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Title: New Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells

Abstract

Operation of SOFCs at intermediate temperatures (500-800 C) requires new combinations of electrolyte and electrode materials that will provide both rapid ion transport across the electrolyte and electrode-electrolyte interfaces and efficient electrocatalysis of the oxygen reduction and fuel oxidation reactions. This project concentrates on materials and issues associated with cathode performance that are known to become limiting factors as the operating temperature is reduced. The specific objectives of the proposed research are to develop cathode materials that meet the electrode performance targets of 1.0 W/cm{sup 2} at 0.7 V in combination with YSZ at 700 C and with GDC, LSGM or bismuth oxide based electrolytes at 600 C. The performance targets imply an area specific resistance of {approx}0.5 {Omega}cm{sup 2} for the total cell. The research strategy is to investigate both established classes of materials and new candidates as cathodes, to determine fundamental performance parameters such as bulk diffusion, surface reactivity and interfacial transfer, and to couple these parameters to performance in single cell tests. The initial choices for study were perovskite oxides based on substituted LaFeO{sub 3} (P1 compositions), where significant data in single cell tests exist at PNNL for example, for La{sub 0.8}Sr{sub 0.2}FeO{sub 3} cathodes on bothmore » YSZ and CSO/YSZ. The materials selection was then extended to La{sub 2}NiO{sub 4} compositions (K1 compositions), and then in a longer range task we evaluated the possibility of completely unexplored group of materials that are also perovskite related, the ABM{sub 2}O{sub 5+{delta}}. A key component of the research strategy was to evaluate for each cathode material composition, the key performance parameters, including ionic and electronic conductivity, surface exchange rates, stability with respect to the specific electrolyte choice, and thermal expansion coefficients. In the initial phase, we did this in parallel with the perovskite compositions that were being investigated at PNNL, in order to assess the relative importance of the intrinsic properties such as oxygen ion diffusion and surface exchange rates as predictors of performance in cell tests. We then used these measurements to select new materials for scaled up synthesis and performance evaluation in single cell tests. The results of the single cell tests than provided feedback to the materials synthesis and selection steps. In this summary, the following studies are reported: (1) Synthesis, characterization, and DC conductivity measurements of the P1 compositions La{sub 0.8}Sr{sub 0.2}FeO{sub 3-x} and La{sub 0.7}Sr{sub 0.3}FeO{sub 3-x} were completed. A combinational approach for preparing a range P1 (La,Sr)FeO{sub 3} compositions as thin films was investigated. Synthesis and heat treatment of amorphous SrFeO{sub 3-x} and LaFeO{sub 3-x} films prepared by pulsed laser deposition are described. (2) Oxygen transport properties of K1 compositions La{sub x}Pr{sub 2-x}NiO{sub 4+d} (x =2.0, 1.9, 1.2, 1.0 and 0) measured by electrical conductivity relaxation are presented in this report. Area specific resistances determined by ac impedance measurements for La{sub 2}NiO{sub 4+{delta}} and Pr{sub 2}NiO{sub 4+{delta}} on CGO are encouraging and suggest that further optimization of the electrode microstructure will enable the target to be reached. (3) The oxygen exchange kinetics of the oxygen deficient double perovskite LnBaCo{sub 2}O{sub 5.5+{delta}} (Ln=Pr and Nd) were determined by electrical conductivity relaxation. The high electronic conductivity and rapid diffusion and surface exchange kinetics of PBCO suggest its application as cathode material in intermediate temperature solid oxide fuel cells. The first complete cell measurements were performed on Ni/CGO/CGO/PBCO/CGO cells. (4) The oxygen exchange kinetics of highly epitaxial thin films of PrBaCo{sub 2}O{sub 5.5+{delta}} (PBCO) has been determined by electrical conductivity relaxation and isotope exchange and depth profiling and confirm the high electronic conductivity and rapid surface exchange kinetics. (5) The phase compatibility of La{sub 2}NiO{sub 4}, Pr{sub 2}NiO{sub 4} and PrBaCo{sub 2}O{sub 5.5+x} with YSZ and GDC electrolytes was investigated by solid state reaction and powder X-ray diffraction. PBCO is found to be compatible with CGO.« less

Authors:
Publication Date:
Research Org.:
University Of Houston
Sponsoring Org.:
USDOE
OSTI Identifier:
901629
DOE Contract Number:  
FC26-03NT41960
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; BISMUTH OXIDES; CATHODES; ELECTRIC CONDUCTIVITY; FOREIGN EXCHANGE RATE; HEAT TREATMENTS; ISOTOPIC EXCHANGE; OXIDES; OXYGEN IONS; PEROVSKITE; SOLID OXIDE FUEL CELLS; THERMAL EXPANSION; THIN FILMS; X-RAY DIFFRACTION

Citation Formats

Allan J. Jacobson. New Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells. United States: N. p., 2006. Web. doi:10.2172/901629.
Allan J. Jacobson. New Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells. United States. doi:10.2172/901629.
Allan J. Jacobson. Sat . "New Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells". United States. doi:10.2172/901629. https://www.osti.gov/servlets/purl/901629.
@article{osti_901629,
title = {New Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells},
author = {Allan J. Jacobson},
abstractNote = {Operation of SOFCs at intermediate temperatures (500-800 C) requires new combinations of electrolyte and electrode materials that will provide both rapid ion transport across the electrolyte and electrode-electrolyte interfaces and efficient electrocatalysis of the oxygen reduction and fuel oxidation reactions. This project concentrates on materials and issues associated with cathode performance that are known to become limiting factors as the operating temperature is reduced. The specific objectives of the proposed research are to develop cathode materials that meet the electrode performance targets of 1.0 W/cm{sup 2} at 0.7 V in combination with YSZ at 700 C and with GDC, LSGM or bismuth oxide based electrolytes at 600 C. The performance targets imply an area specific resistance of {approx}0.5 {Omega}cm{sup 2} for the total cell. The research strategy is to investigate both established classes of materials and new candidates as cathodes, to determine fundamental performance parameters such as bulk diffusion, surface reactivity and interfacial transfer, and to couple these parameters to performance in single cell tests. The initial choices for study were perovskite oxides based on substituted LaFeO{sub 3} (P1 compositions), where significant data in single cell tests exist at PNNL for example, for La{sub 0.8}Sr{sub 0.2}FeO{sub 3} cathodes on both YSZ and CSO/YSZ. The materials selection was then extended to La{sub 2}NiO{sub 4} compositions (K1 compositions), and then in a longer range task we evaluated the possibility of completely unexplored group of materials that are also perovskite related, the ABM{sub 2}O{sub 5+{delta}}. A key component of the research strategy was to evaluate for each cathode material composition, the key performance parameters, including ionic and electronic conductivity, surface exchange rates, stability with respect to the specific electrolyte choice, and thermal expansion coefficients. In the initial phase, we did this in parallel with the perovskite compositions that were being investigated at PNNL, in order to assess the relative importance of the intrinsic properties such as oxygen ion diffusion and surface exchange rates as predictors of performance in cell tests. We then used these measurements to select new materials for scaled up synthesis and performance evaluation in single cell tests. The results of the single cell tests than provided feedback to the materials synthesis and selection steps. In this summary, the following studies are reported: (1) Synthesis, characterization, and DC conductivity measurements of the P1 compositions La{sub 0.8}Sr{sub 0.2}FeO{sub 3-x} and La{sub 0.7}Sr{sub 0.3}FeO{sub 3-x} were completed. A combinational approach for preparing a range P1 (La,Sr)FeO{sub 3} compositions as thin films was investigated. Synthesis and heat treatment of amorphous SrFeO{sub 3-x} and LaFeO{sub 3-x} films prepared by pulsed laser deposition are described. (2) Oxygen transport properties of K1 compositions La{sub x}Pr{sub 2-x}NiO{sub 4+d} (x =2.0, 1.9, 1.2, 1.0 and 0) measured by electrical conductivity relaxation are presented in this report. Area specific resistances determined by ac impedance measurements for La{sub 2}NiO{sub 4+{delta}} and Pr{sub 2}NiO{sub 4+{delta}} on CGO are encouraging and suggest that further optimization of the electrode microstructure will enable the target to be reached. (3) The oxygen exchange kinetics of the oxygen deficient double perovskite LnBaCo{sub 2}O{sub 5.5+{delta}} (Ln=Pr and Nd) were determined by electrical conductivity relaxation. The high electronic conductivity and rapid diffusion and surface exchange kinetics of PBCO suggest its application as cathode material in intermediate temperature solid oxide fuel cells. The first complete cell measurements were performed on Ni/CGO/CGO/PBCO/CGO cells. (4) The oxygen exchange kinetics of highly epitaxial thin films of PrBaCo{sub 2}O{sub 5.5+{delta}} (PBCO) has been determined by electrical conductivity relaxation and isotope exchange and depth profiling and confirm the high electronic conductivity and rapid surface exchange kinetics. (5) The phase compatibility of La{sub 2}NiO{sub 4}, Pr{sub 2}NiO{sub 4} and PrBaCo{sub 2}O{sub 5.5+x} with YSZ and GDC electrolytes was investigated by solid state reaction and powder X-ray diffraction. PBCO is found to be compatible with CGO.},
doi = {10.2172/901629},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2006},
month = {9}
}