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Sulfur Poisoning and Regeneration Behavior of Perovskite-Based NO Oxidation Catalysts

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Abstract

SO x uptake and release properties of LaMnO3, Pd/LaMnO3, LaCoO3 and Pd/LaCoO3 perovskites were investigated via in situ Fourier transform infrared (FTIR) spectroscopy, temperature programmed desorption and X-ray photoelectron spectroscopy. Sulfation of the perovskite leads to the formation of surface sulfite/sulfate and bulk-like sulfate species. Pd addition to LaMnO3 and LaCoO3 significantly increases the sulfur adsorption capacity. Pd/LaMnO3 sample accumulates significantly more sulfur than LaMnO3; however it can also release a larger fraction of the accumulated SO x species in a reversible fashion at elevated temperatures in vacuum. This is not the case for Co-based materials, where thermal regeneration of bulk sulfates on poisoned LaCoO3 and Pd/LaCoO3 is extremely ineffective under similar conditions. However, in the presence of an external reducing agent such as H2 (g), Pd/LaMnO3 requires much lower temperature (873 K) for complete sulfur regeneration as compared to that of Pd/LaCoO3 (973 K). Sequential CO and SO x adsorption experiments performed via in situ FTIR indicate that in the presence of carbonyls and/or carbonates, Pd adsorption sites may have a stronger affinity for SO x as compared to that of the perovskite surface, particularly in the early stages of sulfur poisoning.

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Acknowledgments

The authors acknowledge the financial support from the Scientific and Technical Research Council of Turkey (TUBITAK) (Project Code: 213M585 and TUBITAK 2221 Fellowship Program). Authors also acknowledge the scientific collaboration with TARLA project founded by the Ministry of Development of Turkey under grant no DPT2006K–120470.

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Correspondence to Emrah Ozensoy.

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Kurt, M., Say, Z., Ercan, K.E. et al. Sulfur Poisoning and Regeneration Behavior of Perovskite-Based NO Oxidation Catalysts. Top Catal 60, 40–51 (2017). https://doi.org/10.1007/s11244-016-0721-9

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Keywords

  • LaCoO3
  • LaMnO3
  • Pd
  • FTIR
  • DeNO x
  • LNT