Insights into the mechanism of low-temperature H2S oxidation over Zn-Cu/Al2O3 catalyst

Abstract

Odor pollution caused by toxic chemicals with low human olfactory thresholds, such as hydrogen sulfide (H₂S), has become a major cause of environmental grievance world-wide. Although the low-temperature (<180 °C) catalytic oxidation of H₂S using metal oxides has received widespread attention, desulfurization performance is not ideal. Herein, a series of Zn-Cu/Al₂O₃ catalysts were developed using an impregnation method based on the Al₂O₃ hydrophilicity and the effects of zinc loading on the catalyst physicochemical properties and performance were systematically studied. The catalysts were characterized using inductively coupled plasma-optical emission spectrometry (ICP-OES), N₂ adsorption-desorption isotherms, scanning electron microscopy with energy dispersive spectrometry (SEM-EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared spectroscopy (FTIR) and electron paramagnetic resonance (EPR). It was found that optimization of zinc doping could improve the hydrophilicity of the catalyst, and hence its activity. Catalytic activity was also dependent on operational parameters such as temperature, humidity and space velocity. The Zn₃Cu₃ catalyst exhibited the highest breakthrough capacity of 353.91 mg/g at 50 °C and at a relative humidity of 50%. The excellent desulfurization performance was attributed to oxygen vacancies contributed by CuO, Cu₂O and ZnO, which facilitated the conversion of H₂O into hydroxyl radicals. Consequently, a hydroxyl radical-induced desulfurization mechanism over Zn-Cu/Al₂O₃ is proposed. This work provides a potential green and efficient catalyst for the selective oxidation of H₂S.

Keywords: Catalytic oxidation; Desulfurization mechanism; Hydrogen sulfide; Zn–Cu/Al(2)O(3).