H2O2 activation over Co substitution in Fe1-xS for tetracycline degradation: Effect of Co substitution

Abstract

In this work, the effect of Co substitution in the Fe_1-xS (CSP) on the activation of H₂O₂ to degrade tetracycline (TC) is investigated. A series of CSP samples with different Co content are synthesized via a high-temperature sulfidation method and characterized by XRD, XPS, SEM, and electrochemical analysis. The result showed that low Co content (≤1%) promotes the catalytic activity of Fe_1-xS, while excessive Co (1%﹤x ≤ 3%) inhibits its catalytic activity. The investigation of Behnajady-Modirshahla-Ghanbery kinetic model (BMG) showed that the maximum initial degradation rate of TC over 1.0% CSP/H₂O₂ was 1.6 times than that of in CSP/H₂O₂ system. The Box-Behnken with Response Surface Methodology was employed to verify optimum condition for TC degradation. The quenching experiments and ESR determined that ·OH, ·O₂^- and ¹O₂ were involved in TC degradation with the treatment of 1.0% CSP/H₂O₂ system. Electrochemical analysis, ·OH quantification, and metal ion concentrations measure reveal that Co substitution accelerates electron transfer efficiency and Fe²⁺ regeneration. Furthermore, nine intermediates are identified and the possible degradation pathway of TC is proposed. The unique effect of Co provides novel insight and efficient strategies for improving the reactivity of iron sulfide.

Keywords: Cobalt-substitution; Degradation; Fe(1-x)S; Mechanism; Pathway; Tetracycline.