| Autor: |
Rojas-Buzo S; Instituto de Tecnología Química, Universitat Politècnica de València - Consejo Superior de Investigaciones Científicas, Av. de los Naranjos, s/n, 46022 Valencia, Spain., Salusso D; European Synchrotron Radiation Facility, 71 avenue des Martyrs, CS 40220, 38043 Grenoble Cedex 9, France., Le TT; Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares (CIQUS), University of Santiago de Compostela, 15782 Santiago de Compostela, Spain., Ortuño MA; Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares (CIQUS), University of Santiago de Compostela, 15782 Santiago de Compostela, Spain., Lomachenko KA; European Synchrotron Radiation Facility, 71 avenue des Martyrs, CS 40220, 38043 Grenoble Cedex 9, France., Bordiga S; Department of Chemistry and NIS Centre, University of Turin, Via Giuria 7, 10125 Turin, Italy. |
| Abstrakt: |
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 2+ /Cu + and Ce 4+ /Ce 3+ pairs behavior. Herein, we studied a novel Cu 2+ 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 + sites generated during catalysis play a pivotal role. Moreover, the oxygen vacancies associated with Ce 3+ sites and presented in the defective Cu/UiO-67(Ce) material are able to activate the O 2 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. |
