- Email: [email protected]
Synthesis and luminescent characterization of sol-gel derived zirconia–alumina
Radiation Measurements 45 (2010) 465e467
Contents lists available at ScienceDirect
Radiation Measurements journal homepage: www.elsevier.com/locate/radmeas
Synthesis and luminescent characterization of sol-gel derived zirconiaealumina T. Rivera a, *, R. Sosa b, J. Azorín b, J. Zarate c, A. Ceja c a
Centro de Investigación en Ciencia Aplicada y Tecnología Avanzada-IPN, Unidad Legaria, 11500 Mexico D.F., Mexico Departamento de Física, Universidad Autónoma Metropolitana-Iztapalapa, 09340 Mexico D.F., Mexico c Instituto de Investigaciones en Metalurgia, UMSNH, Edifico “U”, A.P. 888, 58060 Morelia, Mich., Mexico b
a r t i c l e i n f o
a b s t r a c t
Article history: Received 14 August 2009 Received in revised form 21 August 2009 Accepted 29 January 2010
Luminescence and sintering characteristics of a-Al2O3-tetragonal zirconia [t-ZrO2(Y2O3)] mixtures have been investigated. The pseudoboehmite is one of the main precursors of the a-alumina. In this investigation pseudoboehmite has been synthesized through a desulphatation of the commercial Al2(SO4)3 using an ammonia solution. Tetragonal zirconia powders were added in adequate proportion for each composition. The mixture constituted by Al2O3 (pseudoboehmite) and t-ZrO2 has been annealed at different temperatures to obtain the crystalline phases. XRD and SEM techniques measurements have been used to structural characterization. Photoluminescence (PL) emission spectra of Al2O3eZrO2 composites were performed at room temperature. Thermoluminescent emission spectrum of the samples was obtained and analyzed. Ó 2010 Elsevier Ltd. All rights reserved.
Keywords: Al2O3eZrO2 composites Pseudoboehmite Photoluminescence Thermoluminescence
1. Introduction Nanocrystalline ceramic powder promises high purity with homogeneity at the molecular level and submicrometre grain size after syntherization. Some advantages and disadvantages may observe during mixing steps in conventional ceramic powder preparation, which makes nanocrystalline ceramic powder very attractive for the fabrication of high-quality advanced ceramics. A number of nanocrystalline ceramic powders, such as TiO2 (Bhaduri et al., 1996; Panchula and Ying, 1997), Al2O3 (Srdic and Radonjic, 1994) and ZrO2 (Ponthieu et al.,1992; Zheng et al.,1998), have been produced by various methods includes sol-gel method (Piticescu et al., 2001), hydrolysis and precipitation (Avilda and Muccillo, 1995) and hydrothermal method (Matsui and Ohgai, 2000). Sol-gel synthesis has several advantages over other methods for producing nanocrystalline ceramic powder. Al2O3 was one of the materials studied very early for its potential application as a radiation dose-meter owing to its superior thermal and chemical stability and low effective atomic number (Kulkarni et al., 2005; Ranjan et al., 2000; Mehta and Sengupta, 1976; Osvay and Biro, 1980; Lapraz et al., 1991). The uniform dispersion of zirconia particles in the alumina matrix can be controlled by homogeneous powder synthesis techniques. The ZrO2eAl2O3 ceramic composites display different properties depending on the precursors, chemical composition and preparation
* Corresponding author. E-mail address: [email protected] (T. Rivera). 1350-4487/$ e see front matter Ó 2010 Elsevier Ltd. All rights reserved. doi:10.1016/j.radmeas.2010.01.046
route. The ZrO2eAl2O3 ceramic composite has been observed that the structure of the matrix material and the zirconia particles dispersed in the alumina matrix are so important in order to produce optimally tough transformation-toughened composite materials that increase the mechanical and thermal properties of the composite (Zhang and Glasser, 1993; Li et al., 1995). In The present work, structural characterization of ZrO2eAl2O3 composite is determined and related to luminescent application. 2. Experimental Homogeneous mixtures of pseudoboehmite with average formula Al4O3(OH)6 obtained from U.G. Process (Zarate et al., 2001) and t-ZrO2(Y2O3) were prepared by a mechanochemical treatment employing HNO3 as a peptising agent. The U.G. process is related with the alkaline desulphatation of Al2(SO4)3 using an ammonia solution (Zarate et al., 2001). Suspensions of precursory powders were prepared with pseudoboehmite seeded during mechanochemical treatment with 2.5 mass% a-Al2O3 of 0.20 mm (Taimicron, TM10) and tetragonal zirconia powders (TOSOH, TZ-3YS) with average particle size of 0.26 mm were added in adequate proportions for each composition (100, 90, 70, 50, 30, 15 and 0 mass % of ZrO2). The suspensions were stirred and spray dried using a YAMATO Mini-spray dryer ADL31. The precursory powders were submitted at 1200 C. The crystalline phases were characterized using X-ray diffraction techniques (Siemens D5000). Morphological characteristics of the powders have been obtained using the scanning electron microscope SEM (Jeol 6400). Photoluminescent
466
T. Rivera et al. / Radiation Measurements 45 (2010) 465e467
Fig. 4. Typical thermoluminescent glow curve of gamma irradiated Al2O3eZrO2. Fig. 1. Micrographs of the AI2O3eZrO2 composites sintered at 1100 C.
1000
ZTY SDI10 SDI30 SDI50 SDI70 SDI85 SDI95 SDI100
t
Intensity
800
600
m
characteristics of ZrO2eAl2O3 composites were determined using a UVeVIS Perkin Elmer spectrophotomer. Thermoluminescent glow curve of ZrO2eAl2O3 was also measured using a TL reader Harshaw 3500.
m
400
200
0
PB 10
PB 20
30
PB 40
PB 50
60
70
80
2 theta Fig. 2. XRD patterns of sintered aluminaezirconia composites. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
3. Results and discussion In Fig. 1. Scanning electron microscope measurement results of Al2O3eZrO2 composite show fine sized and homogeneous distribution particles with low porosity. In Fig. 2, XRD patterns of sintered Al2O3eZrO2 composites are presented. The characteristic peaks of tetragonal (t) zirconia and alpha (a) alumina phases are depicted. It is observed that as the % wt Al2O3 increases the characteristic peaks of zirconia tetragonal (t) phase decreases, while the a-Al2O3 phase increases. This phenomenon can be explained by the fact of the differences of the internal friction between a-Al2O3, the pseudoboehmite and t-ZrO2 particles in the sample packing process during the synthesizing. In Fig. 3 a typical photoluminescent (PL) spectrum of Al2O3eZrO2 taking at room temperature is observed. In this figure is shown a strong and broad band with its maximum intensity centered at 500 nm. This typical photoluminescence can be mainly attributed to the effect of the oxygen deficiencies. It is known that the oxygen vacancies can be induce the formation of new energy levels in the band gap which results in the PL emission by the radioactive recombination of a photo-excited hole with an electron occupying the oxygen vacancies. Fig. 4 shows a TL glow Al2O3eZrO2 under gamma irradiated which exhibit a thermoluminescent glow curve with a peak centered at around 350 C. Therefore, it can be concluded luminescent results compared to the thermoluminescent glow curve of the ceramic composite could be attributed of the sintering process and the t-ZrO2 % wt concentration.
4. Conclusions
Fig. 3. Typical photoluminescence of Al2O3eZrO2.
The structural and sintered of ZrO2eAl2O3 ceramic composite was determined from luminescent measurements. The results were found to be dependent upon the content of the Al2O3 and ZrO2 concentration. In both cases, the photoluminescent increase up to a maximum for about 100 wt % Al2O3 phase and decreases monotonically thereafter until it reaches the ZrO2 phase. The increase in luminescence is attributed to variation in the chemical composition and bonding of the ceramic composite material under study. This experimental work indicates that it is possible to obtain the luminescent material to thermoluminescent measurements.
T. Rivera et al. / Radiation Measurements 45 (2010) 465e467
Acknowledgements The work supported by a grant from The CGP-IPN Research Project 20090151. References Avilda, D.M., Muccillo, E.N.S., 1995. Thermochim. Acta 256, 391e398. Bhaduri, S., Zhou, E., Bhaduri, S.B., 1996. Nanostruct. Mater. 7, 487e496. Kulkarni, M.S., Mishra, D.R., Muthe, K.P., Singh, A., Roy, M., Gupta, S.K., et al., 2005. Radiat. Meas. 39, 277e282.
467
Lapraz, D., Iacconi, P., Daviller, D., et al.,1991. Phys. Status Solidi A Appl. Res.126, 521e531. Li, C., Chen, Y.W., Yen, T.M., 1995. J. Sol-Gel Sci. Technol. 4, 205e215. Matsui, K., Ohgai, M., 2000. J. Am. Ceram. Soc. 83, 1386e1392. Mehta, S.K., Sengupta, S., 1976. Phys. Med. Biol. 21, 955e964. Osvay, M., Biro, T., 1980. Nucl. Instrum. Methods 175, 60e61. Panchula, M.L., Ying, J.Y., 1997. Nanostruct. Mater. 9, 161e164. Piticescu, R.R., Monty, C., Taloi, D., Motoc, A., Axinte, S., 2001. J. Eur. Ceram. Soc. 21, 2057e2060. Ponthieu, E., Payen, E., Grimblot, J., 1992. J. Non-Cryst. Solids 147e148, 598e605. Ranjan, K., Jagadish, C., Panchanan, P., 2000. Mater. Lett. 44, 299e303. Srdic, V., Radonjic, L., 1994. J. Eur. Ceram. Soc. 14, 237e244. Zhang, W., Glasser, F.P., 1993. J. Eur. Ceram. Soc. 11, 149e155. Zarate, J., Juarez, H., Contreras, M.E., Tartaj, J., Balmori, H., 2001. Atm 3, 19e26. Zheng, W.M., Gao, L., Guo, J.K., 1998. Nanostruct. Mater. 10, 543e550.
Contents lists available at ScienceDirect
Radiation Measurements journal homepage: www.elsevier.com/locate/radmeas
Synthesis and luminescent characterization of sol-gel derived zirconiaealumina T. Rivera a, *, R. Sosa b, J. Azorín b, J. Zarate c, A. Ceja c a
Centro de Investigación en Ciencia Aplicada y Tecnología Avanzada-IPN, Unidad Legaria, 11500 Mexico D.F., Mexico Departamento de Física, Universidad Autónoma Metropolitana-Iztapalapa, 09340 Mexico D.F., Mexico c Instituto de Investigaciones en Metalurgia, UMSNH, Edifico “U”, A.P. 888, 58060 Morelia, Mich., Mexico b
a r t i c l e i n f o
a b s t r a c t
Article history: Received 14 August 2009 Received in revised form 21 August 2009 Accepted 29 January 2010
Luminescence and sintering characteristics of a-Al2O3-tetragonal zirconia [t-ZrO2(Y2O3)] mixtures have been investigated. The pseudoboehmite is one of the main precursors of the a-alumina. In this investigation pseudoboehmite has been synthesized through a desulphatation of the commercial Al2(SO4)3 using an ammonia solution. Tetragonal zirconia powders were added in adequate proportion for each composition. The mixture constituted by Al2O3 (pseudoboehmite) and t-ZrO2 has been annealed at different temperatures to obtain the crystalline phases. XRD and SEM techniques measurements have been used to structural characterization. Photoluminescence (PL) emission spectra of Al2O3eZrO2 composites were performed at room temperature. Thermoluminescent emission spectrum of the samples was obtained and analyzed. Ó 2010 Elsevier Ltd. All rights reserved.
Keywords: Al2O3eZrO2 composites Pseudoboehmite Photoluminescence Thermoluminescence
1. Introduction Nanocrystalline ceramic powder promises high purity with homogeneity at the molecular level and submicrometre grain size after syntherization. Some advantages and disadvantages may observe during mixing steps in conventional ceramic powder preparation, which makes nanocrystalline ceramic powder very attractive for the fabrication of high-quality advanced ceramics. A number of nanocrystalline ceramic powders, such as TiO2 (Bhaduri et al., 1996; Panchula and Ying, 1997), Al2O3 (Srdic and Radonjic, 1994) and ZrO2 (Ponthieu et al.,1992; Zheng et al.,1998), have been produced by various methods includes sol-gel method (Piticescu et al., 2001), hydrolysis and precipitation (Avilda and Muccillo, 1995) and hydrothermal method (Matsui and Ohgai, 2000). Sol-gel synthesis has several advantages over other methods for producing nanocrystalline ceramic powder. Al2O3 was one of the materials studied very early for its potential application as a radiation dose-meter owing to its superior thermal and chemical stability and low effective atomic number (Kulkarni et al., 2005; Ranjan et al., 2000; Mehta and Sengupta, 1976; Osvay and Biro, 1980; Lapraz et al., 1991). The uniform dispersion of zirconia particles in the alumina matrix can be controlled by homogeneous powder synthesis techniques. The ZrO2eAl2O3 ceramic composites display different properties depending on the precursors, chemical composition and preparation
* Corresponding author. E-mail address: [email protected] (T. Rivera). 1350-4487/$ e see front matter Ó 2010 Elsevier Ltd. All rights reserved. doi:10.1016/j.radmeas.2010.01.046
route. The ZrO2eAl2O3 ceramic composite has been observed that the structure of the matrix material and the zirconia particles dispersed in the alumina matrix are so important in order to produce optimally tough transformation-toughened composite materials that increase the mechanical and thermal properties of the composite (Zhang and Glasser, 1993; Li et al., 1995). In The present work, structural characterization of ZrO2eAl2O3 composite is determined and related to luminescent application. 2. Experimental Homogeneous mixtures of pseudoboehmite with average formula Al4O3(OH)6 obtained from U.G. Process (Zarate et al., 2001) and t-ZrO2(Y2O3) were prepared by a mechanochemical treatment employing HNO3 as a peptising agent. The U.G. process is related with the alkaline desulphatation of Al2(SO4)3 using an ammonia solution (Zarate et al., 2001). Suspensions of precursory powders were prepared with pseudoboehmite seeded during mechanochemical treatment with 2.5 mass% a-Al2O3 of 0.20 mm (Taimicron, TM10) and tetragonal zirconia powders (TOSOH, TZ-3YS) with average particle size of 0.26 mm were added in adequate proportions for each composition (100, 90, 70, 50, 30, 15 and 0 mass % of ZrO2). The suspensions were stirred and spray dried using a YAMATO Mini-spray dryer ADL31. The precursory powders were submitted at 1200 C. The crystalline phases were characterized using X-ray diffraction techniques (Siemens D5000). Morphological characteristics of the powders have been obtained using the scanning electron microscope SEM (Jeol 6400). Photoluminescent
466
T. Rivera et al. / Radiation Measurements 45 (2010) 465e467
Fig. 4. Typical thermoluminescent glow curve of gamma irradiated Al2O3eZrO2. Fig. 1. Micrographs of the AI2O3eZrO2 composites sintered at 1100 C.
1000
ZTY SDI10 SDI30 SDI50 SDI70 SDI85 SDI95 SDI100
t
Intensity
800
600
m
characteristics of ZrO2eAl2O3 composites were determined using a UVeVIS Perkin Elmer spectrophotomer. Thermoluminescent glow curve of ZrO2eAl2O3 was also measured using a TL reader Harshaw 3500.
m
400
200
0
PB 10
PB 20
30
PB 40
PB 50
60
70
80
2 theta Fig. 2. XRD patterns of sintered aluminaezirconia composites. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
3. Results and discussion In Fig. 1. Scanning electron microscope measurement results of Al2O3eZrO2 composite show fine sized and homogeneous distribution particles with low porosity. In Fig. 2, XRD patterns of sintered Al2O3eZrO2 composites are presented. The characteristic peaks of tetragonal (t) zirconia and alpha (a) alumina phases are depicted. It is observed that as the % wt Al2O3 increases the characteristic peaks of zirconia tetragonal (t) phase decreases, while the a-Al2O3 phase increases. This phenomenon can be explained by the fact of the differences of the internal friction between a-Al2O3, the pseudoboehmite and t-ZrO2 particles in the sample packing process during the synthesizing. In Fig. 3 a typical photoluminescent (PL) spectrum of Al2O3eZrO2 taking at room temperature is observed. In this figure is shown a strong and broad band with its maximum intensity centered at 500 nm. This typical photoluminescence can be mainly attributed to the effect of the oxygen deficiencies. It is known that the oxygen vacancies can be induce the formation of new energy levels in the band gap which results in the PL emission by the radioactive recombination of a photo-excited hole with an electron occupying the oxygen vacancies. Fig. 4 shows a TL glow Al2O3eZrO2 under gamma irradiated which exhibit a thermoluminescent glow curve with a peak centered at around 350 C. Therefore, it can be concluded luminescent results compared to the thermoluminescent glow curve of the ceramic composite could be attributed of the sintering process and the t-ZrO2 % wt concentration.
4. Conclusions
Fig. 3. Typical photoluminescence of Al2O3eZrO2.
The structural and sintered of ZrO2eAl2O3 ceramic composite was determined from luminescent measurements. The results were found to be dependent upon the content of the Al2O3 and ZrO2 concentration. In both cases, the photoluminescent increase up to a maximum for about 100 wt % Al2O3 phase and decreases monotonically thereafter until it reaches the ZrO2 phase. The increase in luminescence is attributed to variation in the chemical composition and bonding of the ceramic composite material under study. This experimental work indicates that it is possible to obtain the luminescent material to thermoluminescent measurements.
T. Rivera et al. / Radiation Measurements 45 (2010) 465e467
Acknowledgements The work supported by a grant from The CGP-IPN Research Project 20090151. References Avilda, D.M., Muccillo, E.N.S., 1995. Thermochim. Acta 256, 391e398. Bhaduri, S., Zhou, E., Bhaduri, S.B., 1996. Nanostruct. Mater. 7, 487e496. Kulkarni, M.S., Mishra, D.R., Muthe, K.P., Singh, A., Roy, M., Gupta, S.K., et al., 2005. Radiat. Meas. 39, 277e282.
467
Lapraz, D., Iacconi, P., Daviller, D., et al.,1991. Phys. Status Solidi A Appl. Res.126, 521e531. Li, C., Chen, Y.W., Yen, T.M., 1995. J. Sol-Gel Sci. Technol. 4, 205e215. Matsui, K., Ohgai, M., 2000. J. Am. Ceram. Soc. 83, 1386e1392. Mehta, S.K., Sengupta, S., 1976. Phys. Med. Biol. 21, 955e964. Osvay, M., Biro, T., 1980. Nucl. Instrum. Methods 175, 60e61. Panchula, M.L., Ying, J.Y., 1997. Nanostruct. Mater. 9, 161e164. Piticescu, R.R., Monty, C., Taloi, D., Motoc, A., Axinte, S., 2001. J. Eur. Ceram. Soc. 21, 2057e2060. Ponthieu, E., Payen, E., Grimblot, J., 1992. J. Non-Cryst. Solids 147e148, 598e605. Ranjan, K., Jagadish, C., Panchanan, P., 2000. Mater. Lett. 44, 299e303. Srdic, V., Radonjic, L., 1994. J. Eur. Ceram. Soc. 14, 237e244. Zhang, W., Glasser, F.P., 1993. J. Eur. Ceram. Soc. 11, 149e155. Zarate, J., Juarez, H., Contreras, M.E., Tartaj, J., Balmori, H., 2001. Atm 3, 19e26. Zheng, W.M., Gao, L., Guo, J.K., 1998. Nanostruct. Mater. 10, 543e550.