Abstract
The SrO(SrTiO3)1 (Sr2TiO4) Ruddlesden Popper (RP) phase is a natural superlattice comprising of alternately stacking perovskite-type SrTiO3 layers and rock salt SrO layers along the crystallographic c direction. This paper discusses the properties of the Sr2TiO4 and (La, Sm)-doped Sr2TiO4 RP phase synthesized via molten salt method, within the context of thermoelectric applications. A good thermoelectric material requires high electrical conductivity, high Seebeck coefficient and low thermal conductivity. All three conditions have the potential to be fulfilled by the Sr2TiO4 RP phase, in particular, the superlattice structure allows a higher degree of phonon scattering hence resulting in lowered thermal conductivity. In this work, the Sr2TiO4 RP phase is doped with Sm and La respectively, which allows injection of charge carriers, modification of its electronic structure for improvement of the Seebeck coefficient, and most significantly, reduction of thermal conductivity. The particles with submicron size allows excessive phonon scattering along the boundaries, thus reduces the thermal conductivity by fourfold. In particular, the Sm-doped sample exhibited even lower lattice thermal conductivity, which is believed to be due to the mismatch in the ionic radius of Sr and Sm. This finding is useful as a strategy to reduce thermal conductivity of Sr2TiO4 RP phase materials as thermoelectric candidates, by employing dopants of differing ionic radius.
Similar content being viewed by others
References
Ruddlesden, S.N., Popper, P.: The compound Sr3Ti2O7 and its structure. Acta Crystallogr. 11, 54–55 (1958)
Ruddlesden, S.N., Popper, P.: New compounds of the K2NIF4 type. Acta Crystallogr. 10, 538–539 (1957)
Zhang, L., et al.: First principles studies on the thermoelectric properties of (SrO)m (SrTiO3)n superlattice. RSC Adv. 6, 102172–102182 (2016)
Haeni, J.H., et al.: Epitaxial growth of the first five members of the Srn+1TinO3n+1 Ruddlesden–Popper homologous series. Appl. Phys. Lett. 78, 3292–3294 (2001)
Tsai, H., et al.: High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells. Nature 536, 312–316 (2016)
Arredondo, M., et al.: Chemistry of Ruddlesden–Popper planar faults at a ferroelectric-ferromagnet perovskite interface. J. Appl. Phys. 109, 084101 (2011)
Koh, T.M., Febriansyah, B., Mathews, N.: Ruddlesden–Popper perovskite solar cells. Chem 2, 326–327 (2017)
Birol, T., Benedek, N.A., Fennie, C.J.: Interface control of emergent ferroic order in Ruddlesden–Popper Srn+1TinO3n+1. Phys. Rev. Lett. 107, 257602 (2011)
Chen, Y., Zhao, Y., Liang, Z.: Solution processed organic thermoelectrics: towards flexible thermoelectric modules. Energy Environ. Sci. 8, 401–422 (2015)
Lee, K.H., Ishizaki, A., Kim, S.W., Ohta, H., Koumoto, K.: Preparation and thermoelectric properties of heavily Nb-doped SrO (SrTiO3)1 epitaxial films. J. Appl. Phys. 102, 033702 (2007)
Reshak, A.H.: Thermoelectric properties of Srn+1TinO3n+1 (n = 1, 2, 3, ∞) Ruddlesden–Popper homologous series. Renew. Energy 76, 36–44 (2015)
Lee, K.H., Kim, S.W., Ohta, H., Koumoto, K.: Ruddlesden–Popper phases as thermoelectric oxides: Nb-doped SrO(SrTiO3)n (n = 1,2). J. Appl. Phys. 100, 063717 (2006)
Hungria, T., MacLaren, I., Fuess, H., Galy, J., Castro, A.: HREM studies of intergrowths in Sr2[Srn−1TinO3n+1] Ruddlesden–Popper phases synthesized by mechanochemical activation. Mater. Lett. 62, 3095–3098 (2008)
Hungría, T., Lisoni, J.G., Castro, A.: Sr3Ti2O7 Ruddlesden–Popper phase synthesis by milling routes. Chem. Mater. 14, 1747–1754 (2002)
Gutmann, E., et al.: Oriented growth of Srn+1TinO3n+1 Ruddlesden–Popper phases in chemical solution deposited thin films. J. Solid State Chem. 179, 1864–1869 (2006)
Liu, Y.F., Lu, Y.N., Xu, M., Zhoun, L.F.: Formation mechanisms of platelet Sr3Ti2O7 crystals synthesized by the molten salt synthesis method. J. Am. Ceram. Soc. 90, 1774–1779 (2007)
Watari, K., Brahmaroutu, B., Messing, G.L., Trolier-Mckinstry, S., Cheng, S.-C.: Epitaxial growth of anisotropically shaped, single-crystal particles of cubic SrTiO3. J. Mater. Res. 15, 846–849 (2000)
Liu, Y.F., Lu, Y.N., Xu, M., Zhou, L.F., Shi, S.Z.: Topochemical reaction of SrTiO3 platelet crystals based on Sr3Ti2O7 platelet precursor in molten salt synthesis process. Mater. Chem. Phys. 114, 37–42 (2009)
Arendt, R.H., Rosolowski, J.H., Szymaszek, J.W.: Lead zirconate titanate ceramics from molten salt solvent synthesized powders. Mater. Res. Bull. 14, 703–709 (1979)
Oku, M., Wagatsuma, K., Kohiki, S.: Ti 2p and Ti 3p X-ray photoelectron spectra for TiO2, SrTiO3 and BaTiO3. Phys. Chem. Chem. Phys. 1, 5327–5331 (1999)
Myhre, K., et al.: Samarium electrodeposited acetate and oxide thin films on stainless steel substrate characterized by XPS Samarium electrodeposited acetate and oxide thin films on stainless steel substrate characterized by XPS. Surf. Sci. Spectra 23, 70 (2016)
Long, C., Fan, H.: Effect of lanthanum substitution at A site on structure and enhanced properties of new Aurivillius oxide K0.25Na0.25La0.5Bi2Nb2O9. Dalton Trans. 41, 11046 (2012)
Sugimoto, W.: Synthesis and structures of carrier doped titanates with the Ruddlesden–Popper structure (Sr0.95La0.05)n+1TinO3n+1 (n = 1, 2). Solid State Ion. 108, 315–319 (1998)
Warren, W.L., Vanheusden, K., Dimos, D., Pike, G.E., Tuttle, B.A.: Oxygen vacancy motion in perovskite oxides. J. Am. Ceram. Soc. 79, 536–538 (1996)
Trabelsi, H., et al.: Effect of oxygen vacancies on SrTiO3 electrical properties. J. Alloys Compd. 723, 894–903 (2017)
Wang, Y., Lee, K.H., Ohta, H., Koumoto, K.: Thermoelectric properties of electron doped SrO (SrTiO3)n (n = 1,2) ceramics. J. Appl. Phys. 105, 103 (2009)
Mamand, S.M., Omar, M.S., Muhammad, A.J.: Nanoscale size dependence parameters on lattice thermal conductivity of Wurtzite GaN nanowires. Mater. Res. Bull. 47, 1264–1272 (2012)
Abeles, B.: Lattice thermal conductivity of disordered semiconductor alloys at high temperatures. Phys. Rev. 131, 1906–1911 (1963)
Muta, H., Kurosaki, K., Yamanaka, S.: Thermoelectric properties of rare earth doped SrTiO3. J. Alloys Compd. 350, 292–295 (2003)
Acknowledgements
The work was supported by Ministry of Research, Technology and Higher Education of the Republic Indonesia through Research Institute and Community Service (Riset Dasar Grant No. 19/UN.16.03.D/PP/FMIPA/2017) and Domestic Seminar Assistance Program of Andalas University.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Putri, Y.E., Said, S.M., Refinel, R. et al. Low Thermal Conductivity of RE-Doped SrO(SrTiO3)1 Ruddlesden Popper Phase Bulk Materials Prepared by Molten Salt Method. Electron. Mater. Lett. 14, 556–562 (2018). https://doi.org/10.1007/s13391-018-0062-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s13391-018-0062-x