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59. Inorganic Perovskite Oxides Pe 59 | E Part R Tatsumi Ishihara

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59. Inorganic Perovskite Oxides Pe 59 | E Part R Tatsumi Ishihara 1405 Inorganic59. Inorganic Perovskite Oxides PePart E | 59 r Tatsumi Ishihara 59.1 Typical Properties Crystal structure and important functions of of Perovskite Oxides .......................... 1409 inorganic perovskite oxides are introduced. Pe- 59.1.1 Dielectric Properties........................... 1409 rovskite oxides comprise large families among 59.1.2 Electrical Conductivity the structures of oxide compounds, and sev- and Superconductivity ....................... 1409 eral perovskite-related structures are currently 59.1.3 Catalytic Activity ................................ 1410 recognized. Typical structures (ABO3) consist of large-sized 12-coordinated cations at the A-site 59.2 Photocatalytic Activity....................... 1411 and small-sized 6-coordinated cations at the 59.3 Application for Solid Oxide B-site. Several complex halides and sulfides and Fuel Cells (SOFCs) ............................... 1413 many complex oxides have a perovskite structure. 59.3.1 Cathode............................................ 1413 From a variety of compositions and structures, 59.3.2 Anode .............................................. 1414 a variety of functions are observed in perovskite 59.3.3 Electrolyte......................................... 1415 oxides. In particular high electronic conductivity, 59.3.4 Interconnector .................................. 1417 which is at a similar level as metal, and surface 59.4 Oxygen Separating Membrane ........... 1418 activity to oxygen dissociation, are highly attrac- tive in this oxide. Perovskite oxide is now widely 59.5 Summary.......................................... 1419 used for solid oxide fuel cells. References................................................... 1420 Oxide groups consisting of two or more different two different cations. The ilmenite structure has the cations are called complex or mixed oxides, and many same composition as the perovskite one, i. e., ABO3; types of crystal structures are known. In some special however, A and B in this structure are cations of ap- cases, oxides consisting of single cations in different proximately the same size, which occupy an octahedral oxidation states are also classified as mixed oxides. site. Therefore, in spite of the fact that they share the For example, in Eu3O4, the mixed oxide consists of same general chemical formula, structures classified as Eu(III) and Eu(II) in 6- or 8-coordination respectively. ilumenite- or ilmenite-related structures (e.g., LiSbO3) However, the most typical structure of a mixed ox- are different from perovskite. ide consists simply of two or more different cations Perovskite oxides comprise large families among with different oxidation states, ionic radii, and coor- the structures of oxide compounds, and several dination numbers. This diversity, which comes from perovskite-related structures are currently recognized. the complexity of these structures, results in a larger Typical structures consist of large-sized 12-coordinated number of different properties as compared to those of cations at the A-site and small-sized 6-coordinated simple oxides. One of the most well known and im- cations at the B-site. Several complex halides and sul- portant complex oxide structures is the spinel structure fides and many complex oxides have a perovskite struc- (AB2O4), which shows important magnetic properties. ture. In particular, (Mg,Fe)SiO3 or CaSiO3 is thought to The structure of such oxides displays a most interesting be the predominant compound in the geosphere [59.1, complexity. Since the size of the A and B ions in this 2]. Perovskite compounds with different combinations structure is close, oxides of this type are typical exam- of charged cations in the A and B-sites, for example ples of the versatility of mixed oxides. 1 C 5, 2 C 4and3C 3, have been discovered. Even Another important structure of mixed oxide is pe- more complex combinations are observed, such as . 0 00 / 0 00 rovskite and a variety of related structures are classified Pb B1=2B1=2 O3,whereB D Sc, Fe and B D Nb, Ta, . 0 00 / 0 00 as this oxide. The typical chemical formula of the pe- or La B1=2B1=2 O3,whereB D Ni, Mg, etc. and B D rovskite structure is ABO3, where A and B denotes Ru(IV) or Ir(IV). In addition, many ABO3 compounds © Springer International Publishing AG 2017 S. Kasap, P. Capper (Eds.), Springer Handbook of Electronic and Photonic Materials, DOI 10.1007/978-3-319-48933-9_59 1406 Part E Novel Materials and Selected Applications Part E | 59 Table 59.1 Typical peroskite compound O Compound Lattice parameter (Å) a b c B ion Cubic structure KTaO3 3:989 NaTaO3 3:929 NaNbO3 3:949 BaMnO3 4:040 A ion BaZrO3 4:193 SrTiO3 3:904 KMnF3 4:189 KFeF3 4:121 Tetragonal structure BiAlO3 7:61 7:94 PbSnO3 7:86 8:13 BaTiO3 3:994 4:038 Fig. 59.1 Ideal cubic perovskite structure PdTiO3 3:899 4:153 TlMnCl3 5:02 5:04 crystallize in polymorphic structures, which show only LaAlO3 type ı 0 a small distortion from the most symmetrical form of LaAlO3 5:357 ˛ D 60 06 ı 0 the perovskite structure. LaNiO3 5:461 ˛ D 60 05 ı 0 The ideal structure of perovskite, which is illus- BiFeO3 5:632 ˛ D 60 06 ı 0 trated in Fig. 59.1, is a cubic lattice. Although few KNbO3 4:016 ˛ D 60 06 compounds have this ideal cubic structure, many oxides GdFeO3 type have slightly distorted variants with lower symmetry GdFeO3 5:346 5:616 7:668 (e.g., hexagonal or orthorhombic). Furthermore, even YFeO3 5:283 5:592 7:603 though some compounds have ideal cubic structure, NdGaO3 5:426 5:502 7:706 many oxides display slightly distorted variants with CaTiO3 5:381 5:443 7:645 : : : lower symmetry. Several examples of perovskite oxides NaMgF3 5 363 5 503 7 676 are listed in Table 59.1, where it is clear that a large number of perovskite oxides have a rombohedral lat- In perovskite-type compounds, the value of t lies be- tice. Additionally, in many compounds a large extent of tween approximately 0:80 and 1:10. It is noted that the oxygen or cation deficiency has been observed. Due to oxides with the lower t values crystallize in the ilmenite the large lattice energy, many compounds are classified structure, which is a polymorph of the perovskite struc- as perovskite oxides in spite of the large cation and/or ture. It seems superfluous to say that for the ideal cubic oxygen deficiencies. There are various types of distor- structure, the value of t is close to 1 or at least higher tions in the perovskite structure that are strongly related than 0:89. Figure 59.2 shows the crystal groups for 2C 4C 3C 3C to their properties, in particular their ferromagnetic or A B O3 and A B O3 combinations, which are ferroelectricity. related to deviation from the ideal structure [59.3]. As In order to understand the deviations from the ideal the value of t decreases, the structure of the unit lattice cubic structure, these ABO3 oxides are first regarded as is shifted from cubic to triclinic due to the increased dis- purely ionic crystals. In the case of the ideal structure, tortions. Figure 59.3 shows chemical elements that can the following relationship between the radii of the A, B, be accommodated within the perovskite structure. It is and O2 ions holds true evident that almost all elements except for noble gases p can occupy either A or B lattice positions in the per- rA C rO D 2.rB C rO/: ovskite structure, including dopants. The stability and the crystal group is mainly determined by the ratio of Therefore, the deviation from the ideal structure in per- the ionic radii of the A and B cations. Indeed, the struc- ovskite oxides can be expressed through the following ture is dependent not only on the size but also on the so-called tolerance factor t nature of the A and B atoms. For example, AMnO3 compounds crystallize in the perovskite structure when A cation is La or Ce–Dy, whereas a new hexagonal .rA C rO/ t D p structure with 5- and 7-coordination of Mn and A re- . / 2 rB C rO spectively, is formed when A D HoLu or Y if A D La Inorganic Perovskite Oxides Inorganic Perovskite Oxides 1407 Part E | 59 2+ 4 3+ 3+ a) A B O3 b) A B O3 Ionic Mn4+ Ti4+ Hf4+ U4+ Ionic Al3+ Cr3+ Sc3+ Y3+ Nd3+ La3+ size (Å) V4+ Sn4+ Zr4+ Ce4+ Th4+ size (Å) Ga3+ Fe3+ Ti3+ In3+ Sm3+ Ce3+ 1.35 Ba2+ 1.20 Rhombo- La2O3 3+ Tetragonal type La 1.30 Cubic –c < 1 hedral a 1.10 Ce3+ c Perovskite Nd3+ 1.25 – > 1 a 1.00 Sm3+ 2+ 1.20 SrVO Pseudo Pb 3+ 3 cubic 0.90 Orthorhombic Y Eu2+ 1.15 3+ 2+ In Sr 0.80 3+ Tl O type Sc 1.10 Pseudo Rhombohedral 2 3 cubic 0.70 1.05 Corundum Fe3+ Cr3+ Orthorhombic 0.60 3+ 1.00 Ca2+ Ca 2+ Cd 3+ 0.95 0.50 Al 0.55 0.60 0.65 0.70 0.75 0.80 0.85 0.90 0.95 1.00 1.05 0.40 0.50 0.60 0.70 0.80 0.90 1.00 1.10 1.20 1.30 Ionic size (Å) Ionic size (Å) Fig. 59.2a,b The effect of ionic size of A- and B-site cations on the observed distortions of the perovskite structure; 2C 4C 3C 3C (a) A B O3 case (b) A B O3 case Fig. 59.3 Chemical elements that can IA 0 occupy cation sites in the perovskite A-site cation 1 H IIA IIIB IVB VB VIBVIIB He structure 2 Li Be B-site cation BCNOFNe VIII 3 Na Mg IIIA IVA VA VIA VIIA IB IIB Al Si P S Cl Ar 4 KCaScTiVCrMnFeCoNiCuZnGaGeAsSeBrKr 5 Rb Sr Y Zr NbMo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe 6 Cs Ba La Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi Po At Rn 7 Fr Ra Ac Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Th Pa U Np Pu Am Cm Bk Cf Es Fm Md No Lr or Ce–Dy [59.4].
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