Detoxification-Oriented Carbonate Leaching of Selenium and Tellurium from Lead-Rich Fly Ash: Experimental and Kinetic Analysis

Copper anodic slime is often smelted with lead to improve silver and gold recovery, generating a fine lead-rich fly ash that contains notable amounts of selenium and tellurium. Due to its high lead content and sub-micron particle size, this residue poses significant environmental and occupational health risks. This study evaluates sodium carbonate (Na2CO3) leaching as an environmentally benign pre-treatment aimed at partially removing selenium and tellurium while stabilizing lead through carbonate formation. The goal is detoxification rather than maximum metal recovery, enabling safer disposal or subsequent recycling. A central composite design (CCD) in Design-Expert software (Version 12) was used to assess the effects of Na2CO3 concentration, temperature, solid-to-liquid ratio, and time on selenium and tellurium dissolution. Selenium recovery reached up to 53.9%, while tellurium recovery peaked at approximately 33.9%. Scanning electron microscopy showed the dust to consist mainly of semi-spherical and elongated particles, with lead carbonate forming preferentially on particle surfaces during leaching. Energy-dispersive spectroscopy confirmed conversion of lead sulfate phases to lead carbonate, which increasingly restricted selenium and tellurium dissolution. Kinetic evaluation suggested selenium leaching follows mixed control involving both surface reaction and diffusion through product layers, whereas tellurium dissolution lacked consistent kinetic behavior. Thermodynamic calculations supported the stabilization of lead as cerussite (PbCO3), indicating improved environmental safety. The overall dissolution trends were successfully represented using an apparent Shrinking Core Model (SCM) based on measurements collected at 20 °C, 60 °C, and 100 °C.