Evaluation of iron-loaded granular activated carbon used as heterogeneous fenton catalyst for degradation of tetracycline

Abstract

To optimize the efficiency of general adsorption-Fenton oxidation treatment, iron-loaded granular activated carbon (Fe-GAC) was prepared, characterized, and used as a catalyst in the heterogeneous Fenton oxidation of tetracycline (TC). Characterization revealed that the Fe(II) was successfully introduced onto the original granular activated carbon (GAC) and diversified the materials’ surface morphology and elemental compounds. Under an initial pH of 3.0, the Fe-GAC/Fenton system obtained a maximum removal rate of 92.6%, with hydrogen peroxide (H2O2) dosages of 9 mmol g−1. And the GAC/Fenton without iron supplementation was 89.5%, with H2O2 dosages of 8 mmol g−1. Additionally, the Fe-GAC/Fenton system consumed a lower Fe(II) dosage than GAC/Fenton, with Fe(II)/H2O2 molar ratios of 0.007:1 and 0.04:1, respectively. Analysis of total organic carbon demonstrated higher mineralization efficiency in the Fe-GAC/Fenton system (67.2%), which was approximately 1.3 times of GAC/Fenton. Desorption experiments showed that the adsorption and degradation accounted for 19.22% and 80.78% of the total TC removal by GAC/Fenton, and 10.58% and 89.42% in the Fe-GAC/Fenton system, respectively. Electron paramagnetic resonance (EPR) technique and quenching experiments demonstrated that the dominant reactive oxygen species (ROS) in synergistic treatments were hydroxyl (•OH) and hydroxy peroxyl (HO2•) radicals. In addition, three potential degradation pathways for TC were proposed according to the detected fourteen intermediates. Catalyst regeneration treatments were evaluated over six cycles, and the regeneration was 6.5% higher with the iron-supplemented carbon granules. Overall, the Fe-GAC can be used as an efficient catalyst in practical water treatment, and this study demonstrated a promising method to develop adsorption-Fenton technology.