EP4602017A1 - Gegen isotherme hochtemperaturabbau beständige festoxidzelle - Google Patents

Gegen isotherme hochtemperaturabbau beständige festoxidzelle

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Publication number
EP4602017A1
EP4602017A1 EP23789965.3A EP23789965A EP4602017A1 EP 4602017 A1 EP4602017 A1 EP 4602017A1 EP 23789965 A EP23789965 A EP 23789965A EP 4602017 A1 EP4602017 A1 EP 4602017A1
Authority
EP
European Patent Office
Prior art keywords
solid oxide
oxide cell
mol
structural component
cell
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
EP23789965.3A
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English (en)
French (fr)
Inventor
Peyman KHAJAVI
Henrik Lund Frandsen
Peter Vang Hendriksen
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Danmarks Tekniske Universitet
Original Assignee
Danmarks Tekniske Universitet
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Filing date
Publication date
Application filed by Danmarks Tekniske Universitet filed Critical Danmarks Tekniske Universitet
Publication of EP4602017A1 publication Critical patent/EP4602017A1/de
Pending legal-status Critical Current

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    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/48—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zirconium or hafnium oxides, zirconates, zircon or hafnates
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    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/48—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zirconium or hafnium oxides, zirconates, zircon or hafnates
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    • C04B38/0074—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof characterised by the pore distribution, e.g. inhomogeneous distribution of pores expressed as porosity percentage
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    • H01M4/00—Electrodes
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    • H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
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    • H01M4/90—Selection of catalytic material
    • H01M4/9041—Metals or alloys
    • H01M4/905—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC
    • H01M4/9066—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC of metal-ceramic composites or mixtures, e.g. cermets
    • H—ELECTRICITY
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    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
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    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
    • H01M8/1253—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing zirconium oxide
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    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H01M8/184—Regeneration by electrochemical means
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    • C04B2111/00474—Uses not provided for elsewhere in C04B2111/00
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    • C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
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    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
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    • Y02E60/30—Hydrogen technology
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Definitions

  • Solid oxide cells such as SOFCs and SOECs, are high temperature electrochemical devices that can be used for energy conversion applications with a high electrical efficiency.
  • High temperature and non-homogeneous temperature distribution may induce mechanical stresses within SOCs leading to micro cracks and defects, or to propagation of pre-existing cracks, thus causing mechanical failure of the systems.
  • Zirconia ceramics having high fracture toughness and strength have shown promising applicability within SOCs.
  • the long-term mechanical reliability of the SOCs comprising zirconia ceramics is in fact limited by the high-temperature isothermal degradation of their tetragonal doped-zirconia components during operation.
  • the SOCs have a safe operation window of approximately 5-10kh, while the lifetime of the cells is desired to be >40kh.
  • An object of the present invention is to provide an efficient and reliable SOC having a lifetime >40kh when operated at temperatures above 350 °C, or more specifically in the range between 400 and 850 °C, for example in the range between 500 and 800 °C.
  • a further object of the present invention is to provide a SOC having high resistance to degradation, when operated at temperatures above 350 °C, thus providing and SOC having a long-term mechanical reliability.
  • An object of the present invention may also be seen as to provide an alternative to the prior art.
  • a solid oxide cell such as a SOFC or SOEC, containing at least one structural component comprising doped zirconia wherein the doped zirconia has more than 80 vol% of a metastable tetragonal crystalline phase (t-phase) and has an average grain-size between 120-190 nm and wherein the solid oxide cell is configured to be operated at temperature above 350 °C, such as between 400 and 850 °C, thereby improving aging resistance at operational temperature between 400 and 850 °C.
  • t-phase metastable tetragonal crystalline phase
  • the at least one structural component may be a porous structural component.
  • a porous structural component may be defined as a structural component having a porosity level in the oxidized form higher than 5%.
  • the solid oxide cell is configured to be operated at temperature above 400 °C, such as 450 °C.
  • the t-phase is referred herein as a metastable, i.e. transformable, tetragonal crystalline phase.
  • the doped zirconia has less than 20 vol%, such as less than 10%, of other high temperature phases such as cubic phase (c-phase) and non-transformable tetragonal phase (t'-phase).
  • c-phase cubic phase
  • t'-phase non-transformable tetragonal phase
  • the at least one structural component comprises a composite system of nickel oxide and doped zirconia, such as NiO- (Zr02)o.9?(Y203)o.o3 , (Zro.942 YO.O58 Oi.97i) or in short notation; NiO-3YSZ.
  • the composite system may have a porosity level in the oxidized form between 13 and 18%, such as 13.5%.
  • Figure 2 shows the formation of monoclinic phase during operation of a solid oxide cell comprising Nickel oxide/Yttria-stabilized zirconia (Ni(O)-3YSZ) having an average grain size of 239 nm.
  • Nickel oxide/Yttria-stabilized zirconia Ni(O)-3YSZ
  • Figure 1 shows a graphical illustration of an example of a solid oxide cell 1 according to the invention, comprising, as structural component, a porous structural support 2.
  • the solid oxide cell 1 also comprises a porous fuel electrode 3, a dense electrolyte 4 and a porous oxygen electrode 5.
  • Figure 2 is a graph plotting the percentage of monoclinic phase vs time of operation in hours, i.e. aging time (h), for a solid oxide cell comprising Nickel oxide/Yttria-stabilized zirconia (Ni(O)-3YSZ) having an average grain size of 239 nm.
  • h aging time
  • Figure 3 shows SEM images of NiO-3YSZ samples with different average grain size of 3YSZ, a) 309 nm (sample A in Table 1), b) 239 nm (Sample B in Table 1), c) 186 nm (sample C in Table 1), and d) 123 nm (Sample D in Table 1).

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Ceramic Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Sustainable Energy (AREA)
  • Sustainable Development (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Oxide Ceramics (AREA)
EP23789965.3A 2022-10-14 2023-10-12 Gegen isotherme hochtemperaturabbau beständige festoxidzelle Pending EP4602017A1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP22201521 2022-10-14
PCT/EP2023/078410 WO2024079286A1 (en) 2022-10-14 2023-10-12 A solid oxide cell resistant to high-temperature isothermal degradation

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EP4602017A1 true EP4602017A1 (de) 2025-08-20

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US7303833B2 (en) * 2004-12-17 2007-12-04 Corning Incorporated Electrolyte sheet with a corrugation pattern
JP4795949B2 (ja) * 2005-03-23 2011-10-19 株式会社日本触媒 固体酸化物形燃料電池用燃料極材料およびそれを用いた燃料極、並びに燃料電池セル

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