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Article Dans Une Revue Applied Catalysis B: Environmental Année : 2020

Effect of rh in ni-based catalysts on sulfur impurities during methane reforming

Stavros-Alexandros Theofanidis
  • Fonction : Auteur
Johannis A. Z. Pieterse
  • Fonction : Auteur
Hilde Poelman
  • Fonction : Auteur
Alessandro Longo
  • Fonction : Auteur
Maarten K. Sabbe
  • Fonction : Auteur
Christophe Detavernier
  • Fonction : Auteur
Guy B. Marin
  • Fonction : Auteur
Vladimir V. Galvita
  • Fonction : Auteur

Résumé

The addition of Rh, in low concentrations (<1 wt%), to Ni-based catalysts was investigated during steam-dry reforming of a gas mixture, which simulates the effluent of a biomass gasifier, after removal of tar compounds, but in presence of H2S at ppm level. Four Ni-Rh catalysts supported on MgAl2O4, with Ni:Rh molar ratio varying from 18 to 82, were characterized using N2-BET, Inductively Coupled Plasma Atomic Emission Spectroscopy and X-ray Diffraction, while the evolution of the catalyst structure during temperature program reduction and oxidation was examined using time-resolved in-situ XRD. During reduction of the Ni-Rh catalyst, two types of Ni-Rh alloy were formed. The Rh-rich Ni alloy remained stable up to 1123 K under CO2 oxidation. The catalyst with a Ni:Rh molar ratio of 41 showed the best performance in terms of both activity and stability, in presence of 7 ppm H2S as a contaminant, at 1173 K and total pressure of 111.3 kPa, reaching 0.24 molCH4·s−1 ·kgmetals−1 after 42.5 h time-on-stream. Regeneration of the catalysts was performed by removing H2S from the feed stream. The catalyst regeneration ability depended on the formation of a Ni-Rh alloy and hence on the Ni:Rh molar ratio. According to density functional theory calculations on the adsorption and dissociation of H2S on Ni and NiRh (111) surfaces, the Ni-Rh alloy inhibited H2S decomposition in contrast to monometallic Ni.

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Catalyse
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Dates et versions

hal-04552136 , version 1 (19-04-2024)

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Citer

Stavros-Alexandros Theofanidis, Johannis A. Z. Pieterse, Hilde Poelman, Alessandro Longo, Maarten K. Sabbe, et al.. Effect of rh in ni-based catalysts on sulfur impurities during methane reforming. Applied Catalysis B: Environmental, 2020, Applied catalysis. B, Environmental, 267, pp.118691. ⟨10.1016/j.apcatb.2020.118691⟩. ⟨hal-04552136⟩
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