CO2 sequestration and simultaneous zeolite production by carbonation of coal fly ash: Impact on the trapping of toxic elements

Abstract Coal-fired power plants are main contributors to atmospheric CO2 emissions. They also produce huge amounts of coal fly ash (CFA) waste, which is typically landfilled, posing significant environmental risks due to its high content of potentially toxic elements (PTE). However, CFA is an alkaline aluminosilicate-rich waste, which offers the possibility of CO2 mineral capture and the production of economically-relevant mineral by-products such as zeolites. Yet, the combined carbonation and zeolite production from CFA resulting in PTE trapping has never been explored. Here we show that under mild hydrothermal conditions (150 °C) and depending of various process parameters such as pH and background alkali metal ion in (bi)carbonate solutions, a carbonation efficiency of up to 79 %, with a net CO2 mineral capture of 0.045 g/g CFA can be achieved, even when using a low Ca and Mg (3.72 wt% CaO, 1.74 wt% MgO) Class F fly ash. Moreover, amorphous zeolitic precursors and different crystalline zeolites (yield up to 60 wt%) are simultaneously obtained, and PTE in CFA are effectively trapped into the newly formed calcite, zeolitic precursors, and zeolite phases. This is the first time that a combined study of carbonation, zeolitization and PTE trapping in newly formed phases has been developed. These results have important implications for carbon capture and storage, as well as for the safe reutilization and disposal of CFA waste.