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LIU Kun, LI Chenglong, ZHANG Lei, et al. Study on co-sintering characteristics of metal supported solid oxide fuel cells[J]. Acta Materiae Compositae Sinica.
Citation: LIU Kun, LI Chenglong, ZHANG Lei, et al. Study on co-sintering characteristics of metal supported solid oxide fuel cells[J]. Acta Materiae Compositae Sinica.
shu

Study on co-sintering characteristics of metal supported solid oxide fuel cells

  • 1.

    School of Mechanical and Electrical Engineering, Zhengzhou University of Light Industry, Zhengzhou 450002, China

  • 2.

    School of Materials Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, China

  • 3.

    School of Mechanical Engineering, University of Toronto, Toronto M5 S2 E8

  • 4.

    School of Materials Science and Engineering, Xi'an Jiaotong University, Xi'an 710049, China

Funds: National Natural Science Foundation joint fund project (No. U2004169); Henan Province science and technology research project (No. 242102230036); Major science and technology project of Henan Province in 2024 (No. 241100220100)
More Information
  • Received Date: August 07, 2024
  • Revised Date: September 11, 2024
  • Accepted Date: September 30, 2024
  • Available Online: October 21, 2024
    Abstract
  • The sintering mechanism of electrode layer and electrolyte layer was analyzed considering the whole thermal expansion of the battery and the creep of the ceramic. The evolution of the microstructure of the electrode and electrolyte layer and the distribution and change of residual stress of the metal supported solid oxide fuel cell (MS-SOFC) under different sintering temperature and grain size were expounded. The Skorohod-Olevsky Viscous Sintering (SOVS) model was established to simulate the relative density and stress distribution and evolution of different layers and different surfaces of MS-SOFC under different sintering temperatures and different grain sizes. The change of microstructure morphology of dissimilar grain size structure after sintering was revealed by high temperature sintering experiment. The results show that the relative density of electrolyte and electrode, the residual stress value of each layer and the mutation amplitude are affected by sintering temperature. When the initial grain size of each layer of fuel cell material is small, the densification rate caused by sintering is very obvious. With the gradual increase of grain size, the densification rate is relatively small, and the residual stress value and mutation amplitude of each layer of the battery are gradually reduced. Nano-yttrium oxide stabilized zirconia (YSZ) electrolyte layer is easier to sintering, and the micro-defects are reduced more than the micron YSZ electrolyte layer after sintering. After sintering of MS-SOFC, the radial stress of cathode and anode is tensile stress, and the radial stress of electrolyte is compressive stress. Axial stress and shear stress vary periodically between tensile and compressive stress. The electrode layer with micron crystals can maintain large porosity after sintering, while the electrolyte with nanocrystalline can improve the conductivity and reduce the densification sintering temperature. When the crystal size is nanometer, the residual stress value and distribution are sensitive to the sintering temperature.
    • Summary

  • Summary

    Objective 

    Metal-supported solid oxide fuel cell (MS-SOFC) is a novel structure that differs from traditional electrode or electrolyte supports in solid oxide fuel cells (SOFCs). With the advancement of low temperature and cost-effective SOFC technology, the advantages of MS-SOFC become more prominent. Currently, research on MS-SOFC primarily focuses on developing suitable metal matrix materials, new electrolyte and electrode materials, optimizing single battery preparation processes; however, little attention has been given to sintering technology for simple SOFC preparation. This study analyzes the sintering mechanism of the electrode and electrolyte layers by considering overall thermal expansion of the battery and ceramic creep. It elucidates the evolution of microstructure in both layers as well as distribution and alteration of residual stress in metal-supported solid oxide fuel cells (MS-SOFCs) at different sintering temperatures and grain sizes."

    Methods 

    A single MS-SOFC finite element model was established, and the influences of sintering temperature and grain size on the relative density and residual stress between layers of MS-SOFC were investigated using ABAQUS simulation software with its creep subroutine. Additionally, co-sintering of YSZ electrolyte prepared by supersonic plasma spraying was performed. Firstly, the changes in relative density under different sintering temperatures and grain sizes were studied. Secondly, the distribution and variation of residual stress at different sintering temperatures and crystal sizes were analyzed.

    Results 

    The relative density of the cathode, anode, and electrolyte layers gradually increases with the increase in sintering temperature, indicating that increasing the sintering temperature promotes material densification within a certain range. Generally, each layer initially experiences a decrease followed by an increase in relative density. The inflection point for densification initiation varies for different sintering temperatures due to the higher heating rate associated with higher holding temperatures when heating time and holding time are kept constant. Although the initial relative density of the anode layer is equal to that of the cathode layer, the anode layer exhibits a higher densification rate at the same sintering temperature. This difference can be attributed to variations in activation energy Q for viscous flow. Under identical heating rates and sintering temperatures, both electrode and electrolyte densification rates decrease as initial grain size increases while they increase as initial grain size decreases. These observations highlight significant influences of grain size on both densification rate and overall densification of the sintered body. The results demonstrate that after sintering, cracks in submicron YSZ electrolyte layers gradually close while pores diminish over time. Similarly, pores formed by unmelted particles in nano-YSZ electrolyte layers also reduce significantly resulting in a dense structure formation. Co-sintering at 1250 ℃ leads to submicron YSZ and nano-YSZ fractures forming dense columnar crystal structures which differ from their original coating fracture morphology (a mixture of columnar, equiaxial, and unfused particles). During a 2-hour sintering period, porosity decreases from 3.3% to 2.4% for submicron YSZ electrolyte layers and from 2.3% to 1.5% for nano-YSZ electrolyte layers respectively while content of unmelted particles reduces from 8.8% to 6.1%. Conclusions: The relative density increases with increasing sintering temperature but decreases with increasing grain size. Nanoscale grains exhibit faster densification rates compared to submicron and micron grains. The nano-electrolyte layer is easier to sinter compared to submicron and micron electrolyte layers due to the presence of both pores and unmelted particles in it; moreover, the change in pore volume during the sintering process is much larger for unmelted particles than for pores alone. Residual stress levels and sudden change amplitudes increase with increasing sintering temperature but decrease with increasing crystal size. Sintering stress in nanocrystalline SOFCs is more sensitive to variations in sintering temperature compared to submicron or micron grains. Furthermore, submicron and micron grains can inhibit warping deformation at MS-SOFC edges as well as reduce the influence of metal matrix on stress concentration within electrode layers and electrolyte layers.

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    • References (62)
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