Ion exchange equilibrium and structural changes in clinoptilolite irradiated with β- and γ-radiation

Monovalent cations

Daniel Moraetis, George E. Christidis, Vasilios Peridikatsis

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

Thermodynamic calculations of ion-exchange reactions were applied for clinoptilolite in a natural state and after irradiation with three doses of β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). Samples were equilibrated with binary systems of K+ ↔ Na+ and Cs+ ↔ Na+ at 25° and a total normality of 0.025 N. Selectivity for K was not affected after β-radiation with doses of 1012 and 1015 e/cm2 (ΔG° = -6.37 kJ/equiv, lnKα = 2.58 for the original clinoptilolite), whereas it increased considerably after 70 Mrad of γ-radiation (ΔG° = -7.88 kJ/equiv, lnKα = 3.18). Selectivity for Cs+ increased for the clinoptilolite irradiated with β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). ΔG° and lnKα for original sample and Cs+ ↔ Na+ were -7.33 kJ/equiv and 2.96, respectively. Irradiated samples with β-radiation 1012, 1015, 3 × 1016 e/cm2 and 70 Mrad γ-radiation yielded ΔG° and lnKα -7.41, -8.83, -8.60, -8.25 kJ/equiv and 2.99, 3.57, 3.47, 3.33 for Cs+ ↔ Na+, respectively. Remarkable amorphization of clinoptilolite was observed after exposure at the highest dose of β-radiation (3 × 1016 e/cm2) with a concomitant decrease in cation-exchange capacity (CEC). Crystallographic parameters and especially exchangeable cation site coordinates were refined for all samples with the Rietveld method. Cesium-saturated samples exhibited changes in the cation sites Cs2 and Cs3, which are next to clinoptilolite channel walls with lower Al3+ for Si4+ substitution. The observed changes include a shift in cation sites Cs2 and Cs3 toward channel walls and occupancy decrease in site Cs2.

Original languageEnglish
Pages (from-to)1714-1730
Number of pages17
JournalAmerican Mineralogist
Volume92
Issue number10
DOIs
Publication statusPublished - Oct 2007

Fingerprint

Monovalent Cations
clinoptilolite
structural change
ion exchange
Ion exchange
cation
Radiation
cations
radiation
ions
Cations
Dosimetry
dosage
selectivity
normality
Rietveld method
Cesium
Amorphization
cesium
cation exchange capacity

Keywords

  • β-radiation
  • γ-radiation
  • Clinoptilolite
  • Ion exchange
  • Rietveld refinement
  • Thermodynamics

ASJC Scopus subject areas

  • Geophysics
  • Geochemistry and Petrology

Cite this

Ion exchange equilibrium and structural changes in clinoptilolite irradiated with β- and γ-radiation : Monovalent cations. / Moraetis, Daniel; Christidis, George E.; Peridikatsis, Vasilios.

In: American Mineralogist, Vol. 92, No. 10, 10.2007, p. 1714-1730.

Research output: Contribution to journalArticle

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abstract = "Thermodynamic calculations of ion-exchange reactions were applied for clinoptilolite in a natural state and after irradiation with three doses of β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). Samples were equilibrated with binary systems of K+ ↔ Na+ and Cs+ ↔ Na+ at 25° and a total normality of 0.025 N. Selectivity for K was not affected after β-radiation with doses of 1012 and 1015 e/cm2 (ΔG° = -6.37 kJ/equiv, lnKα = 2.58 for the original clinoptilolite), whereas it increased considerably after 70 Mrad of γ-radiation (ΔG° = -7.88 kJ/equiv, lnKα = 3.18). Selectivity for Cs+ increased for the clinoptilolite irradiated with β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). ΔG° and lnKα for original sample and Cs+ ↔ Na+ were -7.33 kJ/equiv and 2.96, respectively. Irradiated samples with β-radiation 1012, 1015, 3 × 1016 e/cm2 and 70 Mrad γ-radiation yielded ΔG° and lnKα -7.41, -8.83, -8.60, -8.25 kJ/equiv and 2.99, 3.57, 3.47, 3.33 for Cs+ ↔ Na+, respectively. Remarkable amorphization of clinoptilolite was observed after exposure at the highest dose of β-radiation (3 × 1016 e/cm2) with a concomitant decrease in cation-exchange capacity (CEC). Crystallographic parameters and especially exchangeable cation site coordinates were refined for all samples with the Rietveld method. Cesium-saturated samples exhibited changes in the cation sites Cs2 and Cs3, which are next to clinoptilolite channel walls with lower Al3+ for Si4+ substitution. The observed changes include a shift in cation sites Cs2 and Cs3 toward channel walls and occupancy decrease in site Cs2.",
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N2 - Thermodynamic calculations of ion-exchange reactions were applied for clinoptilolite in a natural state and after irradiation with three doses of β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). Samples were equilibrated with binary systems of K+ ↔ Na+ and Cs+ ↔ Na+ at 25° and a total normality of 0.025 N. Selectivity for K was not affected after β-radiation with doses of 1012 and 1015 e/cm2 (ΔG° = -6.37 kJ/equiv, lnKα = 2.58 for the original clinoptilolite), whereas it increased considerably after 70 Mrad of γ-radiation (ΔG° = -7.88 kJ/equiv, lnKα = 3.18). Selectivity for Cs+ increased for the clinoptilolite irradiated with β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). ΔG° and lnKα for original sample and Cs+ ↔ Na+ were -7.33 kJ/equiv and 2.96, respectively. Irradiated samples with β-radiation 1012, 1015, 3 × 1016 e/cm2 and 70 Mrad γ-radiation yielded ΔG° and lnKα -7.41, -8.83, -8.60, -8.25 kJ/equiv and 2.99, 3.57, 3.47, 3.33 for Cs+ ↔ Na+, respectively. Remarkable amorphization of clinoptilolite was observed after exposure at the highest dose of β-radiation (3 × 1016 e/cm2) with a concomitant decrease in cation-exchange capacity (CEC). Crystallographic parameters and especially exchangeable cation site coordinates were refined for all samples with the Rietveld method. Cesium-saturated samples exhibited changes in the cation sites Cs2 and Cs3, which are next to clinoptilolite channel walls with lower Al3+ for Si4+ substitution. The observed changes include a shift in cation sites Cs2 and Cs3 toward channel walls and occupancy decrease in site Cs2.

AB - Thermodynamic calculations of ion-exchange reactions were applied for clinoptilolite in a natural state and after irradiation with three doses of β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). Samples were equilibrated with binary systems of K+ ↔ Na+ and Cs+ ↔ Na+ at 25° and a total normality of 0.025 N. Selectivity for K was not affected after β-radiation with doses of 1012 and 1015 e/cm2 (ΔG° = -6.37 kJ/equiv, lnKα = 2.58 for the original clinoptilolite), whereas it increased considerably after 70 Mrad of γ-radiation (ΔG° = -7.88 kJ/equiv, lnKα = 3.18). Selectivity for Cs+ increased for the clinoptilolite irradiated with β-radiation (1012, 1015, 3 × 1016 e/cm2) and γ-radiation (70 Mrad). ΔG° and lnKα for original sample and Cs+ ↔ Na+ were -7.33 kJ/equiv and 2.96, respectively. Irradiated samples with β-radiation 1012, 1015, 3 × 1016 e/cm2 and 70 Mrad γ-radiation yielded ΔG° and lnKα -7.41, -8.83, -8.60, -8.25 kJ/equiv and 2.99, 3.57, 3.47, 3.33 for Cs+ ↔ Na+, respectively. Remarkable amorphization of clinoptilolite was observed after exposure at the highest dose of β-radiation (3 × 1016 e/cm2) with a concomitant decrease in cation-exchange capacity (CEC). Crystallographic parameters and especially exchangeable cation site coordinates were refined for all samples with the Rietveld method. Cesium-saturated samples exhibited changes in the cation sites Cs2 and Cs3, which are next to clinoptilolite channel walls with lower Al3+ for Si4+ substitution. The observed changes include a shift in cation sites Cs2 and Cs3 toward channel walls and occupancy decrease in site Cs2.

KW - β-radiation

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KW - Ion exchange

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