A comparative study between real-world and laboratory accelerated aging of Cu/SSZ-13 SCR catalysts

Yiqing Wu, Tahrizi Andana, Yilin Wang, Ying Chen, Eric D. Walter, Mark H. Engelhard, Kenneth G. Rappé, Yong Wang, Feng Gao, Unmesh Menon, Rohil Daya, Dylan Trandal, Hongmei An, Yuhui Zha, Krishna Kamasamudram

Research output: Contribution to journalArticlepeer-review

18 Scopus citations

Abstract

Elucidating aging mechanisms in real-world applications is a critical component for developing and maintaining Cu/SSZ-13 SCR catalysts. To reveal gaps between laboratory accelerated aging and real-world aging, herein we report thorough comparative studies between 6 representative catalysts. We apply a wide range of catalyst characterization methods to gain atomic-level knowledge on Cu transformation under different aging protocols, including surface area/porosity analysis, X-ray diffraction (XRD), H2-temperature programmed reduction, NH3-temperaure programmed desorption, solid-state nuclear magnetic resonance (NMR), in situ X-ray photoelectron (XPS) and electron paramagnetic resonance (EPR) spectroscopies. We then correlate such knowledge to SCR, NH3/NO oxidation kinetic behavior of the catalysts. We found that sulfur aging plays the most important role in interpreting catalyst degradation during real-world application, including direct sulfur poisoning of isolated CuII SCR active species to CuSO4-like species, the agglomeration of such species to multinuclear CuSO4 clusters, and eventually, CuO formation during desulfation treatments. Such chemistries convert SCR active Cu to SCR inert Cu moieties without severely deteriorating catalyst support integrity. These characteristics are partially replicated by hydrothermal aging in the presence of SOx but are poorly mimicked by hydrothermal aging alone.

Original languageEnglish
Article number121807
JournalApplied Catalysis B: Environmental
Volume318
DOIs
StatePublished - Dec 5 2022
Externally publishedYes

Keywords

  • Catalyst deactivation
  • Cu/SSZ-13
  • DeNOx
  • In situ spectroscopy
  • SCR

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