Linking cesium and strontium uptake to kaolinite weathering in simulated tank waste leachate

Jon Chorover, Sunkyung Choi, Mary Kay Amistadi, K. G. Karthikeyan, Garry Crosson, Karl T. Mueller

Research output: Contribution to journalArticle

74 Citations (Scopus)

Abstract

Weathering behavior of kaolinite was studied in batch systems under geochemical conditions characteristic of tank waste released to the vadose zone at the Hanford Site, WA (0.05 M AIT, 2 M Na+, 1 M NO3-, pH ∼14, Cs+ and Sr2+ present as co-contaminants). Time series experiments were conducted from 0 to 369 d, with initial Cs+ and Sr2+ concentrations ranging from 10-5 to 10-3 M. Dissolution of kaolinite increased soluble Si and Al to maximum levels at 7 d (Cs and Sr concentrations of 10-5 and 10-4 M) or 33 d (Cs and Sr concentrations of 10-3 M). Subsequent precipitation of Si and Al was coupled to the formation of oxalate-extractable solids that incorporated Cs and Sr. Strontium sorption was nearly complete within 24 h for initial Sr concentrations (Sr0) ≤ 10-4 whereas Cs uptake increased over the full year of the experiment for all initial Cs concentrations. Spectroscopic analyses revealed neoformed solids including the zeolite Na-Al silicate (Alchabazite), and feldspathoids sodium aluminum nitrate silicate (NO3-sodalite), and sodium aluminum nitrate silicate hydrate (NO3-cancrinite), which can incorporate Cs. Singlepulse 27Al solid-state nuclear magnetic resonance (NMR) spectroscopy yielded first-order rate constants (k)for mineral transformation that decreased from 3.5 × 10-3 to 2 × 10-3 d-1 as Cs and Sr concentrations were increased from 10-5 to 10-3 M. Discrete strontium silicate solids were also observed. The incongruent dissolution of kaolinite promoted the sequestration of contaminants into increasingly recalcitrant solid phases over the 1-yr time period.

Original languageEnglish (US)
Pages (from-to)2200-2208
Number of pages9
JournalEnvironmental Science and Technology
Volume37
Issue number10
DOIs
StatePublished - May 15 2003

Fingerprint

Kaolin
Cesium
Strontium
Kaolinite
cesium
Weathering
strontium
kaolinite
leachate
weathering
silicate
Silicates
aluminum
dissolution
cancrinite
sodium
nitrate
Nitrates
sodalite
Dissolution

ASJC Scopus subject areas

  • Environmental Engineering
  • Environmental Science(all)
  • Environmental Chemistry

Cite this

Linking cesium and strontium uptake to kaolinite weathering in simulated tank waste leachate. / Chorover, Jon; Choi, Sunkyung; Amistadi, Mary Kay; Karthikeyan, K. G.; Crosson, Garry; Mueller, Karl T.

In: Environmental Science and Technology, Vol. 37, No. 10, 15.05.2003, p. 2200-2208.

Research output: Contribution to journalArticle

Chorover, Jon ; Choi, Sunkyung ; Amistadi, Mary Kay ; Karthikeyan, K. G. ; Crosson, Garry ; Mueller, Karl T. / Linking cesium and strontium uptake to kaolinite weathering in simulated tank waste leachate. In: Environmental Science and Technology. 2003 ; Vol. 37, No. 10. pp. 2200-2208.
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