Geochemical Partitioning of Major Elements in Brine Impacted Coal Fly Ash Residues

Fly ash-brine co-disposal technique has been considered as a way of disposing fly ash and brine (hyper-saline water) by some power stations in South Africa. This practice was aimed at using the fly ash to capture most of the elements in brine. However, the geochemical partitioning of the major elements in the waste materials after the fly ash-brine interaction has not been fully understood. This study focuses on understanding the geochemical partitioning of the major elements captured in the fly ash solid residues after the fly ash-brine interaction experiment. XRF and sequential extraction procedure were respectively applied to determine the chemical composition and partitioning of the major elements in fresh fly ash and the solid residues recovered after fly ash-brine interaction. The comparison of the results of the XRF analysis carried out on the fresh fly ash and the solid residues showed that the major elements such as Si, Ca, Mg and Na increased in the solid residues after the fly ash-brine interaction. This indicates that Ca, Mg and Na in the brine solution were captured by the fly ash during the interaction. However, the sequential extraction results showed that significant concentrations of Ca, Na and Mg were released into the water soluble, exchangeable and carbonate fractions. The results show that significant amounts of the elements captured in the fly ash solid residues during fly ash-brine interaction exist in the form which can be easily leached out when in contact with aqueous solution

A Geochemical Analytical Scheme for the Appraisal of Partitioning and Mobility of Major elements in Weathered Dry Disposed Coal Fly Ash

South Africa is endowed with significant deposits of coal which is utilized in electricity generation to meet the nation’s energy demand. A large volume of waste solid residue from the combustion of pulverized feed coal in power stations is dry disposed in stock piles or dumps. Chemical interactions of dry disposed fly ash with ingressed CO2 from the atmosphere and infiltrating rain water would cause dissolution of the soluble components in the fly ash matrix. Chemical partitioning and mobility of major elements in samples from cores drilled into serially stacked weathered dry disposed fly ash were investigated using a modified five steps sequential extraction scheme. A total acid digestion was carried out on the original ash core samples prior to extraction to validate the extraction procedure. The geochemical distribution of the investigated major elements in 59 drilled core samples was determined by x-ray fluorescence and inductively coupled plasma mass spectrometry. The relationship between SiO2 and chemical index of alteration (CIA) showed 8 year and 20-year-old core samples have a moderate to high degree of weathering. Conversely, 1-year-old cores samples showed characteristics between low and moderate-high degrees of weathering. A cluster and discriminant analysis of the major elements was also able to reveal the subtle chemical alteration differences of the core samples. Functional analysis revealed the disparities in the dissolution patterns of major soluble components in the matrix of the drilled core samples. Modified sequential extractions revealed high concentration of the major species in the leachates for every mineralogical fraction; although the bulk of the major elements are locked up in the insoluble phase of the core samples (i.e. residual fraction) which would not be released under normal environmental conditions. It is noteworthy that the concentration of major elements in the labile fractions (water soluble + exchangeable + carbonate) was high and this has implications for the long-term durability of residual mineral phases. Relative enrichment and depletion trends of major elements are promoted by heterogeneity in the ash dump (i.e. moisture content), gradual reduction of pore water pH and continuous brine and water irrigation.Key words: Coal fly ash; Weathering; Sequential extraction scheme; Cluster analysis; Factor Analysis

An Investigative Study on the Chemical, Morphological and Mineralogical Alterations of Dry Disposed Fly Ash During Sequential Chemical Extraction

The hazardous elements associated with various physicochemical forms in coal fly ash are of environmental concern due to their leaching potential and subsequent contamination of surface and groundwater in the vicinity of the ash dump. Selective sequential extraction was performed on dry disposed fly ash samples from a coal-fired power station in Mpumalanga province, South Africa. The alteration of the chemical, morphological and mineralogical species of weathered fly ash during the selective sequential extraction was investigated using X-ray fluorescence (XRF), Nano-scan electron microscopy (NANOSEM) and X-ray powder diffraction (XRD). Insoluble residue from the water-soluble fraction is composed of amorphous alumino-silicate. The residues from exchangeable carbonate and Fe and Mn fractions consisted mostly of amorphous alumino-silicate spheres with a lesser quantity of iron-rich spheres. The iron-rich spheres are surrounded by amorphous alumino-silicate spheres.  The leaching behavior of trace metals (such as Ce, Y, Nb, Rb, U, and Tl) in weathered dry disposed fly ash was considered to have a dependency relationship with the components of SiO2, CaO, MgO, P2O5, and amount of unburned carbon. The decrease in the quantities of calcite with successive extraction could be considered as a marker of progress of sequential extraction technique. At the same time, the increase in the quantities of quartz could be also considered as an indicator of progress of the sequential extraction scheme. Trace elements bound to exchangeable or carbonate fraction during sequential chemical extraction were found associated with calcite. The elemental concentrations, as determined by electron dispersive x-ray spectroscopy (EDS), were consistent with XRF and XRD data. Therefore, the chemical extractant used in this study proved efficient for extraction of inorganic metals associated with various physicochemical forms in weathered fly ash.Key words: Coal fly ash; Selective sequential extraction; Major components; Trace elements; Morphology; Mineralogical compositio

Laboratory study on the mobility of major species in fly ash–brine co-disposal systems: up-flow percolation test

Apart from the generation of fly ash, brine (hyper-saline wastewater) is also a waste material generated in South African power stations as a result of water re-use. These waste materials contain major species such as Al, Si, Na, K, Ca, Mg, Cl and SO4. The co-disposal of fly ash and brine has been practiced by some power stations in South Africa with the aim of utilizing the fly ash to capture the salts in brine. The effect of the chemical interaction of the species contained in both fly ash and brine, when co-disposed, on the mobility of species in the fly ash–brine systems is the focus of this study. The up-flow percolation test was employed to determine the mobility of some major species in the fly ash–brine systems. The results of the analysed eluates from the up-flow percolation tests revealed that some species such as Al, Ca and Na were leached from the fly ash into the brine solution while some species such as Mg, Cl and SO4 were removed to some extent from the brine solution during the interaction with fly ash. The pH of the up-flow percolation systems was observed to play a significant role on the mobility of major species from the fly ash–brine systems. The study showed that some major species such as Mg, Cl and SO4 could be removed from brine solution using fly ash when certain amount of brine percolates through the ash.Web of Scienc