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Unveiling the Role and Stabilization Mechanism of Cu + into Defective Ce-MOF Clusters during CO Oxidation.
- Source :
-
The journal of physical chemistry letters [J Phys Chem Lett] 2024 Apr 11; Vol. 15 (14), pp. 3962-3967. Date of Electronic Publication: 2024 Apr 03. - Publication Year :
- 2024
-
Abstract
- Copper single-site catalysts supported on Zr-based metal-organic frameworks (MOFs) are well-known systems in which the nature of the active sites has been deeply investigated. Conversely, the redox chemistry of the Ce-counterparts is more limited, because of the often-unclear Cu <superscript>2+</superscript> /Cu <superscript>+</superscript> and Ce <superscript>4+</superscript> /Ce <superscript>3+</superscript> pairs behavior. Herein, we studied a novel Cu <superscript>2+</superscript> single-site catalyst supported on a defective Ce-MOF, Cu/UiO-67(Ce), as a catalyst for the CO oxidation reaction. Based on a combination of in situ DRIFT and operando XAS spectroscopies, we established that Cu <superscript>+</superscript> sites generated during catalysis play a pivotal role. Moreover, the oxygen vacancies associated with Ce <superscript>3+</superscript> sites and presented in the defective Cu/UiO-67(Ce) material are able to activate the O <subscript>2</subscript> molecules, closing the catalytic cycle. The results presented in this work open a new route for the design of active and stable single-site catalysts supported on defective Ce-MOFs.
Details
- Language :
- English
- ISSN :
- 1948-7185
- Volume :
- 15
- Issue :
- 14
- Database :
- MEDLINE
- Journal :
- The journal of physical chemistry letters
- Publication Type :
- Academic Journal
- Accession number :
- 38569092
- Full Text :
- https://doi.org/10.1021/acs.jpclett.4c00324