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A comparative study of the Ruddlesden-Popper series,Lan+1NinO3n+1 (n = 1, 2 and 3), for solid-oxide fuel-cell cathode applications
Institution:1. Defence Research and Development Canada-Atlantic, Ottawa, Ontario, Canada;2. Institute for Chemical Process and Environmental Technology, National Research, Council Canada, Ottawa, Ontario, Canada;3. Department of Materials, Imperial College London, Prince Consort Road, London, SW7, 2BP, UK;1. Energy Storage Research Center, Research Institute of Industrial Science and Technology, Pohang 790-330, Republic of Korea;2. School of Materials Science & Engineering, Yeungnam University, Gyeongsan 712-749, Republic of Korea;1. CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, No. 96 Jinzhai Road, Hefei, Anhui Province, 230026, PR China;2. Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China;3. Hefei National Laboratory of Physical Science at the Microscale, University of Science and Technology of China, Hefei, 230026 Anhui, China;4. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China;1. Graduate School of Science and Technology, Kumamoto University, 2-39-1 Kurokami, Kumamoto 860-8555, Japan;2. Fine Particles Engineering Group, Materials Processing Unit, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan;1. Graduate School of Science and Technology, Kumamoto University, 2-39-1 Kurokami, Kumamoto 860-8555, Japan;2. Fine Particles Engineering Group, Materials Processing Unit, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan
Abstract:A comparative investigation of the much-studied La2NiO4+δ (n = 1) phase and the higher-order Ruddlesden-Popper phases, Lan+1NinO3n+1 (n = 2 and 3), has been undertaken to determine their suitability as cathodes for intermediate-temperature solid-oxide fuel cells. As n is increased, a structural phase transition is observed from tetragonal I4/mmm in the hyperstoichiometric La2NiO4.15 (n = 1) to orthorhombic Fmmm in the oxygen-deficient phases, La3Ni2O6.95 (n = 2) and La4Ni3O9.78 (n = 3). High temperature d.c. electrical conductivity measurements reveal a dramatic increase in overall values from n = 1, 2 to 3 with metallic behavior observed for La4Ni3O9.78. Impedance spectroscopy measurements on symmetrical cells with La0.9Sr0.10Ga0.80Mg0.20O3−δ (LSGM-9182) as the electrolyte show a systematic improvement in the electrode performance from La2NiO4.15 to La4Ni3O9.78 with ∼ 1 Ω cm2 observed at 1073 K for the latter. Long-term thermal stability tests show no impurity formation when La3Ni2O6.95 and La4Ni3O9.78 are heated at 1123 K for 2 weeks in air, in contrast to previously reported data for La2NiO4.15. The relative thermal expansion coefficients of La3Ni2O6.95 and La4Ni3O9.78 were found to be similar at ∼ 13.2 × 10 6 K 1 from 348 K to 1173 K in air compared to 13.8 × 10 6 K 1 for La2NiO4.15. Taken together, these observations suggest favourable use for the n = 2 and 3 phases as cathodes in intermediate-temperature solid-oxide fuel cells when compared to the much-studied La2NiO4+δ (n = 1) phase.
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