Composite materials based on diatomite (DT) with the addition of biochar (BC), dolomite (DL), and bentonite (BN) were developed. The effect of chemical modification on the chemical structure of the resulting composites was investigated, and their influence on heavy metal immobilization and the ecotoxicity of post-flotation sediments was evaluated. It was demonstrated that the chemical modifications resulted in notable alterations to the chemical properties of the composites compared to pure DT and mixtures of DT with BC, DL, and BN. An increase in negative charge was observed in all variants. The addition of BC introduced valuable chemically and thermally resistant organic components into the composite. Among the chemical modifications, composites with the addition of perlite exhibited the lowest values of negative surface charge, which was attributed to the dissolution and transformation of silicon compounds and traces of kaolinite during their initial etching with sodium hydroxide. The materials exhibited varying efficiencies in metal immobilization, which is determined by both the type of DT additive and the type of chemical modification applied. The greatest efficacy in reducing the mobility of heavy metals was observed in the PFS with the addition of DT and BC without modification and with the addition of DT and BC after the modification of H2SO4 and H2O2: Cd 8% and 6%; Cr 71% and 69%; Cu 12% and 14%; Ni 10% and Zn 15%; and 4% and 5%. In addition, for Zn and Pb, good efficacy in reducing the content of mobile forms of these elements was observed for DT and DL without appropriate modification: 4% and 20%. The highest reduction in ecotoxicity was observed in the PFS with the addition of DT and BC, followed by BN and DL, which demonstrated comparable efficacy to materials with DT and BN.
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