TY - JOUR
T1 - A comparative study between real-world and laboratory accelerated aging of Cu/SSZ-13 SCR catalysts
AU - Wu, Yiqing
AU - Andana, Tahrizi
AU - Wang, Yilin
AU - Chen, Ying
AU - Walter, Eric D.
AU - Engelhard, Mark H.
AU - Rappé, Kenneth G.
AU - Wang, Yong
AU - Gao, Feng
AU - Menon, Unmesh
AU - Daya, Rohil
AU - Trandal, Dylan
AU - An, Hongmei
AU - Zha, Yuhui
AU - Kamasamudram, Krishna
N1 - Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/12/5
Y1 - 2022/12/5
N2 - 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.
AB - 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.
KW - Catalyst deactivation
KW - Cu/SSZ-13
KW - DeNOx
KW - In situ spectroscopy
KW - SCR
UR - http://www.scopus.com/inward/record.url?scp=85135869639&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2022.121807
DO - 10.1016/j.apcatb.2022.121807
M3 - Article
AN - SCOPUS:85135869639
SN - 0926-3373
VL - 318
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 121807
ER -