Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/s41467-019-09021-3
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- US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Office
- DOE's Office of Biological and Environmental Research
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Commercial Cu/SAPO-34 selective catalytic reduction (SCR) catalysts have experienced unexpected and quite perplexing failure. Understanding the causes at an atomic level is vital for the synthesis of more robust Cu/SAPO-34 catalysts. Here we show, via application of model catalysts with homogeneously dispersed isolated Cu ions, that Cu transformations resulting from low-temperature hydrothermal aging and ambient temperature storage can be semi-quantitatively probed with 2-dimensional pulsed electron paramagnetic resonance. Coupled with kinetics, additional material characterizations and DFT simulations, we propose the following catalyst deactivation steps: (1) detachment of Cu(II) ions from cationic positions in the form of Cu(OH) 2; (2) irreversible hydrolysis of the SAPO-34 framework forming terminal Al species; and (3) interaction between Cu(OH) 2 and terminal Al species forming SCR inactive, Cu-aluminate like species. Especially significant is that these reactions are greatly facilitated by condensed water molecules under wet ambient conditions, causing low temperature failure of the commercial Cu/SAPO-34 catalysts.
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