10.1039/b205087k
Baedi J, Hosseini SM, Kompany A (2008) The effect of excess titanium and crystal symmetry on electronic properties of Pb(Zr1−xTix)O3 compounds. Comput Mater Sci 43:909–916. https://doi.org/10.1016/J.COMMATSCI.2008.02.008
Banerjee A, Bandyopadhyay A, Bose S (2006) Influence of La2O3, SrO, and ZnO addition on PZT. J Am Ceram Soc 89:1594–1600. https://doi.org/10.1111/j.1551-2916.2006.00927.x
Batra V, Kotru S, Varagas M, Ramana CV (2015) Optical constants and band gap determination of Pb0.95La0.05Zr0.54Ti0.46O3 thin films using spectroscopic ellipsometry and UV–visible spectroscopy. Opt Mater (Amst) 49:123–128. https://doi.org/10.1016/j.optmat.2015.08.019
Bhalla AS, Guo R, Roy R (2000) The perovskite structure—a review of its role in ceramic science and technology. Mater Res Innov 4:3–26. https://doi.org/10.1007/s100190000062
Bindu P, Thomas S (2014) Estimation of lattice strain in ZnO nanoparticles: X-ray peak profile analysis. J Theor Appl Phys 8:123–134. https://doi.org/10.1007/s40094-014-0141-9
Boher P, Garnier P, Gavarri JR, Hewat AW (1985) Monoxyde quadratique PbOα(I): description de la transition structurale ferroe´lastique. J Solid State Chem 57:343–350. https://doi.org/10.1016/0022-4596(85)90197-5
Boukamp BA, Pham MTN, Blank DHA, Bouwmeester HJM (2004) Ionic and electronic conductivity in lead-zirconate-titanate (PZT). Solid State Ionics 170:239–254. https://doi.org/10.1016/j.ssi.2004.03.005
Bruncková H, Medvecký L, Briančin J, Saksl K (2004) Influence of hydrolysis conditions of the acetate sol–gel process on the stoichiometry of PZT powders. Ceram Int 30:453–460. https://doi.org/10.1016/S0272-8842(03)00131-7
Chaput F, Boilot J-P, Beauger A (1990) Alkoxide-hydroxide route to syntheltize BaTiO3-based powders. J Am Ceram Soc 73:942–948. https://doi.org/10.1111/j.1151-2916.1990.tb05141.x
Cho W-S (1998) Structural evolution and characterization of BaTiO3 nanoparticles synthesized from polymeric precursor. J Phys Chem Solids 59:659–666. https://doi.org/10.1016/S0022-3697(97)00227-8
Cullity BD, Stock SR (2001) Elements of X-ray diffraction, 3rd edition
Dittmer R, Clemens F, Schoenecker A et al (2010) Microstructural analysis and mechanical properties of Pb(Zr, Ti)O 3 fibers derived by different processing routes. J Am Ceram Soc 93:2403–2410. https://doi.org/10.1111/j.1551-2916.2010.03742.x
Durruthy-Rodríguez MD, Costa-Marrero J, Hernández-García M et al (2010) Photoluminescence in “hard” and “soft” ferroelectric ceramics. Appl Phys A 98:543–550. https://doi.org/10.1007/s00339-009-5501-y
Ghasemifard M, Hosseini SM, Khorsand Zak A, Khorrami GH (2009) Microstructural and optical characterization of PZT nanopowder prepared at low temperature. Phys E Low-dimensional Syst Nanostructu 41:418–422. https://doi.org/10.1016/J.PHYSE.2008.09.017
Gopejenko A, Piskunov S, Zhukovskii YF (2017) Ab initio modelling of the effects of varying Zr (Ti) concentrations on the atomic and electronic properties of stoichiometric PZT solid solutions. Comput Theor Chem 1104:56–60. https://doi.org/10.1016/j.comptc.2017.02.006
Gueye I, Le Rhun G, Gergaud P et al (2016) Chemistry of surface nanostructures in lead precursor-rich PbZr0.52Ti0.48O3sol-gel films. Appl Surf Sci 363:21–28. https://doi.org/10.1016/j.apsusc.2015.11.118
Heifets E (2002) Ab initio study of elastic properties of Pb(Ti, Zr)O3. AIP Conf Proc 626:150–159. https://doi.org/10.1063/1.1499563
Heywang W, Lubitz K, Wersing W (2008) Piezoelectricity: evolution and future of a technology. Springer Science & Business Media, Berlin
Hill RJ (1985) Refinement of the structure of orthorhombic PbO (massicot) by rietveld analysis of neutron powder diffraction data. Acta Crystallogr Sect C Cryst Struct Commun 41:1281–1284. https://doi.org/10.1107/S0108270185007454
Hinterstein M, Hoelzel M, Rouquette J et al (2015) Interplay of strain mechanisms in morphotropic piezoceramics. Acta Mater 94:319–327. https://doi.org/10.1016/j.actamat.2015.04.017
Holman RL, Fulrath RM (1973) Intrinsic nonstoichiometry in the lead zirconate-lead titanate system determined by Knudsen effusion. J Appl Phys 44:5227–5236. https://doi.org/10.1063/1.1662136
Horchidan N, Ciomaga CE, Frunza RC et al (2016) A comparative study of hard/soft PZT-based ceramic composites. Ceram Int 42:9125–9132. https://doi.org/10.1016/j.ceramint.2016.02.179
Ibn-Mohammed T, Koh SCL, Reaney IM et al (2016) Integrated hybrid life cycle assessment and supply chain environmental profile evaluations of lead-based (lead zirconate titanate) versus lead-free (potassium sodium niobate) piezoelectric ceramics. Energy Environ Sci 9:3495–3520. https://doi.org/10.1039/C6EE02429G
Ibn-Mohammed T, Koh SCL, Reaney IM et al (2017) Are lead-free piezoelectrics more environmentally friendly? MRS Commun 7:1–7. https://doi.org/10.1557/mrc.2017.10
Ibn-Mohammed T, Reaney IM, Koh SCL et al (2018) Life cycle assessment and environmental profile evaluation of lead-free piezoelectrics in comparison with lead zirconate titanate. J Eur Ceram Soc 38:4922–4938. https://doi.org/10.1016/j.jeurceramsoc.2018.06.044
Ihlefeld JF, Kotula PG, Gauntt BD et al (2015) Solution chemistry, substrate, and processing effects on chemical homogeneity in lead zirconate titanate thin films. J Am Ceram Soc 98:2028–2038. https://doi.org/10.1111/jace.13576
Jha P, Arya P, Ganguli A (2003) Dielectric properties of lead zirconium titanates with nanometer size grains synthesized by the citrate precursor route. Mater Chem Phys 82:355–361. https://doi.org/10.1016/S0254-0584(03)00266-9
Kalita A, Kalita MPC (2017) Williamson-Hall analysis and optical properties of small sized ZnO nanocrystals. Phys E Low-Dimensional Syst Nanostruct 92:36–40. https://doi.org/10.1016/j.physe.2017.05.006
Khorrami GH, Khorsand Zak A, Banihashemian SM (2014) Magnetic and dielectric properties on sol–gel combustion synthesis of Pb(Zr0.52, Ti0.43X0.05)O3 (X=Fe, Ni, and Co) nanoparticles. Adv Powder Technol 25:1319–1324. https://doi.org/10.1016/j.apt.2014.03.011
Khorsand Zak A, Abd Majid WH, Abrishami ME, Yousefi R (2011) X-ray analysis of ZnO nanoparticles by Williamson–Hall and size–strain plot methods. Solid State Sci 13:251–256. https://doi.org/10.1016/j.solidstatesciences.2010.11.024
Kityk I, Kassiba A, Plucinski K, Berdowski J (2000) Band structure of large-sized SiC nanocomposites. Phys Lett A 265:403–410. https://doi.org/10.1016/S0375-9601(99)00912-3
Kozielski L, Piechowiak M, Czekaj D et al (2008) Mechanical examination of PZT microfibre defects structure. Phase Trans 81:1081–1088. https://doi.org/10.1080/01411590802460668
Kumar L, Kumar P, Narayan A, Kar M (2013) Rietveld analysis of XRD patterns of different sizes of nanocrystalline cobalt ferrite. Int Nano Lett 3:1–12. https://doi.org/10.1186/2228-5326-3-8
Kumar A, Dhoble SJ, Bhatt J et al (2019) Structural characterization and influence of calcination temperature on luminescence properties of Sr0.91Mg2Al5.82Si9.18O30: Eu3+ nanophosphors. Powder Technol 354:591–600. https://doi.org/10.1016/j.powtec.2019.06.031
Lakeman CDE, Payne DA (1992) Processing effects in the Sol–Gel preparation of PZT dried gels, powders, and ferroelectric thin layers. J Am Ceram Soc 75:3091–3096. https://doi.org/10.1111/j.1151-2916.1992.tb04392.x
Liu D, White KW (2004) Mechanical aspects of epitaxial ferroelectric Pb(Zr 0.5 Ti 0.5)O 3 films investigated by nanoindentation methods and piezoresponse force microscopy. Appl Phys Lett 85:3459–3461. https://doi.org/10.1063/1.1806563
Lutterotti L, Scardi P, Maistrelli P (1992) LSI - a computer program for simultaneous refinement of material structure and microstructure. J Appl Crystallogr 25:459–462. https://doi.org/10.1107/S0021889892001122
Majumder SB, Mohapatra YN, Agrawal DC (1997) Optical and microstructural characterization of sol–gel derived cerium-doped PZT thin films. J Mater Sci 32:2141–2150
Mandal TK (2015) Rietveld refinement on XRD and TEM study of nanocrystalline PbZr0:5Ti0:5O3 ceramics prepared with a soft chemistry route. Mater Sci 33:18–24. https://doi.org/10.1515/msp-2015-0040
Mirzaei A, Bonyani M, Torkian S (2016) Synthesis and characterization of nanocrystalline PZT powders: from sol to dense ceramics. Process Appl Ceram. https://doi.org/10.2298/PAC1601009M
Moret MP, Devillers MAC, Wörhoff K, Larsen PK (2002) Optical properties of PbTiO3, PbZrxTi1−xO3, and PbZrO3 films deposited by metalorganic chemical vapor on SrTiO3. J Appl Phys 92:468–474. https://doi.org/10.1063/1.1486048
Nguyen MD, Trinh TQ, Dekkers M et al (2014) Effect of dopants on ferroelectric and piezoelectric properties of lead zirconate titanate thin films on Si substrates. Ceram Int 40:1013–1018. https://doi.org/10.1016/j.ceramint.2013.06.098
Noheda B, Cox DE (2006) Bridging phases at the morphotropic boundaries of lead oxide solid solutions. Phase Trans 79:5–20. https://doi.org/10.1080/01411590500467262
Noheda B, Gonzalo J, Cross L et al (2000) Tetragonal-to-monoclinic phase transition in a ferroelectric perovskite: the structure. Phys Rev B Condens Matter Mater Phys 61:8687–8695. https://doi.org/10.1103/PhysRevB.61.8687
Oliveira CA, Longo E, Varela JA, Zaghete MA (2014) Synthesis and characterization of lead zirconate titanate (PZT) obtained by two chemical methods. Ceram Int 40:1717–1722. https://doi.org/10.1016/j.ceramint.2013.07.068
Pandey SK, James AR, Raman R et al (2005) Structural, ferroelectric and optical properties of PZT thin films. Phys B Condens Matter 369:135–142. https://doi.org/10.1016/j.physb.2005.08.024
Park C-S, Lee J-W, Lee S-M et al (2010) Effect of excess PbO on microstructure and orientation of PZT(60/40) films. J Electroceram 25:20–25. https://doi.org/10.1007/s10832-009-9584-9
Patil RP, More PV, Jain GH et al (2017) BaTiO3 nanostructures for H2S gas sensor: Influence of band-gap, size and shape on sensing mechanism. Vacuum 146:455–461. https://doi.org/10.1016/j.vacuum.2017.08.008
Peng CH, Chang J-F, Desu SB (1991) Optical properties of PZT, PLZT, and PNZT thin films. MRS Proc 243:21. https://doi.org/10.1557/PROC-243-21
Pintilie L, Vrejoiu I, Le Rhun G, Alexe M (2007) Short-circuit photocurrent in epitaxial lead zirconate-titanate thin films. J Appl Phys 101:064109. https://doi.org/10.1063/1.2560217
Prado LR, de Resende NS, Silva RS et al (2016) Influence of the synthesis method on the preparation of barium titanate nanoparticles. Chem Eng Process Process Intensif 103:12–20. https://doi.org/10.1016/j.cep.2015.09.011
Rajender G, Giri PK (2016) Strain induced phase formation, microstructural evolution and bandgap narrowing in strained TiO2 nanocrystals grown by ball milling. J Alloys Compd 676:591–600. https://doi.org/10.1016/j.jallcom.2016.03.154
Rodríguez-Aranda MC, Calderón-Piñar F, Hernández-Landaverde MA et al (2016) Photoluminescence of sol–gel synthesized PZT powders. J Lumin 179:280–286. https://doi.org/10.1016/J.JLUMIN.2016.07.030
Rossetti GA, Popov G, Zlotnikov E, Yao N (2006) Domain structures and nonlinear mechanical deformation of soft Pb(ZrxTi1−x)O3 (PZT) piezoelectric ceramic fibers. Mater Sci Eng A 433:124–132. https://doi.org/10.1016/j.msea.2006.06.029
Rouquette J, Haines J, Bornand V et al (2006) Use of resonance Raman spectroscopy to study the phase diagram of PbZr0.52Ti0.48O3. Phys Rev B 73:224118. https://doi.org/10.1103/PhysRevB.73.224118
Rožić L, Petrović S, Lončarević D et al (2019) Influence of annealing temperature on structural, optical and photocatalytic properties of TiO2–CeO2 nanopowders. Ceram Int 45:2361–2367. https://doi.org/10.1016/j.ceramint.2018.10.153
Samanta S, Muralidhar M, Sankaranarayanan V et al (2017) Band gap reduction and redshift of lattice vibrational spectra in Nb and Fe co-doped PLZT. J Mater Sci 52:13012–13022. https://doi.org/10.1007/s10853-017-1425-7
Samanta S, Sankaranarayanan V, Sethupathi K (2018) Band gap, piezoelectricity and temperature dependence of differential permittivity and energy storage density of PZT with different Zr/Ti ratios. Vacuum 156:456–462. https://doi.org/10.1016/j.vacuum.2018.08.015
Sanders PG, Witney AB, Weertman JR et al (1995) Residual stress, strain and faults in nanocrystalline palladium and copper. Mater Sci Eng A 204:7–11. https://doi.org/10.1016/0921-5093(95)09928-X
Sczancoski JC, Cavalcante LS, Joya MR et al (2008) SrMoO4 powders processed in microwave-hydrothermal: synthesis, characterization and optical properties. Chem Eng J 140:632–637. https://doi.org/10.1016/j.cej.2008.01.015
Sczancoski JC, Cavalcante LS, Joya MR et al (2009) Synthesis, growth process and photoluminescence properties of SrWO4 powders. J Colloid Interface Sci 330:227–236. https://doi.org/10.1016/j.jcis.2008.10.034
Silva MS, Cilense M, Orhan E et al (2005) The nature of the photoluminescence in amorphized PZT. J Lumin 111:205–213. https://doi.org/10.1016/J.JLUMIN.2004.08.045
Solanki RG, Rajaram P, Bajpai PK (2017) Growth, characterization and estimation of lattice strain and size in CdS nanoparticles: X-ray peak profile analysis. Indian J Phys. https://doi.org/10.1007/s12648-017-1134-8
Stokes AR, Wilson AJC (1944) The diffraction of X rays by distorted crystal aggregates-I. Proc Phys Soc 56:174
Sun D, Jin X, Liu H et al (2007) Investigation on FTIR spectrum of barium titanate ceramics doped with alkali ions. Ferroelectrics 355:145–148. https://doi.org/10.1080/00150190701517630
Tadigadapa S, Mateti K (2009) Piezoelectric MEMS sensors: state-of-the-art and perspectives. Meas Sci Technol 20:092001. https://doi.org/10.1088/0957-0233/20/9/092001
Tariq GH, Lane DW, Anis-ur-Rehman M (2015) Physical properties of chalcogenide Sn–Bi–S graded thin films annealed in argon. Appl Phys A 120:1407–1414. https://doi.org/10.1007/s00339-015-9325-7
Tawfik A, Hemeda OM, Henaish AMA, Dorgham AM (2018) High piezoelectric properties of modified nano lead titanate zirconate ceramics. Mater Chem Phys 211:1–8. https://doi.org/10.1016/j.matchemphys.2018.01.073
Teixeira GF, Zaghete MA, Gasparotto G et al (2012) Photoluminescence properties and synthesis of a PZT mesostructure obtained by the microwave-assisted hydrothermal method. J Alloys Compd 512:124–127. https://doi.org/10.1016/j.jallcom.2011.09.036
Trinquier G, Hoffmann R (1984) Lead monoxide. Electronic structure and bonding. J Phys Chem 88:6696–6711. https://doi.org/10.1021/j150670a038
Uchino K (2008) Piezoelectric actuators 2006. J Electroceramics 20:301–311. https://doi.org/10.1007/s10832-007-9196-1
Venkateswarlu K, Chandra Bose A, Rameshbabu N (2010) X-ray peak broadening studies of nanocrystalline hydroxyapatite by Williamson–Hall analysis. Phys B Condens Matter 405:4256–4261. https://doi.org/10.1016/j.physb.2010.07.020
Warren BE, Averbach BL (1950) The effect of cold-work distortion on X-ray patterns. J Appl Phys 21:595–599. https://doi.org/10.1063/1.1699713
Wei H, Wang H, Xia Y et al (2018) An overview of lead-free piezoelectric materials and devices. J Mater Chem C 6:12446–12467. https://doi.org/10.1039/c8tc04515a
Wong GHL, Chua BW, Li L, Lai MO (2001) Processing of thermally stable doped perovskite PZT ceramics. J Mater Process Technol 113:450–455. https://doi.org/10.1016/S0924-0136(01)00631-8
Wu A, Salvado IMM, Vilarinho PM, Baptista L (1998) Lead zirconate titanate prepared from different zirconium and titanium precursors by Sol–Gel. 44:2640–2644
Yan X, Zheng M, Hou Y et al (2018) High energy conversion efficiency in Mn-modified Ba 09 Ca 01 Ti 093 Zr 007 O 3 lead-free energy harvester. J Am Ceram Soc. https://doi.org/10.1111/jace.15396
Yashima M, Hoshina T, Ishimura D et al (2005) Size effect on the crystal structure of barium titanate nanoparticles. J Appl Phys 98:014313. https://doi.org/10.1063/1.1935132
Yen F-S, Hsiang H-I, Chang Y-H (1995) Cubic to tetragonal phase transformation of ultrafine BaTiO3 crystallites at room temperature. Jpn J Appl Phys 34:6149–6155. https://doi.org/10.1143/JJAP.34.6149
Zhao FX, Xu XC, Liu HQ, Wang YL (2014) Effect of annealing treatment on the microstructure and mechanical properties of ultrafine-grained aluminum. Mater Des 53:262–268. https://doi.org/10.1016/j.matdes.2013.06.075
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Omran, K.H., El-sadek, M.S.A., Mostafa, M. et al. Influence of PbO phase content on structural and optical properties of PZT nanopowders. Appl Nanosci 10, 2315–2327 (2020). https://doi.org/10.1007/s13204-020-01390-2
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DOI: https://doi.org/10.1007/s13204-020-01390-2