A series of gas-phase reactants is used to treat a Cu-exchanged mordenite zeolite with the aim of studying the influence of the reaction environment on the formation of Cu pairs. The rearrangement of Cu ions to form multimeric sites as a function of their oxidation state was probed by X-ray absorption spectroscopy (XAS) and also by applying advanced analysis through wavelet transform, a method able to specifically locate Cu–Cu interactions also in the presence of overlapping contributions from other scattering paths. The nature of the Cu-oxo species formed upon oxidation was further crosschecked by DFT-assisted fitting of the EXAFS data and by resonant Raman spectroscopy. Altogether, the CuI/CuII speciation clearly correlates with Cu proximity, with metal ion pairs quantitatively forming under an oxidative environment.

Copper Pairing in the Mordenite Framework as a Function of the CuI/CuII Speciation

Deplano G.;Martini A.;Signorile M.;Borfecchia E.;Crocella V.;Bordiga S.
2021

Abstract

A series of gas-phase reactants is used to treat a Cu-exchanged mordenite zeolite with the aim of studying the influence of the reaction environment on the formation of Cu pairs. The rearrangement of Cu ions to form multimeric sites as a function of their oxidation state was probed by X-ray absorption spectroscopy (XAS) and also by applying advanced analysis through wavelet transform, a method able to specifically locate Cu–Cu interactions also in the presence of overlapping contributions from other scattering paths. The nature of the Cu-oxo species formed upon oxidation was further crosschecked by DFT-assisted fitting of the EXAFS data and by resonant Raman spectroscopy. Altogether, the CuI/CuII speciation clearly correlates with Cu proximity, with metal ion pairs quantitatively forming under an oxidative environment.
ANGEWANDTE CHEMIE. INTERNATIONAL EDITION
60
49
25891
25896
https://onlinelibrary.wiley.com/doi/full/10.1002/anie.202109705
copper; EXAFS; methane-to-methanol conversion; mordenite; wavelet transform; XANES
Deplano G.; Martini A.; Signorile M.; Borfecchia E.; Crocella V.; Svelle S.; Bordiga S.
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2318/1837816
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