Issue 7, 2024

Thermodynamic driving forces for autoreduction of Cu sites in the zeolite SSZ-13

Abstract

Cu-exchanged zeolites are widely used redox catalysts and the oxidation state of Cu is crucial in understanding their performance over a wide range of applications. Interestingly, a fraction of Cu sites in zeolites is reported to reduce at high temperatures in the absence of a reducing agent and as of today a detailed understanding of this process is still missing. In this contribution, we use first principles-based phase diagrams to explore thermodynamic driving forces for the autoreduction of Cu sites in the zeolite SSZ-13. We find that mainly monovalent Cu(II)–OH sites anchored at well-separated Al atoms and to a lesser degree di-hydroxyl Cu dimers drive the autoreduction of Cu sites in the zeolite SSZ-13. Using these insights, we can reproduce experimental trends in autoreduction reported in the literature. This work gives detailed insights into the autoreduction of Cu sites in SSZ-13 and demonstrates that the nature of Cu sites in the zeolite SSZ-13 depends on the exact conditions the material is exposed to. Optimizing these reaction conditions might allow to improve the performance of Cu-exchanged zeolites over a wide range of applications.

Graphical abstract: Thermodynamic driving forces for autoreduction of Cu sites in the zeolite SSZ-13

Article information

Article type
Paper
Submitted
31 Oct 2023
Accepted
15 Mar 2024
First published
15 Mar 2024
This article is Open Access
Creative Commons BY-NC license

React. Chem. Eng., 2024,9, 1685-1695

Thermodynamic driving forces for autoreduction of Cu sites in the zeolite SSZ-13

D. J. Hutton, D. H. Lopez and F. Göltl, React. Chem. Eng., 2024, 9, 1685 DOI: 10.1039/D3RE00580A

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