Nitrogen-doped carbon nanotubes decorated silicon carbide as a metal-free catalyst for partial oxidation of H2S

• Synthesis of N-CNTs/SiC composite with controlled macroscopic shape.
• High effective surface area and low diffusion pathway.
• Metal-free catalyst for the partial oxidation of H2S into elemental sulfur.
• High activity and stability as a function of time on stream.

Hierarchical metal-free catalyst based on the CVD synthesis of nitrogen-doped carbon nanotubes decorated silicon carbide (N-CNTs/SiC) macroscopic host structure has been prepared. The catalyst was evaluated in the partial oxidation of H2S by oxygen into elemental sulfur in a fixed-bed reactor. The catalytic results indicate that the N-CNTs/SiC catalyst exhibits an extremely high desulfurization performance even under severe reaction conditions such as low temperature, high space velocity and at low O2-to-H2S molar ratio. The high desulfurization performance was attributed to the high effective surface area of the catalyst along with a short diffusion length associated with the nanoscopic dimension of the carbon nanotubes. The N-CNTs/SiC catalyst also displays a high stability as a function of time on stream which could be attributed to the strong anchoring of the nitrogen doping within the carbon matrix. The extrudates shape of the SiC support allows the direct macroscopic shaping of the catalyst for use in conventional fixed-bed reactor without facing problems linked with catalyst handling, transportation and pressure drop across the catalyst bed as encountered with nanoscopic carbon-based catalyst.

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