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Deactivation of Cu‐Exchanged Automotive‐Emission NH 3 ‐SCR Catalysts Elucidated with Nanoscale Resolution Using Scanning Transmission X‐ray Microscopy
Author(s) -
Ye Xinwei,
Schmidt Joel E.,
Wang RuPan,
Ravenhorst Ilse K.,
Oord Ramon,
Chen Tiehong,
Groot Frank,
Meirer Florian,
Weckhuysen Bert M.
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201916554
Subject(s) - xanes , catalysis , chemistry , nanoscopic scale , copper , absorption (acoustics) , selective catalytic reduction , brønsted–lowry acid–base theory , analytical chemistry (journal) , crystallography , inorganic chemistry , materials science , spectroscopy , nanotechnology , organic chemistry , physics , quantum mechanics , composite material
To gain insight into the underlying mechanisms of catalyst durability for the selective catalytic reduction (SCR) of NO x with an ammonia reductant, we employed scanning transmission X‐ray microscopy (STXM) to study Cu‐exchanged zeolites with the CHA and MFI framework structures before and after simulated 135 000‐mile aging. X‐ray absorption near‐edge structure (XANES) measurements were performed at the Al K‐ and Cu L‐edges. The local environment of framework Al, the oxidation state of Cu, and geometric changes were analyzed, showing a multi‐factor‐induced catalytic deactivation. In Cu‐exchanged MFI, a transformation of Cu II to Cu I and Cu x O y was observed. We also found a spatial correlation between extra‐framework Al and deactivated Cu species near the surface of the zeolite as well as a weak positive correlation between the amount of Cu I and tri‐coordinated Al. By inspecting both Al and Cu in fresh and aged Cu‐exchanged zeolites, we conclude that the importance of the preservation of isolated Cu II sites trumps that of Brønsted acid sites for NH 3 ‐SCR activity.