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Sintering behaviour of the protonic conductors BaZr(x)Ce(0.8-x)Ln(0.2)O(3-delta) (x=0.8, 0.5, 0.1; Ln=Y, Sm, Gd, Dy) during the solid-state reactive-sintering process
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Process Metallurgy.ORCID iD: 0000-0001-5258-099X
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Process Metallurgy.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Process Metallurgy. Shanghai Institute of Technology, China .ORCID iD: 0000-0003-3060-9987
2015 (English)In: Ceramics International, ISSN 0272-8842, E-ISSN 1873-3956, Vol. 41, no 2, 2558-2564 p.Article in journal (Refereed) Published
Abstract [en]

The protonic conductors BaZr(x)Ce(0.8-x)Ln(0.2)O(3-delta) (x=0.8, 0.5, 0.1; Ln=Y, Sm, Gd, Dy) were successfully prepared using a solid-state reactive-sintering method. NiO (1 wt.%) was added as a sintering aid, and it was proven that NiO produced tremendous enhancement in the densification process. The morphologies of the variously doped BaZr(0.8)Ln(0.2)O(3-delta), BaZr(0.5)Ce(0.3)Ln(0.2)O(3-delta) and BaZr(0.1)Ce(0.7)Ln(0.2)O(3-delta) ceramics, as well as their sintering behaviour, were investigated. The results show that the Ce content in the BaZr(0.8)Ln(0.2)O(3-delta), BaZr(0.5)Ce(0.3)Ln(0.2)O(3-delta) and BaZr(0.1)Ce(0.7)Ln(0.2)O(3-delta) compounds influences the sintering temperature significantly, and a larger Ce content will lead to a lower sintering temperature. In addition, ionic radii of the dopants that are similar to the ionic radii of the B-site will also result in a lowered sintering temperature. Based on the present study, NiO has no influence on the lattice parameters.

Place, publisher, year, edition, pages
2015. Vol. 41, no 2, 2558-2564 p.
Keyword [en]
Solid state reaction, Milling, Sintering, Fuel cells
National Category
Materials Engineering
URN: urn:nbn:se:kth:diva-161094DOI: 10.1016/j.ceramint.2014.10.177ISI: 000348961400080ScopusID: 2-s2.0-84919443842OAI: diva2:797619

QC 20150324

Available from: 2015-03-24 Created: 2015-03-09 Last updated: 2015-04-23Bibliographically approved
In thesis
1. Advanced BaZrO3-BaCeO3 Based Proton Conductors Used for Intermediate Temperature Solid Oxide Fuel Cells (ITSOFCs)
Open this publication in new window or tab >>Advanced BaZrO3-BaCeO3 Based Proton Conductors Used for Intermediate Temperature Solid Oxide Fuel Cells (ITSOFCs)
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In this thesis, the focus is on studying BaZrO3-BaCeO3 based proton conductors due to that they represent very promising proton conductors to be used for Intermediate Temperature Solid Oxide Fuel Cells (ITSOFCs). Here, dense BaZr0.5Ce0.3Y0.2O3-δ (BZCY532) ceramics were selected as the major studied materials. These ceramics were prepared by different sintering methods and doping strategies. Based on achieved results, the thesis work can simply be divided into the following parts:

1) An improved synthesis method, which included a water-based milling procedure followed by a freeze-drying post-processing, was presented. A lowered calcination and sintering temperature for a Hf0.7Y0.3O2-δ (YSH) compound was achieved. The value of the relative density in this work was higher than previously reported data. It is also concluded that this improved method can be used for mass-production of ceramics.

2) As the solid-state reactive sintering (SSRS) represent a cost-effective sintering method, the sintering behaviors of proton conductors BaZrxCe0.8-xLn0.2O3-δ (x = 0.8, 0.5, 0.1; Ln = Y, Sm, Gd, Dy) during the SSRS process were investigated. According to the obtained results, it was found that the sintering temperature will decrease, when the Ce content increases from 0 (BZCLn802) to 0.3 (BZCLn532) and 0.7 (BZCLn172). Moreover, the radii of the dopant ions similar to the radii of Zr4+ or Ce4+ ions show a better sinterability. This means that it is possible to obtain dense ceramics at a lower temperature. Moreover, the conductivities of dense BZCLn532 ceramics were determined. The conductivity data indicate that dense BZCY532 ceramics are good candidates as either oxygen ion conductors or proton conductors used for ITSOFCs.

3) The effect of NiO on the sintering behaviors, morphologies and conductivities of BZCY532 based electrolytes were systematically investigated. According to the achieved results, it can be concluded that the dense BZCY532B ceramics (NiO was added during ball-milling before a powder mixture calcination) show an enhanced oxygen and proton conductivity. Also, that BZCY532A (NiO was added after a powder mixture calcination) and BZCY532N (No NiO was added in the whole preparation procedures) showed lower values. In addition, dense BZCY532B and BZCY532N ceramics showed only small electronic conductivities, when the testing temperature was lower than 800 ℃. However, the BZCY532A ceramics revealed an obvious electronic conduction, when they were tested in the range of 600 ℃ to 800 ℃. Therefore, it is preferable to add the NiO powder during the BZCY532 powder preparation, which can lower the sintering temperature and also increase the conductivity.

4) Dense BZCY532 ceramics were successfully prepared by using the Spark Plasma Sintering (SPS) method at a temperature of 1350 ℃ with a holding time of 5 min. It was found that a lower sintering temperature (< 1400 ℃) and a very fast cooling rate (> 200 ℃/min) are two key parameters to prepare dense BZCY532 ceramics. These results confirm that the SPS technique represents a feasible and cost-effective sintering method to prepare dense Ce-containing BaZrO3-BaCeO3 based proton conductors.

5) Finally, a preliminary study for preparation of Ce0.8Sm0.2O2-δ (SDC) and BZCY532 basedcomposite electrolytes was carried out. The novel SDC-BZCY532 based composite electrolytes were prepared by using the powder mixing and co-sintering method. The sintering behaviors, morphologies and ionic conductivities of the composite electrolytes were investigated. The obtained results show that the composite electrolyte with a composition of 60SDC-40BZCY532 has the highest conductivity. In contrast, the composite electrolyte with a composition of 40SDC-60BZCY532 shows the lowest conductivity.

In summary, the results show that BaZrO3-BaCeO3 based proton-conducting ceramic materials represent very promising materials for future ITSOFCs electrolyte applications.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. x, 66 p.
Solid oxide fuel cells (SOFCs); Intermediate temperature solid oxide fuel cells (ITSOFCs); Electrolyte; Electrochemical impedance spectroscopy (EIS); Barium zirconate (BaZrO3); Barium cerate (BaCeO3); Solid-state reaction (SSR); Sintering; Conventional sintering (CS); Solid-state reactive sintering (SSRS); Spark plasma sintering (SPS); Ionic conductivity; Oxygen ion conductivity; Proton conductivity; Electronic conductivity; Oxygen ion conductor; Proton conductor; Oxygen partial pressure (OPP); Composite electrolyte
National Category
Research subject
Materials Science and Engineering
urn:nbn:se:kth:diva-165073 (URN)978-91-7595-517-9 (ISBN)
Public defence
2015-05-20, B2, Brinellvägen 23, KTH, Stockholm, 10:00 (English)

QC 20150423

Available from: 2015-04-23 Created: 2015-04-22 Last updated: 2015-06-01Bibliographically approved

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