Selective sulfur removal from semi-dry flue gas desulfurization coal fly ash for concrete and carbon dioxide capture applications.

High-sulfur mixed fly ash residues from semi-dry flue gas desulfurization units in coal-fired power plants are unsuitable for use as supplementary cementitious material (SCM) for concrete production or carbon dioxide utilization. In this work, we explore the potential for upcycling a representative spray dry absorber ash (10.44 wt% SO) into concrete-SCM by selective sulfur removal via weak acid dissolution while simultaneously exploring the possibility for CO capture. Towards this effort, parametric studies varying liquid-to-solid ratio, acidity, and CO pressure were conducted in a batch reactor to establish the sulfur removal characteristics in de-ionized water, nitric acid, and carbonic acid, respectively. The dissolution studies show that the leaching of sulfur from calcium sulfite hemihydrate, which is the predominant S phase, is rapid and achieves a concentration plateau within 5 min, and subsequently, appears to be controlled by the primary mineral solubility. Preferential S removal was sufficient to meet SCM standards (e.g., 5.0 wt% as per ASTM C618) using all three washing solutions with 0.62-0.72 selectivity (S^), defined as the molar ratio of S to Ca in the leachate, for a raw fly ash with bulk S^ = 0.3. Acid dissolution with 1.43 meq/g of ash or under 5 atm CO retained > 18 wt% CaO and other Si-, Al-rich phases in the fly ash. Based on the experimental findings, two sulfur removal schemes were suggested for either integration with CO capture and utilization processes using flue gas or to produce fly ash for use as a SCM.