Immobilization of Boron and Arsenic in Alkaline Coal Fly Ash through an Aging Process with Water and Elucidation of the Immobilization Mechanism

We previously reported that a simple treatment—addition of only small amounts of water to coal fly ash (CFA) to form CFA paste followed by aging for 1–4 weeks—is advantageous for the immobilization of highly soluble B, F, Cr, and As. In this study, we investigated the leachability of Ca, SO4, B, and As over time from non-aged and aged CFA samples to elucidate a possible immobilization mechanism. For this purpose, two types of CFA samples, one showing effective immobilization of B and As by water addition and aging (sample A) and the other showing less or no immobilization (sample B), were examined. Calcium and SO4, B, and As in non-aged sample A dissolved immediately after the start of the leaching test, indicating that these elements existed in highly soluble particles. After the rapid dissolution, their concentrations in the leachate gradually increased, possibly due to the dissolution of glassy phases. During the 1-week leaching test, the B and As concentrations in the leachate finally decreased. The addition of only small amounts of water to CFA (Sample A) for aging produce both alkaline and supersaturation conditions for the formation of several types of Ca-bearing secondary minerals such as calcite and ettringite, which are formed under alkaline conditions. Boron and As originally existing as highly soluble particles in CFA are expected to be incorporated into and/or sorbed on these secondary minerals as water-insoluble phases. Compared to non-aged CFA, their leachability from the aged sample A remained lower throughout the entire leaching test. Possibly due to these secondary minerals being formed on the CFA surface, B and As dissolutions associated with glassy phases are also prevented. In contrast, the pH of the leachate from CFA (sample B) at the beginning of the leaching test was acidic and then abruptly became alkaline. This means that water-soluble particles that can produce acidic conditions are also contained in these alkaline CFAs. Dissolution of these substances during aging makes it difficult to generate alkaline conditions in the CFA paste. Consequently, the formation of secondary minerals and the concomitant immobilization of toxic elements are prevented.