Utilization of low-calcium fly ash via direct aqueous carbonation with a low-energy input: Determination of carbonation reaction and evaluation of the potential for CO2 sequestration and utilization

Abstract

Environmental impacts from coal-fired power generation that produces large amounts of CO₂ and fly ash are of great interest. To reduce negative environmental impacts, fly ash utilization was investigated via a direct aqueous carbonation with a low-energy input in which the alkali calcium content in the fly ash reacted with CO₂ to form carbonate. Raw fly ash was characterized to understand the potential for direct aqueous carbonation of fly ash. The performance of the fly ash as a calcium source for direct aqueous carbonation at atmospheric pressure was investigated for different solid-liquid ratios and introduced CO₂ concentrations. Variations in fly ash elemental composition, reaction solution pH, CO₂ concentration in the reactor outlet, CO₂ uptake efficiency, CaCO₃ content and degree of carbonation were used to illustrate this process reaction. The maximum CO₂ uptake efficiency was ~0.016 g-CO₂/g-fly ash. This value was compared with previous studies, and the CO₂ uptake efficiency was comparable despite the use of a low-energy input method, i.e., direct aqueous carbonation with atmospheric pressure and unconcentrated CO₂. The calculated maximum degree of carbonation was 31.0%, which corresponds to 0.0063 g-CO₂/g-fly ash. Carbonated product characterization confirmed the carbonation reaction mechanism and safety for further utilization. A comparison of CO₂ uptake efficiency in this work with previous work, and considering the energy input and reactive species content, is provided. An assessment of the CO₂ reduction potential is provided.

Keywords: CO(2) sequestration; CO(2) utilization; Direct aqueous carbonation; Low-calcium fly ash; Low-energy input.