Accelerated and natural carbonation of concrete with high volumes of fly ash: chemical, mineralogical and microstructural effects.

Today, a rather poor carbonation resistance is being reported for high-volume fly ash (HVFA) binder systems. This conclusion is usually drawn from accelerated carbonation experiments conducted at CO2 levels that highly exceed the natural atmospheric CO2 concentration of 0.03-0.04%. However, such accelerated test conditions may change the chemistry of the carbonation reaction (and the resulting amount of CH and C-S-H carbonation), the nature of the mineralogical phases formed (stable calcite versus metastable vaterite, aragonite) and the resulting porosity and pore size distribution of the microstructure after carbonation. In this paper, these phenomena were studied on HVFA and fly ash + silica fume (FA + SF) pastes after exposure to 0.03-0.04%, 1% and 10% CO2 using thermogravimetric analysis, quantitative X-ray diffraction and mercury intrusion porosimetry. It was found that none of these techniques unambiguously revealed the reason for significantly underestimating carbonation rates at 1% CO2 from colorimetric carbonation test results obtained after exposure to 10% CO2 that were implemented in a conversion formula that solely accounts for the differences in CO2 concentration. Possibly, excess water production due to carbonation at too high CO2 levels with a pore blocking effect and a diminished solubility for CO2 plays an important role in this.