Sorption of Cs+ to Micaceous Subsurface Sediments from the Hanford Site, USA

Zachara, John M; Smith, Steven C; Liu, Chongxuan; McKinley, James P; Serne, R Jeffrey; Gassman, Paul L

doi:10.1016/S0016-7037(01)00759-1

Title: Sorption of Cs+ to Micaceous Subsurface Sediments from the Hanford Site, USA

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Abstract

The sorption of Cs{sup +} was investigated over a large concentration range (10{sup -9}-10{sup -2} mol/L) on subsurface sediments from a United States nuclear materials site (Hanford) where high-level nuclear wastes (HLW) have been accidentally released to the vadose zone. The sediment sorbs large amounts of radiocesium, but expedited migration has been observed when HLW (a NaNO{sub 3} brine) is the carrier. Cs{sup +} sorption was measured on homoionic sediments (Na{sup +}, K{sup +}, Ca{sup 2+}) with electrolyte concentrations ranging from 0.01 to 1.0 mol/L. In Na{sup +} electrolyte, concentrations were extended to near saturation with NaNO{sub 3(s)} (7.0 mol/L). The sediment contained nonexpansible (biotite, muscovite) and expansible (vermiculite, smectite) phyllosilicates. The sorption data were interpreted according to the frayed edge-planar site conceptual model. A four-parameter, two-site (high- and low-affinity) numeric ion exchange model was effective in describing the sorption data. The high-affinity sites were ascribed to wedge zones on the micas where particle edges have partially expanded due to the removal of interlayer cations during weathering, and the low-affinity ones to planar sites on the expansible clays. The electrolyte cations competed with Cs{sup +} for both high- and low-affinity sites according to the trend K{sup +} >> Na{sup +}more »« less

Authors:: Zachara, John M; Smith, Steven C; Liu, Chongxuan; McKinley, James P; Serne, R Jeffrey; Gassman, Paul L

Publication Date:: Tue Jan 15 00:00:00 EST 2002

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1033470

Report Number(s):: PNNL-SA-33718
Journal ID: ISSN 0016-7037; GCACAK; KP1301020; TRN: US201202%%769

DOE Contract Number:: AC05-76RL01830

Resource Type:: Journal Article

Journal Name:: Geochimica et Cosmochimica Acta

Additional Journal Information:: Journal Volume: 66; Journal Issue: 2; Journal ID: ISSN 0016-7037

Country of Publication:: United States

Language:: English

Subject:: 12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; ADSORPTION; BIOTITE; CATIONS; CLAYS; ELECTROLYTES; ELECTRONS; ILLITE; ION EXCHANGE; MICA; MUSCOVITE; RADIOACTIVE WASTES; REMOVAL; SATURATION; SEDIMENTS; SMECTITE; SORPTION; VERMICULITE; WEATHERING; Cs adsorption; ion exchange; high ionic strength; AgTU; adsorption modeling

Citation Formats


                    Zachara, John M, Smith, Steven C, Liu, Chongxuan, McKinley, James P, Serne, R Jeffrey, and Gassman, Paul L. Sorption of Cs+ to Micaceous Subsurface Sediments from the Hanford Site, USA.  United States: N. p., 2002. 
        Web.  doi:10.1016/S0016-7037(01)00759-1.

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                    Zachara, John M, Smith, Steven C, Liu, Chongxuan, McKinley, James P, Serne, R Jeffrey, & Gassman, Paul L. Sorption of Cs+ to Micaceous Subsurface Sediments from the Hanford Site, USA.  United States.  https://doi.org/10.1016/S0016-7037(01)00759-1

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                    Zachara, John M, Smith, Steven C, Liu, Chongxuan, McKinley, James P, Serne, R Jeffrey, and Gassman, Paul L. 2002.  
        "Sorption of Cs+ to Micaceous Subsurface Sediments from the Hanford Site, USA".  United States.  https://doi.org/10.1016/S0016-7037(01)00759-1.

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@article{osti_1033470,

  title        = {Sorption of Cs+ to Micaceous Subsurface Sediments from the Hanford Site, USA},

  author       = {Zachara, John M and Smith, Steven C and Liu, Chongxuan and McKinley, James P and Serne, R Jeffrey and Gassman, Paul L},

  abstractNote = {The sorption of Cs{sup +} was investigated over a large concentration range (10{sup -9}-10{sup -2} mol/L) on subsurface sediments from a United States nuclear materials site (Hanford) where high-level nuclear wastes (HLW) have been accidentally released to the vadose zone. The sediment sorbs large amounts of radiocesium, but expedited migration has been observed when HLW (a NaNO{sub 3} brine) is the carrier. Cs{sup +} sorption was measured on homoionic sediments (Na{sup +}, K{sup +}, Ca{sup 2+}) with electrolyte concentrations ranging from 0.01 to 1.0 mol/L. In Na{sup +} electrolyte, concentrations were extended to near saturation with NaNO{sub 3(s)} (7.0 mol/L). The sediment contained nonexpansible (biotite, muscovite) and expansible (vermiculite, smectite) phyllosilicates. The sorption data were interpreted according to the frayed edge-planar site conceptual model. A four-parameter, two-site (high- and low-affinity) numeric ion exchange model was effective in describing the sorption data. The high-affinity sites were ascribed to wedge zones on the micas where particle edges have partially expanded due to the removal of interlayer cations during weathering, and the low-affinity ones to planar sites on the expansible clays. The electrolyte cations competed with Cs{sup +} for both high- and low-affinity sites according to the trend K{sup +} >> Na{sup +} {ge} Ca{sup 2+}. At high salt concentration, Cs{sup +} adsorption occurred only on high-affinity sites. Na{sup +} was an effective competitor for the high-affinity sites at high salt concentrations. In select experiments, silver-thiourea (AgTU) was used as a blocking agent to further isolate and characterize the high-affinity sites, but the method was found to be problematic. Mica particles were handpicked from the sediment, contacted with Cs{sub eq}{sup +}, and analyzed by electron microprobe to identify phases and features important to Cs{sup +} sorption. The microprobe study implied that biotite was the primary contributor of high-affinity sites because of its weathered periphery. The poly-phase sediment exhibited close similarity in ion selectivity to illite, which has been well studied, although its proportion of high-affinity sites relative to the cation exchange capacity (CEC) was lower than that of illite. Important insights are provided on how Na{sup +} in HLW and indigenous K{sup +} displaced from the sediments may act to expedite the migration of strongly sorbing Cs{sup +} in subsurface environments.},

  doi          = {10.1016/S0016-7037(01)00759-1},

  url          = {https://www.osti.gov/biblio/1033470},
  journal      = {Geochimica et Cosmochimica Acta},

  issn         = {0016-7037},

  number       = 2,

  volume       = 66,

  place        = {United States},

  year         = {Tue Jan 15 00:00:00 EST 2002},

  month        = {Tue Jan 15 00:00:00 EST 2002}

}

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