Hostname: page-component-586b7cd67f-r5fsc Total loading time: 0 Render date: 2024-11-24T14:13:16.116Z Has data issue: false hasContentIssue false

Nanocrystalline Nd2–yGdyZr2O7 pyrochlore: Facile synthesis and electrical characterization

Published online by Cambridge University Press:  31 January 2011

Balaji P. Mandal
Affiliation:
Chemistry Division, Bhabha Atomic Research Centre, Mumbai 400085, India
Atanu Dutta
Affiliation:
Central Glass and Ceramic Research Institute, CSIR, Kolkata 700032, India
S.K. Deshpande
Affiliation:
UGC-DAE Consortium for Scientific Research, Bhabha Atomic Research Centre, Mumbai 400085, India
R.N. Basu
Affiliation:
Central Glass and Ceramic Research Institute, CSIR, Kolkata 700032, India
Avesh K. Tyagi*
Affiliation:
Chemistry Division, Bhabha Atomic Research Centre, Mumbai 400085, India
*
a) Address all correspondence to this author. e-mail: [email protected]
Get access

Abstract

Three solid solutions of pyrochlores in the series Nd2-yearsGdyZr2O7 (y = 0.8, 1.0, 1.2) were synthesized by the gel combustion method using citric acid as fuel. This results in a soft agglomerate powder as verified by dynamic light scattering. The single-phase nature of the products has been confirmed by x-ray diffraction. The increase in full width at half-maxima in the Raman spectra with an increase in Gd3+ content indicates that disorder increases with Gd3+ content. The morphology and particle size of the products were investigated by transmission electron microscopy. Scanning electron microscopy study reveals that the sintered pellets have a density higher than 92% of theoretical densities. The total ionic conductivity measurements in the temperature range 375–800 °C show that with the increase of disorder (Gd3+ content) in the system the activation energy of conduction increases from 0.98 to 1.06 eV and the preexponential factor, which is proportional to the number of mobile species, also follow the same trend of increase. The total conductivity measured in reducing atmosphere shows no change in electrical conductivity, which verifies a negligible contribution of electronic contribution in this system.

Type
Articles
Copyright
Copyright © Materials Research Society 2009

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1Cho, Y.S., Glicksman, H.D. and Amarakoon, V.R.W.: Encylopedia of Nanoscience and Nanotechnology, Vol. 1, edited by Nalwa, H.S. (American Scientific Publishers, Stevenson Ranch, CA, 2004), p. 7.Google Scholar
2Moreno, K.J., Mendonza-Suarez, G., Fuentes, A.F., Garcia-Barriocanal, J., Leon, C. and Santamaria, J.: Mechanochemical synthesis and ionic conductivity in the Gd2(Sn1–yZry)2O7 (0 [notdef] y [notdef]1) solid solution. Phys. Rev. B 71, 132301 (2005).CrossRefGoogle Scholar
3Weller, M.T., Hughes, R.W., Rouke, J., Knee, C.S. and Reading, J.: The pyrochlore family—A potential panacea for the frustrated perovskite chemist. Dalton Trans. 3032 (2004).Google Scholar
4Moon, P.K. and Tuller, R.H.: Ionic conduction in the Gd2Ti2O7[C0] Gd2Zr2O7 system. Solid State Ionics 28, 470 (1988).CrossRefGoogle Scholar
5Pirzada, M., Grimes, R.W., Minervini, L., Maguire, J.F. and Sickafus, K.E.: Oxygen migration in A2B2O7 pyrochlores. Solid State Ionics 140, 201 (2001).CrossRefGoogle Scholar
6Mandal, B.P., Banerji, A., Sathe, V., Deb, S.K. and Tyagi, A.K.: Order-disorder transition in Nd2–yGdyZr2O7 pyrochlore solid solution: An x-ray diffraction and Raman spectroscopic study. J. Solid State Chem. 180, 2643 (2007).CrossRefGoogle Scholar
7Riess, I., Braunshtein, D. and Tannhauser, D.S.: Density and ionic conductivity of sintered (CeO2)0.82(GdO1.5)0.18. J. Am. Ceram. Soc. 64, 479 (1981).CrossRefGoogle Scholar
8Kingsley, J.J., Suresh, K. and Patil, K.C.: Combustion synthesis of fine-particle metal aluminates. J. Mater. Sci. 25, 1305 (1990).CrossRefGoogle Scholar
9Bhaduri, S., Bhaduri, S.B. and Zhou, E.: Auto ignition synthesis and consolidation of Al2O3–ZrO2 nano/nano composite powders. J. Mater. Res. 13, 156 (1998).CrossRefGoogle Scholar
10Dutta, A., Patra, S., Bedekar, V., Tyagi, A.K. and Basu, R.N.: Nanocrystalline gadolinium doped ceria: Combustion synthesis and electrical characterization. J. Nanosci. Nanotechnol. 9, 3075 (2009).CrossRefGoogle ScholarPubMed
11Mandal, B.P., Deshpande, S.K. and Tyagi, A.K.: Ionic conductivity enhancement in Gd2Zr2O7 pyrochlore by Nd doping. J. Mater. Res. 23, 911 (2008).CrossRefGoogle Scholar
12Pederson, L.R., Chick, L.A. and Exarhos, G.J.: Method of making metal oxide ceramic powders by using a combustible amino acid compound. U.S. Patent No. 5114702, May 19, 1992.Google Scholar
13Mandal, B.P. and Tyagi, A.K.: Preparation and high temperature-XRD studies on a pyrochlore series with the general composition Gd2–xNdxZr2O7. J. Alloys Compd. 437, 260 (2007).CrossRefGoogle Scholar
14Shannon, R.D.: Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr., Sect. A 32, 751 (1976).CrossRefGoogle Scholar
15Vandenborre, M.T., Husson, E., Chatry, J.P. and Michel, D.: Rare-earth titanates and stannates of pyrochlore structure; Vibrational spectra and force fields. J. Raman Spectrosc. 14, 63 (1983).CrossRefGoogle Scholar
16Bedekar, V., Chavan, S.V. and Tyagi, A.K.: Highly sinter-active nanocrystalline RE2O3 (RE = Gd, Eu, Dy) by a combustion process, and role of oxidant-to-fuel ratio in preparing their different crystallographic modifications. J. Mater. Res. 22, 587 (2007).CrossRefGoogle Scholar
17Hara, A., Hirata, Y., Sameshima, S., Matsunaga, N. and Horita, T.: Grain size dependence of electrical properties of Gd-doped ceria. J. Ceram. Soc. Jpn. 116, 291 (2008).CrossRefGoogle Scholar
18Ji, Y., Liu, J., He, T., Cong, L., Wang, J. and Su, W.: Single intermediate-temperature SOFC prepared by glycine-nitrate process. J. Alloys Compd. 353, 257 (2003).CrossRefGoogle Scholar
19Belous, A.G., Kravchyk, K.V., Pashkova, E.V., Bohnke, O. and Galven, C.: Influence of the chemical composition on structural properties and electrical conductivity of YCe–ZrO2. Chem. Mater. 19, 5179 (2007).CrossRefGoogle Scholar
20Abrantes, J.C.C., Levchenko, A., Shlyakhtina, A.V., Shcherbakova, L.G., Horovistiz, A.L., Fagg, D.P. and Frade, J.R.: Ionic and electronic conductivity of Yb2+xTi2–xO7–x/2 materials. Solid State Ionics 177, 1785 (2006).CrossRefGoogle Scholar
21Holtappels, P., Poulsen, F.W. and Mogensen, M.: Electrical conductivities and chemical stabilities of mixed conducting pyrochlores for SOFC applications. Solid State Ionics 135, 675 (2000).CrossRefGoogle Scholar
22Tuller, H.L.: Semiconduction and mixed ionic-electronic conduction in nonstoichiometric oxides: Impact and control. Solid State Ionics 94, 63 (1997).CrossRefGoogle Scholar
23Chapman, R.A., Meadowcrofts, D.B. and Walkden, A.J.: Some properties of zirconates and stannates with the pyrochlore structure. J. Phys. D: Appl. Phys. 3, 307 (1970).CrossRefGoogle Scholar
24Porat, O., Heremans, C. and Tuller, H.L.: Phase stability and electrical conductivity in Gd2Ti2O7–Gd2Mo2O7 solid solutions. J. Am. Ceram. Soc. 80, 2278 (1997).CrossRefGoogle Scholar