Controlling the Fe2O3-SiO2 interaction: The effect on the H2S selective catalytic oxidation and catalyst deactivation

Environ Res. 2022 Dec;215(Pt 2):114354. doi: 10.1016/j.envres.2022.114354. Epub 2022 Sep 17.

Abstract

Biogas utilization is one of the most promising options for reducing the consumption of fossil fuels for energy production, but the presence of H2S represents a serious industrial and environmental problem. In this work, two different synthesis methods (sol-gel and incipient wetness impregnation) were used to synthesize iron oxide supported on silica catalysts (Fe2O3/SiO2) with metal loadings ranging from 0.5 to 10 %wt. The catalysts were tested for the selective oxidation of H2S, changing the operating conditions like O2/H2S (0.5-2.5), temperature (170-250°C), and water content (0-50%). The optimum condition was O2/H2S = 0.5 and no water at 230 °C with the conversion of approximately 100%, the selectivity of 97%, and the deactivation of 0.6%. A detailed characterization of the fresh and spent catalysts' surface revealed the presence of four deactivation mechanisms: metal surface reduction, oxygen vacancy loss, pore plugging, and sintering. Among the observed deactivation mechanisms, the sintering showed the highest impact on catalytic activity and deactivation. The sol-gel catalysts (SG) showed the highest metal-oxide/support interaction, which reduced the metal-oxide nanoparticles sintering compared with the incipient wetness impregnation method (IWI), reporting a lower sintering, higher activity, and selectivity, lower deactivation rates and lower sensitivity to the operating conditions. A catalytic cycle representing the possible surface intermediate states of the catalyst is proposed based on the performance and characterization results obtained.

Keywords: Deactivation; H(2)S selective Oxidation; Metal-oxide/support interaction; Nanoparticles sintering; Sol-gel.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Biofuels*
  • Fossil Fuels
  • Metals
  • Oxides
  • Oxygen
  • Silicon Dioxide*

Substances

  • Biofuels
  • Fossil Fuels
  • Metals
  • Oxides
  • Silicon Dioxide
  • Oxygen