期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 49, 页码 25891-25896出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202109705
关键词
copper; EXAFS; methane-to-methanol conversion; mordenite; wavelet transform; XANES
资金
- Horizon 2020 Excellence Science ERC-Synergy program 2019-CUBE: Unravelling the secrets of Cu-based catalysts for C-H activation [856446]
- Research Council of Norway [237922]
- Sigma2 Norwegian High Performance Computing program [NN4683K]
- Universita degli Studi di Torino within the CRUI-CARE Agreement
- European Research Council (ERC) [856446] Funding Source: European Research Council (ERC)
In this study, a series of gas-phase reactants were used to investigate the formation of Cu pairs in a Cu-exchanged mordenite zeolite under different reaction environments. The rearrangement of Cu ions to form multimeric sites was studied using X-ray absorption spectroscopy and advanced analysis through wavelet transform. The results showed that under an oxidative environment, Cu-I/Cu-II speciation correlated with Cu proximity, with metal ion pairs quantitatively forming.
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 Cu-I/Cu-II speciation clearly correlates with Cu proximity, with metal ion pairs quantitatively forming under an oxidative environment.
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