Adsorption of ions on zirconium oxide surfaces from aqueous solutions at high temperatures

D. A. Palmer, M. L. MacHesky, P. Bénézeth, D. J. Wesolowski, L. M. Anovitz, J. C. Deshon

Research output: Contribution to journalArticlepeer-review

Abstract

Surface titrations were carried out on suspensions of monoclinic ZrO 2 from 25 to 290∈°C slightly above saturation vapor pressure at ionic strengths of 0.03, 0.1 and 1.0 mol · kg-1(NaCl). A typical increase in surface charge was observed with increasing temperature. There was no correlation between the radius of the cations, Li+, Na+, K+ and (CH3)4N+, and the magnitude of their association with the surface. The combined results were treated with a 1-pKa MUSIC model, which yielded association constants for the cations (and chloride ion at low pH) at each temperature. The pH of zero-point-charge, pHzpc, decreased with increasing temperature as found for other metal oxides, reaching an apparent minimum value of 4.1 by 250∈°C. Batch experiments were performed to monitor the concentration of LiOH in solutions containing suspended ZrO2 particles from 200 to 360∈°C. At 350 and 360∈°C, Li+ and OH- ions were almost totally adsorbed when the pressure was lowered to near saturation vapor pressure. This reversible trend has implications not only to pressure-water reactor, PWR, operations, but is also of general scientific and other applied interest. Additional experiments probed the feasibility that boric acid/borate ions adsorb reversibly onto ZrO2 surfaces at near-neutral pH conditions as indicated in earlier publications.

Original languageEnglish (US)
Pages (from-to)907-924
Number of pages18
JournalJournal of Solution Chemistry
Volume38
Issue number7
DOIs
StatePublished - Jul 2009
Externally publishedYes

Keywords

  • Adsorption
  • Batch experiments
  • Borate anions
  • High temperature
  • Lithium ions
  • MUSIC model
  • PWR applications
  • Potentiometry
  • Zirconium oxide

ASJC Scopus subject areas

  • Biophysics
  • Biochemistry
  • Molecular Biology
  • Physical and Theoretical Chemistry

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