Regeneration of sulfur-poisoned Pd-based catalyst for natural gas oxidation

Mari Honkanen*, Jianguang Wang, Marja Kärkkäinen, Mika Huuhtanen, Hua Jiang, Kauko Kallinen, Riitta L. Keiski, Jaakko Akola, Minnamari Vippola

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

13 Citations (Scopus)

Abstract

Sulfur deactivation and regeneration behavior of the Pd/Al2O3 catalyst has been investigated via experimental characterization and density functional theory (DFT) simulations. During the sulfur exposure, PdO crystallites grow slightly while bulk Al2(SO4)3 forms on the support. DFT calculations indicate that SOx species interact strongly with the catalyst surface making it chemically inactive in agreement with the experimental results. During the regeneration treatment (CH4 conditions), PdO particles reduce, Al2(SO4)3 is partially removed, and the activity for CH4 conversion is increased. No full recovery can be observed due to remaining Al2(SO4)3, the formation of encapsulating sulfur species, and the partial reduction of PdO particles. To reoxidize Pd, the catalyst is further regenerated (O2 conditions). The resulting CH4 conversion is at the same level than with the regenerated catalyst. Thus, a small amount of Al2(SO4)3 appears to have a stronger effect on the performance than the state of Pd.

Original languageEnglish
Pages (from-to)253-265
Number of pages13
JournalJournal of Catalysis
Volume358
DOIs
Publication statusPublished - 1 Feb 2018
MoE publication typeA1 Journal article-refereed

Keywords

  • Catalytic testing
  • Density functional theory simulations
  • Fourier transform infrared spectrometry
  • Pd-based catalyst
  • Regeneration
  • Sulfur poisoning
  • Transmission electron microscopy

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    Honkanen, M., Wang, J., Kärkkäinen, M., Huuhtanen, M., Jiang, H., Kallinen, K., ... Vippola, M. (2018). Regeneration of sulfur-poisoned Pd-based catalyst for natural gas oxidation. Journal of Catalysis, 358, 253-265. https://doi.org/10.1016/j.jcat.2017.12.021