Trace contaminant concentration affects mineral transformation and pollutant fate in hydroxide-weathered Hanford sediments

Nicolas Perdrial; Nelson Rivera; Aaron Thompson; Peggy A. O'Day; Jon Chorover

doi:10.1016/j.jhazmat.2011.09.063

Trace contaminant concentration affects mineral transformation and pollutant fate in hydroxide-weathered Hanford sediments

Nicolas Perdrial, Nelson Rivera, Aaron Thompson, Peggy A. O'Day, Jon Chorover

Research output: Contribution to journal › Article › peer-review

23 Scopus citations

Abstract

Prior work has shown that when silicaceous sediments are infused with caustic radioactive waste, contaminant fate is tightly coupled to ensuing mineral weathering reactions. However, the effects of local aqueous geochemical conditions on these reactions are poorly studied. Thus, we varied contaminant concentration and pCO ₂ during the weathering of previously uncontaminated Hanford sediments over 6 months and 1 year in a solution of caustic waste (pH 13, high ionic strength). Co-contaminants Sr, Cs and I were added at " low" (Cs/Sr: 10 ^-5m; I: 10 ^-7m) and " high" (Cs/Sr: 10 ^-3m; I: 10 ^-5m) concentrations, and headspace was held at atmospheric or undetectable (<10ppmv) CO ₂ partial pressure. Solid phase characterization revealed the formation of the zeolite chabazite in " high" samples, whereas feldspathoids, sodalite and cancrinite, were formed preferentially in " low" samples. Sr, Cs and I were sequestered in all reacted sediments. Native calcite dissolution in the CO ₂-free treatment drove the formation of strätlingite (Ca ₂Al ₂SiO ₇·8H ₂O) and diminished availability of Si and Al for feldspathoid formation. Results indicate that pCO ₂ and contaminant concentrations strongly affect contaminant speciation in waste-weathered sediments, and are therefore likely to impact reaction product stability under any remediation scenario.

Original language	English (US)
Pages (from-to)	119-127
Number of pages	9
Journal	Journal of Hazardous Materials
Volume	197
DOIs	https://doi.org/10.1016/j.jhazmat.2011.09.063
State	Published - Dec 15 2011

Keywords

Cesium
Feldspathoids
Strontium
Strätlingite
Zeolite

ASJC Scopus subject areas

Environmental Engineering
Environmental Chemistry
Waste Management and Disposal
Pollution
Health, Toxicology and Mutagenesis

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10.1016/j.jhazmat.2011.09.063

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title = "Trace contaminant concentration affects mineral transformation and pollutant fate in hydroxide-weathered Hanford sediments",

abstract = "Prior work has shown that when silicaceous sediments are infused with caustic radioactive waste, contaminant fate is tightly coupled to ensuing mineral weathering reactions. However, the effects of local aqueous geochemical conditions on these reactions are poorly studied. Thus, we varied contaminant concentration and pCO 2 during the weathering of previously uncontaminated Hanford sediments over 6 months and 1 year in a solution of caustic waste (pH 13, high ionic strength). Co-contaminants Sr, Cs and I were added at {"} low{"} (Cs/Sr: 10 -5m; I: 10 -7m) and {"} high{"} (Cs/Sr: 10 -3m; I: 10 -5m) concentrations, and headspace was held at atmospheric or undetectable (<10ppmv) CO 2 partial pressure. Solid phase characterization revealed the formation of the zeolite chabazite in {"} high{"} samples, whereas feldspathoids, sodalite and cancrinite, were formed preferentially in {"} low{"} samples. Sr, Cs and I were sequestered in all reacted sediments. Native calcite dissolution in the CO 2-free treatment drove the formation of str{\"a}tlingite (Ca 2Al 2SiO 7·8H 2O) and diminished availability of Si and Al for feldspathoid formation. Results indicate that pCO 2 and contaminant concentrations strongly affect contaminant speciation in waste-weathered sediments, and are therefore likely to impact reaction product stability under any remediation scenario.",

keywords = "Cesium, Feldspathoids, Strontium, Str{\"a}tlingite, Zeolite",

author = "Nicolas Perdrial and Nelson Rivera and Aaron Thompson and O'Day, {Peggy A.} and Jon Chorover",

note = "Funding Information: This research is funded by the Environmental Remediation Science Program (ERSP) , Biological and Environmental Research (BER) , Office of Science, U.S. Department of Energy , Grant no. DE-FG02-06ER64190 . Dr. T. Fridriksson (ISOR, Iceland) kindly provided the reference chabazite sample. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences. The SSRL Structural Molecular Biology Program is supported by the Department of Energy, Office of Biological and Environmental Research, and by the National Institutes of Health, National Center for Research Resources, Biomedical Technology Program. ",

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doi = "10.1016/j.jhazmat.2011.09.063",

language = "English (US)",

volume = "197",

pages = "119--127",

journal = "Journal of Hazardous Materials",

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T1 - Trace contaminant concentration affects mineral transformation and pollutant fate in hydroxide-weathered Hanford sediments

AU - Perdrial, Nicolas

AU - Rivera, Nelson

AU - Thompson, Aaron

AU - O'Day, Peggy A.

AU - Chorover, Jon

N1 - Funding Information: This research is funded by the Environmental Remediation Science Program (ERSP) , Biological and Environmental Research (BER) , Office of Science, U.S. Department of Energy , Grant no. DE-FG02-06ER64190 . Dr. T. Fridriksson (ISOR, Iceland) kindly provided the reference chabazite sample. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences. The SSRL Structural Molecular Biology Program is supported by the Department of Energy, Office of Biological and Environmental Research, and by the National Institutes of Health, National Center for Research Resources, Biomedical Technology Program.

PY - 2011/12/15

Y1 - 2011/12/15

N2 - Prior work has shown that when silicaceous sediments are infused with caustic radioactive waste, contaminant fate is tightly coupled to ensuing mineral weathering reactions. However, the effects of local aqueous geochemical conditions on these reactions are poorly studied. Thus, we varied contaminant concentration and pCO 2 during the weathering of previously uncontaminated Hanford sediments over 6 months and 1 year in a solution of caustic waste (pH 13, high ionic strength). Co-contaminants Sr, Cs and I were added at " low" (Cs/Sr: 10 -5m; I: 10 -7m) and " high" (Cs/Sr: 10 -3m; I: 10 -5m) concentrations, and headspace was held at atmospheric or undetectable (<10ppmv) CO 2 partial pressure. Solid phase characterization revealed the formation of the zeolite chabazite in " high" samples, whereas feldspathoids, sodalite and cancrinite, were formed preferentially in " low" samples. Sr, Cs and I were sequestered in all reacted sediments. Native calcite dissolution in the CO 2-free treatment drove the formation of strätlingite (Ca 2Al 2SiO 7·8H 2O) and diminished availability of Si and Al for feldspathoid formation. Results indicate that pCO 2 and contaminant concentrations strongly affect contaminant speciation in waste-weathered sediments, and are therefore likely to impact reaction product stability under any remediation scenario.

AB - Prior work has shown that when silicaceous sediments are infused with caustic radioactive waste, contaminant fate is tightly coupled to ensuing mineral weathering reactions. However, the effects of local aqueous geochemical conditions on these reactions are poorly studied. Thus, we varied contaminant concentration and pCO 2 during the weathering of previously uncontaminated Hanford sediments over 6 months and 1 year in a solution of caustic waste (pH 13, high ionic strength). Co-contaminants Sr, Cs and I were added at " low" (Cs/Sr: 10 -5m; I: 10 -7m) and " high" (Cs/Sr: 10 -3m; I: 10 -5m) concentrations, and headspace was held at atmospheric or undetectable (<10ppmv) CO 2 partial pressure. Solid phase characterization revealed the formation of the zeolite chabazite in " high" samples, whereas feldspathoids, sodalite and cancrinite, were formed preferentially in " low" samples. Sr, Cs and I were sequestered in all reacted sediments. Native calcite dissolution in the CO 2-free treatment drove the formation of strätlingite (Ca 2Al 2SiO 7·8H 2O) and diminished availability of Si and Al for feldspathoid formation. Results indicate that pCO 2 and contaminant concentrations strongly affect contaminant speciation in waste-weathered sediments, and are therefore likely to impact reaction product stability under any remediation scenario.

KW - Cesium

KW - Feldspathoids

KW - Strontium

KW - Strätlingite

KW - Zeolite

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DO - 10.1016/j.jhazmat.2011.09.063

M3 - Article

C2 - 21993146

AN - SCOPUS:82155172860

SN - 0304-3894

VL - 197

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EP - 127

JO - Journal of Hazardous Materials

JF - Journal of Hazardous Materials

ER -

Trace contaminant concentration affects mineral transformation and pollutant fate in hydroxide-weathered Hanford sediments

Abstract

Keywords

ASJC Scopus subject areas

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