Enhancing Mo leaching efficiency from spent catalyst via Fenton-like oxidation process: A comprehensive investigation of leaching effects, mechanism and environmental impacts

Abstract

Spent hydrodesulfurization (HDS) catalyst contains considerable amounts of Mo, Ni and V, is an important secondary resource for these valuable metals. Direct acid solution leaching method exhibits poor separation effect from catalyst carrier for Mo due to greater stability of MoS2. This study explored Mo leaching efficiencies from spent HDS catalyst by Fenton-like oxidation systems (H2O2 and K2S2O8), which were frequently employed in the wastewater treatment. To further improve Mo leaching efficiency, nano zero-valent iron (nZVFe) was used to activate H2O2/K2S2O8 and produce more free radicals (·OH and ·SO4-). Approximate 96.0 % and 93.3 % of Mo were leached from spent HDS catalyst in nZVFe + H2O2 + H2SO4 and nZVFe + K2S2O8 + H2SO4 systems under optimal experimental conditions, increased by 16.2 % and 8.2 % than normal H2O2 (79.8 %) and K2S2O8 (85.1 %) system without nZVFe. The leaching process of Mo in both nZVFe + H2O2 + H2SO4 and nZVFe + K2S2O8 + H2SO4 systems conformed to the shrinkage core model. Kinetic analysis and molecular calculation demonstrated the leaching process of Mo in nZVFe + H2O2 + H2SO4 system was driven by chemical reaction and solid film diffusion, and the leaching and oxidation reactions of MoS2 occurred simultaneously. However, the leaching process of Mo in nZVFe + K2S2O8 + H2SO4 system was driven only by chemical reaction, solid MoS2 was firstly dissolved into Mo4+ by H+, and then oxidized into Mo6+ by ·SO4-. The economic and environmental impacts evaluation indicated that the separation of Mo from spent HDS catalysts by nZVFe + H2O2 + H2SO4 was assigned as a better choice than normal H2O2 and K2S2O8 system without nZVFe due to higher leaching efficiency and lower cost.