Journal
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
Volume 650, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.colsurfa.2022.129636
Keywords
Plutonium; Zirconium; Colloidal Chinese Bentonite; Small Angle X-ray scattering; Adsorption
Categories
Funding
- National Nature Science Foundation of China [U1932117]
- State Key Laboratory of Environment -friendly Energy Materials [20fksy07]
- China Academy of Engineering Physics [21zh0313]
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Carrier colloids have been identified as the primary mechanism for enhancing the transport of actinides in the subsurface at former nuclear weapons facilities. However, there is a lack of sub-micrometer size investigations on the sorption/interactions between radionuclides and natural colloids. This study evaluated the interactions between Pu (IV)/Zr (IV) and colloids formed from Chinese Gaomiaozi bentonite, providing valuable insights into the potential migration of these elements in subsurface waters.
According to previous field experiments, carrier colloids represent the primary mechanism for enhancing the transport of actinides in the subsurface at former nuclear weapons facilities. However, sub-micrometer size investigations on the sorption/interactions between radionuclides and natural colloids are scarce. In the present study, interactions between Pu (IV)/Zr (IV) and the colloids formed from Chinese Gaomiaozi bentonite in water were evaluated using sorption experiments, scanning electron microscopy, transmission electron microscopy, dynamic light scattering, X-ray photoelectron spectroscopy, and small-angle X-ray scattering. Stable GMZ bentonite colloids showed zeta potentials of -31.8(0.9) mV at 25-85 degrees C. Small-angle X-ray scattering from these colloids showed that the d-space (2.12 nm) of the colloidal particles dispersed in water exceeded that of mineral fragments obtained from the bulk powder (1.45 nm) in air, an indication of swelling. In addition, these colloidal particles (336 nm in size) exhibited higher affinities (K-d similar to 10(4) mL g(-1)) for Pu (IV) compared with bulk GMZ fragments (K-d - 10(3) mL g(-1)) at pH 7. X-ray diffraction showed that montmorillonite was the primarily component of colloidal GMZ particles, while X-ray photoelectron spectroscopy indicated that this clay mineral played an important role in the interaction with Pu (IV)/Zr (IV). Small-angle X-ray scattering from Zr (IV) solutions, showed power-law scattering (Intensity proportional to q(-)(alpha)) exponent a that increased from 2.6 to 3.4 (0(.1) nm(-1) < q < 0.5 nm(-1)), and decreased from 1.56 to 0.87 (q similar to 0.2 nm(-1)) as the Zr (IV) was raised from 0 to 9.8 x 10(-11) mol dm(-3). These results related to the partial agglomeration and precipitation of GMZ bentonite colloids. The remaining associative colloids pose a potential threat of Pu (IV) or Zr (IV) migration in subsurface waters.
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