This work assesses a combined accelerated
carbonation and wet granulation
treatment applied to circulating fluidized bed combustion fly ash
with the aim of producing secondary aggregates for civil engineering
applications and of achieving a net storage of CO2. The
experiments were carried out at both a laboratory scale and larger
scale, and the effects of the CO2 content of the gas flow
(40 or 100%), temperature (from 25 to 60 °C), and the use of
an alkaline activator solution as binder for the granulation process
were investigated. Specifically, the particle size distribution, aggregate
crushing value, leaching behavior, and CO2 uptake of the
products after 28 days curing under ambient air were analyzed. In
addition, the energy requirements of the process were estimated on
the basis of the results of the larger scale tests and were used to
calculate the CO2 emissions of the process to estimate
the net CO2 avoided that could be achieved per kilogram
of produced aggregate. The carbo-granulation process allowed us to
achieve a relevant increase in particle size with respect to the starting
material. The conditions that yielded the best performance in terms
of product properties (both technical and environmental) and the maximum
amount of CO2 avoided (above 75 g of CO2/kg
aggregate) was the carbo-granulation treatment performed at 60 °C
with water as binder and a gas phase containing 40% CO2. Although the products obtained employing the alkaline activator
solution presented a lower mobility of trace elements of potential
environmental concern and generally a higher CO2 uptake
compared to the granules produced with water as granulation binder,
the carbon footprint of the additives (sodium silicate in particular)
would make the process carbon positive, even considering the CO2 avoided by replacing natural aggregates.