Bulk carbonation of cements can have several beneficial effects, including
permeability and porosity reduction, increased compressive strength, and pH
reduction. Using supercritical and near-critical CO2, we examined both in-
situ molding processes and postsetting treatments of cement mixtures, inclu
ding those with fly ash, cement slag, and reactive silica. Specimens were c
haracterized by X-ray diffraction analysis, scanning electron microscopy, a
nd thermogravimetric analysis (for carbonate content), pH by a contact meth
od, and porosity measurements such as Na adsorption and water absorption. S
urface carbonation was almost instantaneous for cured cements using supercr
itical CO2, and rapid bulk carbonation of forms several millimeters thick c
ould be effected using in-situ molding. Carbonation by supercritical CO2 fo
rmed a dense layer of interlocking CaCO3 crystals in minutes. The best way
to rapidly carbonate large cement forms was to harden them in a mold under
CO2 pressure; these materials cured at an accelerated rate, were densified,
and showed enhanced formation of crystalline calcite. In some cases this w
as accomplished without significant loss of microporosity. The presence of
different types of reinforcing fibers did not impede carbonation by this me
thod.