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Ceria–Zirconia Solid Solutions (Ce1–x Zr x O2−δ, x ≤ 0.2) for Solar Thermochemical Water Splitting: A Thermodynamic Study

Hao, Yong ; Yang, Chih-Kai ; Haile, Sossina M

Chemistry of materials, 2014-10, Vol.26 (20), p.6073-6082 [Peer Reviewed Journal]

American Chemical Society

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  • Title:
    Ceria–Zirconia Solid Solutions (Ce1–x Zr x O2−δ, x ≤ 0.2) for Solar Thermochemical Water Splitting: A Thermodynamic Study
  • Author: Hao, Yong ; Yang, Chih-Kai ; Haile, Sossina M
  • Is Part Of: Chemistry of materials, 2014-10, Vol.26 (20), p.6073-6082
  • Description: The redox behavior of ceria–zirconia solid solutions (or Zr-substituted ceria, ZSC) with a Zr content of up to 20 mol % is studied by thermogravimetry (TG) between 600 °C and 1490 °C under controlled atmospheres. Thermodynamic properties, specifically standard oxidation enthalpy, ΔH oxd ⊖, and entropy, ΔS oxd ⊖, are derived from TG data. The raw TG results show that the extent of reduction is significantly increased (compared with undoped ceria), even at a low Zr substitution level of 5 mol %. Concomitantly, the magnitude of the thermodynamic functions dramatically decreases as a function of Zr content, particularly at low values of oxygen non-stoichiometry, δ (<3 mol %). Thermochemical fuel production from Zr-substituted ceria generally increases with increasing Zr content under both two-temperature and isothermal cycling conditions. In the case of two-temperature cycling, the benefit is accompanied by a penalty in the (computed) steam-to-hydrogen conversion ratio, whereas it is accompanied by a gain in this ratio for isothermal cycling. Overall, introduction of Zr has the potential to enhance solar-driven thermochemical fuel production, depending on the details of cycling conditions and reactor design.
  • Publisher: American Chemical Society
  • Language: English
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