Unraveling the mysterious failure of Cu/SAPO-34 selective catalytic reduction catalysts

Aiyong Wang, Ying Chen, Eric D. Walter (), Nancy M. Washton, Donghai Mei (), Tamas Varga, Yilin Wang, János Szanyi, Yong Wang, Charles H. F. Peden and Feng Gao ()
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Aiyong Wang: Institute for Integrated Catalysis, Pacific Northwest National Laboratory
Ying Chen: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory
Eric D. Walter: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory
Nancy M. Washton: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory
Donghai Mei: Institute for Integrated Catalysis, Pacific Northwest National Laboratory
Tamas Varga: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory
Yilin Wang: Institute for Integrated Catalysis, Pacific Northwest National Laboratory
János Szanyi: Institute for Integrated Catalysis, Pacific Northwest National Laboratory
Yong Wang: Institute for Integrated Catalysis, Pacific Northwest National Laboratory
Charles H. F. Peden: Institute for Integrated Catalysis, Pacific Northwest National Laboratory
Feng Gao: Institute for Integrated Catalysis, Pacific Northwest National Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract 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.

Date: 2019
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DOI: 10.1038/s41467-019-09021-3

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