Ra. Olson et al., EARLY CONTAINMENT OF HIGH-ALKALINE SOLUTION SIMULATING LOW-LEVEL RADIOACTIVE-WASTE IN BLENDED CEMENT, Journal of hazardous materials, 52(2-3), 1997, pp. 223-236
Portland cement blended with fly ash and attapulgite clay was mixed wi
th high-alkaline solution simulating low-level radioactive waste at a
one-to-one weight ratio. The pastes were adiabatically and isothermall
y cured at various temperatures and analyzed for phase composition, to
tal alkalinity, pore solution chemistry, and transport properties as m
easured by impedance spectroscopy. The total alkalinity is characteriz
ed by two main drops. The early one corresponds to a rapid removal of
phosphorus, aluminum, sodium, and to a lesser extent potassium from th
e pore solution. The second drop from about 10 h to 3 days is mainly a
ssociated with the removal of aluminum, silicon, and sodium. Thereafte
r, the total alkalinity continues to decrease, but at a lower rate. Al
l pastes display a rapid loss in fluidity that is attributed to an ear
ly precipitation of hydrated products. Hemicarbonate appears as early
as 1 h after mixing and is probably followed by apatite precipitation.
The hemicarbonate is unstable, however, and decomposes at a rate that
is inversely related to the curing temperature. At high temperatures,
a sodalite-type zeolite appears at about 10 h after mixing. At 30 day
s the stabilized crystalline composition includes zeolite, apatite and
other minor amounts of CaCO3, quartz, and monosulfate. The impedance
behavior correlates with the pore solution chemistry and X-ray diffrac
tion data. The normalized conductivity of the pastes displays an early
drop followed by a large decrease from about 12 h to 3 days. At 3 day
s the permeability of the cement-based waste as calculated by the Katz
-Thompson equation is over three orders of magnitude lower than that o
f Ordinary Portland cement paste. A further decrease in the calculated
permeability is not apparent. This particular cement-based system pro
vides rapid stabilization/solidification of the waste material. The tr
ansport of waste species is reduced by probable incorporation into apa
tite, zeolite, and other solid phases. (C) 1997 Elsevier Science B.V.