Characterization and modeling of major constituent equilibrium chemistry of a blended cement mortar

¹ Vanderbilt University, Department of Civil and Environmental Engineering, Nashville, Tennessee, USA
² Nuclear Research and consultancy Group, Radiation and Environment, Petten, Netherlands
³ Hans van der Sloot Consultancy, Langedijk, Netherlands

^a e-mail: David.Kosson@vanderbilt.edu

Abstract

Cementitious materials containing ground granulated iron blast furnace slag and coal combustion fly ash as admixtures are being used extensively for nuclear waste containment applications. Whereas the solid phases of ordinary Portland cement (OPC) have been studied in great detail, the chemistry of cement, fly ash and slag blends has received relatively less study. Given that OPC is generally more reactive than slag and fly ash, the mineralogy of OPC provides a logical starting point for describing the major constituent chemistry of blended cement mortars. To this end, a blended cement mortar containing Portland cement, granulated blast furnace slag, fly ash and quartz sand was modeled using a set of solid phases known to form in hydrated OPC with the geochemical speciation solver LeachXS/ORCHESTRA. Comparison of modeling results to the experimentally determined pH-dependent batch leaching concentrations (USEPA Method 1313) indicates that major constituent concentrations are described reasonably well with the Portland cement mineral set; however, modeled and measured aluminum concentrations differ greatly. Scanning electron microscopic analysis of the mortar reveals the presence of Al-rich phyllosilicate minerals heretofore unreported in similar cementitious blends: kaolinite and potassic phyllosilicates similar in composition to illite and muscovite. Whereas the potassic phyllosilicates are present in the quartz sand aggregate, the formation of kaolinite appears to be authigenic. The inclusion of kaolinite in speciation modeling provides a substantially improved description of the release of Al and therefore, suggests that the behavior of phyllosilicate phases may be important for predicting long-term physico-chemical behavior of such systems.