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Literature DB >> 34330914

¹⁷O-EPR determination of the structure and dynamics of copper single-metal sites in zeolites.

Paolo Cleto Bruzzese^1,2, Enrico Salvadori², Stefan Jäger³, Martin Hartmann³, Bartolomeo Civalleri², Andreas Pöppl⁴, Mario Chiesa⁵.

Abstract

The bonding of copper ions to lattice oxygens dictates the activity and selectivity of copper exchanged zeolites. By 17O isotopic labelling of the zeolite framework, in conjunction with advanced EPR methodologies and DFT modelling, we determine the local structure of single site CuII species, we quantify the covalency of the metal-framework bond and we assess how this scenario is modified by the presence of solvating H216O or H217O molecules. This enables to follow the migration of CuII species as a function of hydration conditions, providing evidence for a reversible transfer pathway within the zeolite cage as a function of the water pressure. The results presented in this paper establish 17O EPR as a versatile tool for characterizing metal-oxide interactions in open-shell systems.

Entities: Chemical Disease Species

Year: 2021 PMID： 34330914 DOI： 10.1038/s41467-021-24935-7

Source DB: PubMed Journal: Nat Commun ISSN： 2041-1723 Impact factor: 14.919

31 in total

1. High-field pulsed EPR spectroscopy for the speciation of the reduced [PV(2)Mo(10)O(40)](6-) polyoxometalate catalyst used in electron-transfer oxidations.

Authors: Ilia Kaminker; Hila Goldberg; Ronny Neumann; Daniella Goldfarb
Journal: Chemistry Date: 2010-09-03 Impact factor: 5.236

2. Detection of Brønsted acid sites in zeolite HY with high-field 17O-MAS-NMR techniques.

Authors: Luming Peng; Yun Liu; Namjun Kim; Jennifer E Readman; Clare P Grey
Journal: Nat Mater Date: 2005-02-13 Impact factor: 43.841

Review 3. Active sites and mechanisms in the direct conversion of methane to methanol using Cu in zeolitic hosts: a critical examination.

Authors: Mark A Newton; Amy J Knorpp; Vitaly L Sushkevich; Dennis Palagin; Jeroen A van Bokhoven
Journal: Chem Soc Rev Date: 2020-02-28 Impact factor: 54.564

Review 4. Iron and Copper Active Sites in Zeolites and Their Correlation to Metalloenzymes.

Authors: Benjamin E R Snyder; Max L Bols; Robert A Schoonheydt; Bert F Sels; Edward I Solomon
Journal: Chem Rev Date: 2017-12-19 Impact factor: 60.622

5. Spectroscopy and redox chemistry of copper in mordenite.

Authors: Pieter Vanelderen; Julie Vancauwenbergh; Ming-Li Tsai; Ryan G Hadt; Edward I Solomon; Robert A Schoonheydt; Bert F Sels
Journal: Chemphyschem Date: 2014-01-13 Impact factor: 3.102

6. On the Mechanism Underlying the Direct Conversion of Methane to Methanol by Copper Hosted in Zeolites; Braiding Cu K-Edge XANES and Reactivity Studies.

Authors: Mark A Newton; Amy J Knorpp; Ana B Pinar; Vitaly L Sushkevich; Dennis Palagin; Jeroen A van Bokhoven
Journal: J Am Chem Soc Date: 2018-08-06 Impact factor: 15.419

Review 7. Cu-CHA - a model system for applied selective redox catalysis.

Authors: Elisa Borfecchia; Pablo Beato; Stian Svelle; Unni Olsbye; Carlo Lamberti; Silvia Bordiga
Journal: Chem Soc Rev Date: 2018-11-12 Impact factor: 54.564

8. The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment.

Authors: Dimitrios K Pappas; Andrea Martini; Michael Dyballa; Karoline Kvande; Shewangizaw Teketel; Kirill A Lomachenko; Rafal Baran; Pieter Glatzel; Bjørnar Arstad; Gloria Berlier; Carlo Lamberti; Silvia Bordiga; Unni Olsbye; Stian Svelle; Pablo Beato; Elisa Borfecchia
Journal: J Am Chem Soc Date: 2018-11-02 Impact factor: 15.419

¹⁷O-EPR determination of the structure and dynamics of copper single-metal sites in zeolites.

1. High-field pulsed EPR spectroscopy for the speciation of the reduced [PV(2)Mo(10)O(40)](6-) polyoxometalate catalyst used in electron-transfer oxidations.

2. Detection of Brønsted acid sites in zeolite HY with high-field 17O-MAS-NMR techniques.

Review 3. Active sites and mechanisms in the direct conversion of methane to methanol using Cu in zeolitic hosts: a critical examination.

Review 4. Iron and Copper Active Sites in Zeolites and Their Correlation to Metalloenzymes.

5. Spectroscopy and redox chemistry of copper in mordenite.

6. On the Mechanism Underlying the Direct Conversion of Methane to Methanol by Copper Hosted in Zeolites; Braiding Cu K-Edge XANES and Reactivity Studies.

Review 7. Cu-CHA - a model system for applied selective redox catalysis.

8. The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment.

9. Structures and reaction pathways of the molybdenum centres of sulfite-oxidizing enzymes by pulsed EPR spectroscopy.

10. Fast room temperature lability of aluminosilicate zeolites.

1. The Structure of Monomeric Hydroxo-Cu^II Species in Cu-CHA. A Quantitative Assessment.

Review 2. Emerging analytical methods to characterize zeolite-based materials.