Remediation of fluoride-contaminated wastes: Chelator-assisted washing and subsequent immobilization using CaO and H3PO4

Fluoride (F) contamination in industrial waste is a significant challenge for sustainable materials recycling. Existing techniques for mitigating F contamination focus on immobilization, converting F compounds to insoluble forms while leaving the total F content untreated. Chelator-assisted washing is considered a promising alternative remediation strategy that can indirectly release F by entrapping and dissolving F-bearing minerals. This study evaluates the effectiveness of chelator-assisted washing in removing F from three real F-contaminated waste samples (TCS-49, TCS-51, and TCS-52) by treating with four different chelators, ethylenediaminetetraacetic acid (EDTA), ethylenediamine N,N′-disuccinic acid (EDDS), diethylenetriaminepentaacetic acid (DTPA), and 3-hydroxy-2,2′-imino disuccinic acid (HIDS). The influence of key washing variables, including chelator type, solution pH, chelator concentration, washing time, and liquid-to-solid (L/S) ratio toward F extraction was assessed and optimized for attaining the maximum extraction. All chelators exhibited the highest F extraction from TCS-49 and TCS-51 at pH 11, whereas in TCS-52 it showed a discrete extraction pattern. Under optimized conditions (concentration, 10 mmol L−1; pH, 11; washing duration, 3 h; and L/S ratio, 10:1), EDTA outperformed the other chelators, enhancing F extraction by 2.1 and 1.2 times for TCS-49 and TCS-51, respectively, compared with those of control treatments. However, for TCS-52, the efficiency of EDTA was analogous to that of the control under the same washing conditions. The linear correlation between the extracted F and F-containing minerals suggests that the chelator-induced F removal from contaminated waste involves the entrapment and dissolution of F-bearing minerals, especially Ca and Fe. The subsequent post-washing immobilization of chelator-washed waste residues using CaO or H3PO4 significantly reduced the content of leachable F under the regulatory limit. © 2024 Elsevier Ltd