Modification of iron-containing silicate tailings with oxalic acid to develop a long-efficacy utilization peroxymonosulfate-based system for the efficient decomplexation and removal of Cr(III)-ethylenediamine tetraacetic acid.

Ferrous oxalate (FeCO)-based composite has been recognized as an eminent catalyst for Cr(III)-ethylenediamine tetraacetic acid (Cr(III)-EDTA) decomplexation. However, their practical application has been limited by low cycling capacity and an ambiguous mechanism. In this research, a composite catalyst consisting of biotite loaded with nano FeCO (CFS90) was prepared directly from iron-containing silicate tailing. The removal efficiency (91.3 %, k = 0.0185 min) of Cr(III)-EDTA by CFS90/peroxymonosulfate (PMS) system was remarkably higher than that of other typical systems. The Si site in biotite lost electrons while the electron cloud density around the Fe atom in FeCO increased, which facilitates the activation of PMS and the generation of reactive oxygen species (ROS). In this system, abundant singlet oxygen (O) was primarily produced via interactions between carbon-centered radicals (CO) and dissolved oxygen (DO), rather than through oxygen vacancies (Ovs) in CFS90. Both CO and Fe(II) provided reducing conditions, preventing the released Cr(III) from being re-oxidized. Notably, the released Cr(III) was effectively precipitated by elevating the solution pH with NaOH, therefore endowing superior stability and deactivation capacity of CFS90 to enable its removal rate of Cr(III)-EDTA to remain above 84.1 % for 18 h in a fix-bed reactor. These findings provide an in-depth analysis of the enhanced Cr(III)-EDTA removal mechanism and highlight the environmental remediation potential of iron-containing silicate tailings.