Junichiro Mizusaki

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• Dr. Engineering
• Professor Emeritus at Tohoku University

So far tremendous works have been reported on the oxide-ion conductivity of fluorite-type oxides typically stabilized zirconia and doped ceria. It is well known that the oxide-ion conductivity vs. dopant concentration plot shows maximum around 10 mol percent dopant concentration and the maximum conductivity varies with the dopant species. Interests...

Solid oxide fuel cell (SOFC) technology has made significant progress in the past 30 years and is currently in the early commercialization stage. The progress of the technology can be seen clearly through review of the papers and presentations at the biennial International Symposium on Solid Oxide Fuel Cells series initiated in 1989. This paper det...

In this paper we try to tailor the chemical stability of cobalt-rich perovskite Ba0.5Sr0.5Co0.8Fe0.2O3 − δ (BSCF) by B-site doping Sb. The chemical stability of Ba0.5Sr0.5Co0.8Fe0.1Sb0.1O3 − δ (BSCFS) was investigated by studying the oxygen nonstoichiometry, crystal structure and oxidation state by means of coulometric titration, high-temperature X...

Temperature and oxygen partial pressure, P(O2), dependence of oxygen nonstoichiometry of LaNi0.6Fe0.4O3 − δ, which is a new candidate cathode material for solid oxide fuel cells, has been determined by the equilibrium thermogravimetry. The P(O2) and temperature dependence of the electrical conductivity of LaNi0.6Fe0.4O3 − δ has also been measured....

In this review, two topics are selected from the application of fluorite-type defective oxides in the field of solid state ionics. One is on the nature of oxygen ionic conductivity maximum with dopant concentration. Oxygen vacancy diffusion coefficients of various systems were calculated from the reported ionic conductivity data and were displayed...

Fluorite-based oxide materials such as stabilized zriconias, doped cerias, and urania represent a group of the most important key engineering materials in our modern society, with their well-known various electrochemical, ceramic and nuclear etc. applications. This is primarily due to their multi-lateral excellent physical/chemical properties such...

To evaluate the electrochemical and electronic properties of strained film specimen, La1−xSrxCoO3−δ (x = 0.4, 0.5) films were evaluated by means of electrochemical impedance spectroscopy and electrical conductivity measurement. Dense polycrystalline La1−xSrxCoO3−δ films were fabricated on a polycrystalline Ce0.9Gd0.1O1.95 substrate by a pulsed lase...

In order to survey history and state of art of theoretical and kinetic studies of gas electrode reaction on solid oxide electrolyte, overview was made on the research works reported by the author and his co-investigators. Through reviewing their works, frontier of research is clarified. It was shown that electrode reaction is controlled by non-fara...

The orthorhombic-tetragonal structural phase transition behaviors of Pr2NiO4 + δ and Nd2NiO4 + δ were investigated by DSC and TG-DTA under controlled oxygen partial pressure, P(O2), and their difference was discussed. A discrete weight variation originating from the variation of oxide ion content, Δδ, was observed during the phase transition in bot...

The oxygen nonstoichiometry and the crystal structure of Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) were investigated by using coulometric titration, high-temperature gravimetry and in situ HT-XRD. The chemical stability diagram of BSCF was established as a function of temperature between room temperature and 1373 K and oxygen partial pressure, p(O2), between...

In this study, the crystal structures and the thermal expansibilities of La1 − xSrxMnO3 + δ (LSM) with oxygen stoichiometric composition, δ = 0, were studied by an atmosphere and temperature controlled X-Ray diffractometer (XRD). Pre-heat-treatment conditions for the samples and oxygen partial pressures for XRD measurements at high temperature were...

Structural phase transition behavior of Pr2NiO4+δ, which attracts interest as new cathode material for solid oxide fuel cells, was investigated by DSC and TG–DTA under controlled oxygen partial pressure, P(O2). It was revealed that the structural phase transition from orthorhombic phase to tetragonal phase involved discrete decrease of oxygen conte...

To evaluate the electrochemical and electronic properties of strained film specimen, La 1−x Sr x CoO 3−δ (x = 0.4, 0.5) films were evaluated by means of electrochemical impedance spectroscopy and electrical conductivity measurement. Dense polycrystalline La 1−x Sr x CoO 3−δ films were fabricated on a polycrystalline Ce 0.9 Gd 0.1 O 1.95 substrate b...

We previously developed a technique by which to measure the mechanical damage of SOFC using the acoustic emission (AE) method. In the present paper, we applied an adapted Self-Organizing Map (SOM), which is an artificial neural network model, to produce a cluster map reflecting the similarity of AE events. The obtained map visualized the change in...

Cubic perovskite Ba0.5Sr0.5Co0.8Fe0.1R0.1O3-delta (R=Fe, Nb, Mo, Sb) was synthesized, and the chemical stability under high oxygen partial pressure (p(O-2)) was studied by using HT-XRD in the temperature range of 773-1373 K. It was found that Ba0.5Sr0.5Co0.8Fe0.1Sb0.1O3-delta was remarkably stable than Ba0.5Sr0.5Co0.8Fe0.1Sb0.1O3-delta and Ba0.5Sr0...

The effect of cation composition in LaNi1-xFexO3-delta on oxygen nonstoichiometry has been investigated with iodometric titration. For LaNi0.6Fe0.4O3-delta, temperature and oxygen partial pressure dependence of oxygen nonstoichiometry has been determined by equilibrium thermogravimetry. The P(O-2) and temperature dependence of the electrical conduc...

The effect of Mn-doping on the stability of ScSZ electrolyte under dual atmosphere of solid oxide fuel cells (SOFCs) was investigated in this study. Scandia stabilized zirconia electrolytes with and without 5 mol % MnO2 (ScSZ and Mn-ScSZ) were annealed under dual atmosphere of air and 1.2%H2O-H2 at T = 1273 K. The surfaces of the ScSZ electrolytes...

La0.6Sr0.4Co1 − yFeyO3 − δ (LSCF) mixed-conducting perovskite oxides, a SOFC cathode candidate material, exhibit oxygen nonstoichiometry under reducing atmosphere and elevated temperatures. Reduction of the B-site transition metals and formation of oxygen vacancies result in chemical expansion of the LSCF lattice. Knowledge of both thermal and chem...

Comprehensive modeling of the spectra of the state-of-the-art Ni–YSZ/YSZ/LSM solid oxide cells including the instrumental stray impedance allowed the systematic deconvolution of the four major polarization losses ranging over one order of impedance magnitude. The stray impedance can be successfully modeled as an inductor connected in parallel with...

The oxygen nonstoichiometry of La0.6Sr0.4CoO3−δ has been the topic of various reports in the literature, but has been exclusively measured at high oxygen partial pressures, pO2, and/or elevated temperatures. For applications of La0.6Sr0.4CoO3−δ, such as solid oxide fuel cell cathodes or oxygen permeation membranes, knowledge of the oxygen nonstoich...

The oxygen nonstoichiometry of La0.6Sr0.4Co1-yFeyO3-delta (LSCF) mixed-conducting perovskite oxides strongly depends on the iron content: the cobalt-rich compounds (y = 0, 0.2, 0.4) were previously reported to show a sharp decrease in oxygen content with reducing atmosphere, while the oxygen vacancy concentration increased steadily for the iron-ric...

Effects of of the redox cycling on the volume expansion of Ni-YSZ cermets was investigated as a function of porosity and Ni/YSZ volume ratio by using a thermo-mechanical analysis (TMA). The first re-oxidation tests results obtained from TMA demonstrated that the amount of expansion was decreased and suppressed by lowering the Ni content of the anod...

The relationship between oxygen content and crystal structure of LaMnO3+δ, which is mother phase of cathode material for solid oxide fuel cells, has been investigated by X-ray diffraction, thermogravimetry and iodometric titration. It was confirmed that LaMnO3+δ with different oxygen content can be prepared by controlling sintering temperature in s...

In this study, a redox evaluation system for anode supported SOFCs using in-situ acoustic emission (AE) and electrochemical technique has been developed. The system consists of a gas blending unit, moisture controlling unit, AE cell evaluation probe, gas cooling exhaust, electrochemical cell test system and AE signal measurement system. The anode s...

In this study, we research the mechanical correlations among components of solid oxide fuel cell (SOFC) by analyzing the co-occurrence of acoustic emission (AE) events which are caused by damage. Then we propose a novel method for mining patterns from the numerical data such as AE. The proposed method extracts patterns of two clusters considering c...

In-situ micro Raman spectroscopy has been adopted as one of the most powerful analytical techniques with high spacial resolution under controlled atmospheres. In the present study, phase transformation of NiO doped yttria stabilized zirconia (YSZ) was monitored by in-situ micro-Raman spectroscopy. Raman spectra change caused by the phase transforma...

Ni-YSZ composites are widely used as SOFC anode materials for electrochemical devices. The mechanical properties of Ni-YSZ composites were investigated by using a Small Punch(SP) testing method under SOFC operating condition. The compositions of the Ni-YSZ composites tested in this study were 0:100 vol.%, 15:85 vol.%, 30:70 vol.%, and 50:50 vol.%....

In this study, NiO–Ce0.9Gd0.1O1.95 (NiO–GDC) nanocomposite powders, which were applied as anode materials of low temperature solid oxide fuel cells (SOFCs), were synthesized by hydroxide and oxalate reverse co-precipitation methods, respectively. The crystal phases, crystallite size, particle size, particle size distribution, and sintering characte...

Solid oxide fuel cell (SOFC) is an efficient generator and researched for practical use. However, one of the problems is the durability. In this study, we research the mechanical correlations among components of SOFC by analyzing the co-occurrence of acoustic emission (AE) events which are caused by damage. Then we proposed a novel method for minin...

Oxygen isotope diffusion coefficient, D*, of La0.6Sr 0.4Co0.2Fe0.8O3-δ (LSCF6428) was measured as a function of p(O2) and temperature. Vacancy diffusion coefficient, DV, was calculated from D* and reported values of oxygen nonstoichiometry, δ. There was little dependence of DV on δ or p(O2) while DV by conductivity relaxation method was reported to...

For the commercialization of solid oxide fuel cell (SOFC), in addition to the electrochemical reliability, it is also important to ensure the mechanical reliability of SOFC. Thus, the establishment of a suitable mechanical testing method under various temperatures and oxygen partial pressure conditions is a prerequisite for the development of relia...

The dependence of the structural phase transition behavior of Nd2NiO4+δ between the tetragonal and orthorhombic phases on the oxygen partial pressure, P(O2), has been investigated by differential scanning calorimetry, DSC, and thermogravimetry and differential thermal analysis, TG-DTA. The structural phase transition temperature, TP, decreased with...

The oxygen nonstoichiometry of La0.6Sr0.4FeO3−δ was measured at intermediate temperatures (773 to 1173K) between 1bar and the decomposition oxygen partial pressure by thermogravimetry and coulometric titration. The decomposition of the ABO3 perovskite phase was found to occur at low oxygen partial pressures (below 10−20bar). Using an atmosphere-con...

The electrical conductivities of SrZr0.9Y0.1O3-δ (SZY10) and BaCe0.95Y0.05O3-δ(BCY5) were measured as a function of hydrogen partial pressure P(H2), oxygen partial pressure P(O2), steam partial pressure P(H2O) and temperature. Their relaxation processes were analyzed using the solution of Fick's diffusion equation to determine the chemical diffusio...

The influence of uniaxial compressive strain/stress on the O2- ion conductivity of an yttria-stabilized zirconia (YSZ) sample was investigated by using electrochemical measurement. The conductivity was investigated by the AC four-probe method and molecular dynamics simulation. The applied compressive strain/stress ranged from 0 to 0.0003 (stress: 1...

The influence of uniaxial compressive strain/stress on the O²⁻ ion conductivity of an yttria-stabilized zirconia (YSZ) sample was investigated by using electrochemical measurement. The conductivity was investigated by the AC four-probe method and molecular dynamics simulation. The applied compressive strain/stress ranged from 0 to 0.0003 (stress: 1...

Effects of redox cycling on the mechanical properties of Ni-YSZ cermets were investigated by using an in-situ small punch (SP) testing method. The Ni contents in the Ni-YSZ cermets tested in this study were 0, 15, 30 and 50 vol.%. Electrical conductivity measurements suggested that Ni particles formed a network-like structure at Ni contents greater...

Deformation and mechanical damage measurement techniques were developed in order to investigate the degradation process of SOFC cell/stack and module under SOFC operation. In this study, the deformation and mechanical damage test was applied to simulated cell and stack. The deformation, microcrack and delamination in the cell and stack were detecte...

The electrical conductivity of La0.6Sr0.4Co1-yFeyO3-delta (y=0, 0.2, 0.4, 0.5, 0.6, 0.8, 1.0) were measured as a function of P(O-2) and temperature. The conductivity variation can be well explained only by change in electron-hole concentration due to oxygen nonstoichiometry regardless of temperature. Conductivity relaxation analyses were also condu...

The oxygen nonstoichiometry of La0.6Sr0.4Co1-yFeyO3-δ (LSCF) mixed-conducting perovskite-oxides can be classified into two groups: the cobalt-rich compounds (y=0, 0.2, 0.4) were previously reported to show a sharp decrease in oxygen content with reducing atmosphere, while the oxygen vacancy concentration increased more smoothly for the iron-rich co...

Young's modulus, shear modulus, Poisson's ratio and internal friction of La0.6Sr0.4CoO3-δ (LSC) and La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF6428) were evaluated in the temperature range between 298 to 1173 K, and the oxygen partial pressure, P(O2), range between 1 x 10-1 to 1 x 10-4 bar using the resonance method. The apparent Young's moduli of LSC and LSCF6...

Numerical simulations are performed to characterize the micro- and macro-scale aspects of the electro-chemo-mechanical coupling behavior of a positive-electrolyte-negative (PEN) structure under SOFC operation. The mathematical homogenization method is applied to evaluate the macroscopic material properties of porous electrodes by performing the cor...

The fuel cell is regarded as a highly efficient, low-pollution power generation system. In particular, Solid Oxide Fuel Cell (SOFC) has a high generation efficiency. However, a crucial issue in putting SOFC to practical use is the establishment of a technique for evaluating the deterioration. We previously developed a technique by which to measure...

Rutile-type Ti0.93Nb0.07O2 was characterized and evaluated as a potential interconnect material for low temperature solid oxide fuel cells. It was revealed that Ti 0.93Nb0.07O2 shows the conductivity of ca. 50 S/cm in reducing atmospheres over a wide temperature range of 400 ∼ 1000 °C. Also, the effect of Cr-doping on conductivity and the segregati...

Although sudden changes of the event phase in complex system may indicate underlying essential forces, such events are not frequent. In the present paper, we propose an essential event extractor (E3) scheme to extract relatively rare but co-occurring event sequences in event phase transitions. In E3, the self-organizing map (SOM) is used as vector...

Change in the lattice parameters of La0.6Sr0.4Co1 − yFeyO3 − δ (y = 0.2, 0.4, 0.6 and 0.8) was observed by in-situ XRD under the various temperature and oxygen partial pressure conditions for thermo-chemical expansivity study. By combination of the lattice parameters and oxygen non-stoichiometry, the linear thermal expansion rates were formulated i...

The electrical conductivity of a pseudoternary system, consisting of LaFeO3-SrFeO3-delta-SrZrO3, {La0.05(1-x)Sr0.95+ 0.05x} (Zr0.95Fe0.05)O3-delta (x = 0-0.5), was evaluated both in oxygen and hydrogen containing environments by a two-probe ac technique. Correlations of oxygen partial pressure, water vapor pressure, and composition dependences of t...

Stabilized zirconia (ZrO 2 ) is recognized as the major candidate for the electrolyte material of solid oxide fuel cells (SOFCs) owing to its high ionic conductivity and chemical stability. The ionic conductivity originates from the oxygen vacancies introduced by doping 2+ or 3+ valence cations on the Zr ⁴⁺ site. The conductivity shows the maximum...

The oxygen nonstoichiometry of La0.6Sr0.4Co1-yFeyO3-δ (y = 0.2, 0.4, 0.6, 0.8) was measured by high temperature gravimetry and coulometric titration. The results of the oxygen nonstoichiometry measurements could be categorized into Co rich compounds (y = 0.2, 0.4) and Fe rich compounds (y = 0.6, 0.8). The Co rich compounds decomposed into A2BO4 and...

In order to make clear the relationship between the microstructure of the porous oxide layer and electrochemical properties of air electrodes of solid oxide fuel cells, air/porous oxide/yttria stabilized zirconia, complex-impedance and cathodic polarization were measured on the air/La0.6Ca0.4MnO3/YSZ electrodes at 900-1000°C with the porous La0.6Ca...

The present work developed a basis to explore numerous damage events utilizing Self-Organizing Map (SOM) introducing Kullback-Leibler (KL) divergence as an appropriate similarity for frequency spectra of damage events. Firstly, we validated the use of KL divergence to frequency spectra of damage events. The experiment using the datasets of damage r...

Fluorescence yield (FY) X-ray absorption spectroscopic experiments with a grazing- exit geometry for detection of emitted fluorescence were carried out. The observed XAFS spectra provide the information about depth-resolved chemical state in the surface layer of film materials through the take-off angle dependence of the escape depth of the fluores...

The defect chemical relationship in Nd doped BaCeO3 was discussed based on the defect concentration determined by thermogravimetry and electrical conductivity measured by D.C. 4-terminal method as a function of oxygen partial pressure, P(O2), water vapor partial pressure, P(H2O), and temperature. In BaCe0.9Nd0.1O3−δ, the defect concentration strong...

In the present paper, we investigated the electrical performance of anode-supported solid oxide fuel cells (SOFCs) composed of Gd0.1Ce0.9O1.95 (GDC) electrolyte films of 1–75μm in thickness prepared by simple and cost-effective methods (dry co-pressing process and spray dry co-pressing process), and discussed the effect of thickness of the GDC elec...

The influence of chemically induced expansion on the fracture damage of a nonstoichiometric oxide (ceria) based solid oxide fuel cell (SOFC) single cell laminate was investigated by using numerical stress analyses under oxidizing/reducing gradient condition. The single cell examined in this study was composed of electrolyte (Ce0.8Sm0.2O2−δ), anode...

In this study, NiO–Ce0.9Gd0.1O1.95 (NiO–GDC) nanocomposite powders were synthesized by hydroxide co-precipitation method, and applied to improve the microstructure of solid oxide fuel cell (SOFC) anodes. The NiO–GDC anodes prepared from the NiO–GDC nanocomposite powders showed uniform microstructure with uniform distribution of NiO and GDC phases....

The electrical conductivity of SrZr0.99Fe0.01O3−δ was evaluated by a four-probe ac technique. The measurements were conducted in hydrogen and in oxygen containing atmospheres at 823≤T/K≤1273. It was found from the X-ray absorption spectroscopic measurements that Fe in the oxide is trivalent both in hydrogen and in oxygen. In order to determine the...

To elucidate the electronic state and the conduction mechanism of Nd2NiO4+δ series oxides at high temperatures, the electrical conductivity, Seebeck coefficient, and nonstoichiometric oxygen content of Nd2−xSrxNiO4+δ (x=0, 0.2, 0.4) were measured as a function of the Sr content, temperature, and oxygen partial pressure. The hole mobility is estimat...

High temperature X-ray diffraction measurements were carried out on K2NiF4-type Nd2−xSrxNiO4+δ (x=0, 0.2, 0.4) in N2–O2 atmosphere at 873–1173K. Diffraction patterns of Nd2−xSrxNiO4+δ were indexed by a tetragonal symmetry except for that of Nd2NiO4+δ measured at 873K in 1bar O2. Tetragonal-orthorhombic phase transition was observed in Nd2NiO4+δ. Th...

High temperature X-ray diffraction measurements were made on oxygen nonstoichiometric La2 − xSrxNiO4 + δ in N2–O2 atmosphere at 873–1173 K. Crystal structure of La2−xSrxNiO4 + δ at high temperatures was analyzed using the tetragonal symmetry, I4/mmm. As the amount of excess oxygen increases, the lattice parameter perpendicular to the perovskite and...

Fuel cell is regarded as a highly efficient power generation system as well as low-pollution. In particular, SOFC (Solid Oxide Fuel Cell) has high generation efficiency. However, a crucial issue in putting SOFC into practical use is the establishment of a technique for evaluating the deterioration. We have previously developed a technique to measur...

For the evaluation of electrode reaction at H2–H2O(g), Pt/BaCe0.95Y0.05O3−δ, the electrode impedance and steady-state polarization measurements were examined as the functions of hydrogen partial pressure, PH2, steam partial pressure, PH20 and hydrogen activity on the electrolyte surface at triple phase boundary (TPB), aH, using three-terminal metho...

Acoustic Emission (AE) technique is employed to detect degradation events inside of lithium-ion batteries. A commercial 18650 type battery and a model half cell (Li/organic electrolyte /LiCoO2) are monitored with AE technique during charge and discharge cycles. In the commercial battery, AE events are detected during every discharge process at SOC...

For the commercialization of solid oxide fuel cell (SOFC), in addition to the electrical reliability, it is also important to ensure the mechanical reliability of SOFC. Thus, the establishment of a suitable mechanical testing method under various temperatures and oxygen partial pressure conditions is a prerequisite for the development of reliable S...

Oxygen nonstoichiometry and thermo-chemical stability of the perovskite mixed-conductors La0.6Sr0.4FeO3-δ and La0.6Sr0.4CoO3-δ were investigated by coulometric titration and high-temperature gravimetry in the oxygen partial pressure range of log(pO2/bar)=-28 to 0 at 773 to 1173 K. For both materials, the oxygen content decreased with decreasing oxy...

High temperature X-ray diffraction measurements High temperature X-ray diffraction measurements were carried out on K 2 NiF 4-type Nd 2 − x Sr x NiO 4 + δ (x = 0, 0.2, 0.4) in N 2-O 2 atmosphere at 873-1173 K. Diffraction patterns of Nd 2 − x Sr x NiO 4 + δ were indexed by a tetragonal symmetry except for that of Nd 2 NiO 4 + δ measured at 873 K in...

To elucidate the electronic state and the conduction mechanism of Nd 2 NiO 4+ı series oxides at high temperatures, the electrical conductivity, Seebeck coefficient, and nonstoichiometric oxygen content of Nd 2−x Sr x NiO 4+ı (x = 0, 0.2, 0.4) were measured as a function of the Sr content, temperature, and oxygen partial pressure. The hole mobility...

Solid Oxide Fuel Cell, which has high efficiency of electric power generation, is one of the key technologies for us to reach to the low carbon society. Over 30 years' basic research of SOFC leads it just to launch to practical use in the real world, whereas the accumulation of huge amount of research data, especially material data, urges to be res...

In order to elucidate how oxygen content changes in Nd2−xSrxNiO4+δ (x=0, 0.2, 0.4), defect chemical and statistical thermodynamic analyses were carried out. The relationship among δ, P(O2), and T were analyzed by a defect equilibrium model. Since Nd2−xSrxNiO4+δ shows metal like band conduction at high temperatures, chemical potential of hole is exp...

A series of doped LaGaO3 perovskite type oxides is considered as the electrolyte of solid oxide fuel cells (SOFCs), due to their high oxide ionic conductivity. However, detailed defect chemistry, particularly the relationship between oxygen nonstoichiometry and lattice parameter under operating condition of SOFCs has not been understood well so far...

Strontium titanate, SrTiO3 has a cubic perovskite-type structure in the wide range of the temperature and is chemically stable from oxidizing to reducing atmospheres. Moreover donor-doped-SrTiO3 oxides have high electric conductivity. In this study, the examination was made on the possibilities of the application of polycrystalline of SrTi1-yNbyO3...

Mechanical damages and their formation mechanisms in SOFC were investigated. Generalized schemes of the occurrence of mechanical failures were summarized, and among them, common features in various cell designs were extracted. They were discussed in three categories of (a) deformation of a cell due to its asymmetry, (b) propagation of mechanical de...

In this paper, we discuss the effects of different oxygen partial pressures on the elastic modulus and fracture strength of 8 mol% yittria stabilized zirconia (8YSZ) and 10 mol% gadolinia doped ceria (10GDC). The specimens of 8YSZ and 10GDC prepared by a sintering process were treated at 800 åC under different oxygen partial pressures in the range...

Oxygen nonstoichiometry of La0.6Sr0.4Co1-yFeyO3-δ (y=0.2, 0.8) were measured by high temperature gravimetry and coulometric titration as a function of temperature and oxygen partial pressure. The lattice constant is also observed by HT-XRD as a function of temperature and oxygen partial pressure. The relationship between lattice constant and oxygen...

Crystal structure and mechanical properties of La2NiO4+d were measured by high temperature X-ray diffractometry and in-situ small punch test as a function of temperature and oxygen partial pressure. As P(O2) increases, the lattice parameter perpendicular to the perovskite layer increases and that parallel to the layer slightly decreases, and the la...