Elucidating the Effect of Ion Exchange Protocol on the Copper Exchange Efficacy, Copper Siting, and SCR activity in Cu‐SSZ‐13

Author:

Koishybay Aibolat1,Umhey Charles2,Kuo Chun‐Te3,Groden Kyle2,McEwen Jean‐Sabin24567,Karim Ayman M.3,Shantz Daniel F.1

Affiliation:

1. Department of Chemical and Biomolecular Engineering Tulane University 6823 St. Charles Avenue New Orleans LA 70118 USA

2. The Gene and Linda Voiland School of Chemical Engineering and Bioengineering Washington State University Pullman WA 99164 USA

3. Department of Chemical Engineering Virginia Polytechnic Institute and State University Blacksburg VA 24061 USA

4. Department of Physics and Astronomy Washington State University Pullman WA 99164 USA

5. Department of Chemistry Washington State University Pullman WA 99163 USA

6. Department of Biological Systems Engineering Washington State University Pullman 99164 USA

7. Institute for Integrated Catalysis Pacific Northwest National Laboratory Richland WA 99354 USA

Abstract

AbstractThe influence of the copper ion exchange protocol on SCR activity of SSZ‐13 is quantified. Using the same parent SSZ‐13 zeolite, four exchange protocols are used to assess how exchange protocol impacts metal uptake and SCR activity. Large differences in the SCR activity, nearly 30 percentage points at 160 °C at constant copper content, are observed for different exchange protocols implying that different exchange protocols lead to different copper species. Hydrogen temperature programmed reduction on selected samples and infrared spectroscopy of CO binding corroborates this conclusion as the reactivity at 160 °C correlates with the intensity of the IR band at 2162 cm−1. DFT‐based calculations show that such an IR assignment is consistent with CO adsorbed on a Cu(I) cation within an eight‐membered ring. This work shows that SCR activity can be influenced by the ion exchange process even when different protocols lead to the same metal loading. Perhaps most interesting, a protocol used to generate Cu‐MOR for methane to methanol studies led to the most active catalyst both on a unit mass or unit mole copper basis. This points to a yet not recognized means to tailor catalyst activity as the open literature is silent on this issue.

Funder

American Chemical Society Petroleum Research Fund

National Science Foundation

Publisher

Wiley

Subject

Physical and Theoretical Chemistry,Atomic and Molecular Physics, and Optics

Reference54 articles.

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