Valorization of Silicon-Rich Solid Waste into Highly Active Silicate Adsorbents for Heavy Metal Removal.

Abstract

Waste stone powder is a major solid waste byproduct of stone operations. This study developed a novel "alkali activation-calcination" process that efficiently converts waste stone powder into high-value-added silicon-based materials (SSM). This study elucidated the morphological evolution of silicon during the conversion process and revealed the formation mechanism of active silicon. Through further integration of batch adsorption experiments and multi-technique characterization analysis, the immobilization efficacy of this material for heavy metals cadmium/lead was elucidated, revealing both direct and indirect interfacial reaction mechanisms. The results demonstrate that in-creasing the calcination temperature, alkali activator concentration, and calcination duration enhances the reactive silica content in SSM. NaOH as activator, the calcination process significantly reduces both the thermal decomposition temperature of raw materials and the initial temperature required for silicon conversion. Under optimized conditions (WG:MD:activator = 1:0.8:0.32, temperature = 800 °C, time = 1 h), the reactive silica content reached 24.30%. The generation rate of reactive silica is governed by the combined effects of interfacial chemical reactions and solid-phase product layer diffusion. Under idealized laboratory conditions, the maximum adsorption capacities (Qm) of SSM were determined to be 57.40 mg/g for cadmium and 496 mg/g for lead, which are significantly higher than those of many other adsorbents. Continuous desorption experiments and characterization analyses confirm that Cd and Pb adsorption by SSM is primarily driven by electro-static interactions, complexation, precipitation, and coordination, while ion ex-change plays a secondary role. Highly reactive silica facilitates interactions between Cd/Pb and oxygen-containing functional groups (e.g., -OH, ≡Si-OH, Si-O-Si), promoting precipitate formation for effective heavy metal removal. This work offers theoretical guidance for valorizing silica-rich waste rock powder. It is important to note, however, that while the adsorption capacity of SSM is encouraging, its practical implementation requires resolving key issues identified during the lab-to-application transition.