Revisiting the nature of Cu sites in the activated Cu-SSZ-13 catalyst for SCR reaction† †Electronic supplementary information (ESI) available: experimental section (sample description, in situ FTIR spectroscopy, synchrotron characterization, DFT-based analysis of XAS and XES data); XAS of hydrated Cu-SSZ-13; reversibility of the Cu(i) ↔ Cu(ii) redox chemistry and extra-ligand loss process upon high-temperature gas-flow switching; full report on DFT-optimized geometries; full report on EXAFS fitting results on O2-activated Cu-SSZ-13; EXAFS spectra for a low Cu-loading Cu-SSZ-13 sample after O2-activation at 400 °C. See DOI: 10.1039/c4sc02907k Click here for additional data file.
نویسندگان
چکیده
Department of Chemistry and INSTM Refe Giuria 7, 10125 Turin, Italy. E-mail: carlo.l NIS Centre of Excellence, University of Turi Haldor Topsøe A/S, Nymøllevej 55, 2800 Kg CrisDI Center of Crystallography, Universit Southern Federal University, Zorge street 5 † Electronic supplementary information (sample description, in situ FTIR spectr DFT-based analysis of XAS and XES reversibility of the Cu(I) 4 Cu(II) redox c upon high-temperature gas-ow switch geometries; full report on EXAFS ttin EXAFS spectra for a low Cu-loading Cu-S C. See DOI: 10.1039/c4sc02907k Cite this: Chem. Sci., 2015, 6, 548
منابع مشابه
Characterization of Cu-exchanged SSZ-13: a comparative FTIR, UV-Vis, and EPR study with Cu-ZSM-5 and Cu-β with similar Si/Al and Cu/Al ratios.
Cu-SSZ-13 has been characterized by different spectroscopic techniques and compared with Cu-ZSM-5 and Cu-β with similar Si/Al and Cu/Al ratios and prepared by the same ion exchange procedure. On vacuum activated samples, low temperature FTIR spectroscopy allowed us to appreciate a high concentration of reduced copper centres, i.e. isolated Cu(+) ions located in different environments, able to f...
متن کاملComposition-driven Cu-speciation and reducibility in Cu-CHA zeolite catalysts: a multivariate XAS/FTIR approach to complexity† †Electronic supplementary information (ESI) available: Sample description and synthesis details, experimental setup for in situ XAS and FTIR spectroscopy, details on the MCR-ALS method, details on DFT-assisted XANES simulations, details on the determination of N pure by PCA, MCR-ALS results for downsized and upsized component spaces, additional information to support the assignment of theoretical XANES curves, details on EXAFS analysis, details on IR spectral deconvolution. See DOI: 10.1039/c7sc02266b Click here for additional data file.
Department of Chemistry, NIS Centre and Turin, Via P. Giuria 7, Turin, 10125 Italy. E Haldor Topsøe A/S, Haldor Topsøes Allé 1, European Synchrotron Radiation Facility, 71 Cedex 9, 38043 France IRC “Smart Materials”, Southern Federal 344090 Russia Department of Chemistry, CrisDi Centre an Turin, Via P. Giuria 7, Turin, 10125 Italy † Electronic supplementary information ( synthesis details, expe...
متن کاملEffect of Heteroatom Concentration in SSZ-13 on the Methanol-to-Olefins Reaction
SSZ-13 materials have been synthesized with varying amounts of Al to produce samples with different concentrations of Brønsted acid sites, and consequently, these SSZ-13 materials contain increasing numbers of paired Al heteroatoms with increasing Al content. These materials were then characterized and tested as catalysts for the methanol-toolefins (MTO) reaction at 400 °C and 100% methanol con...
متن کاملSynthesis and functionalization of SSZ-13 as an NH3-SCR catalyst
Hydrothermal synthesis of Na-SSZ-13 using a low concentration of the structure-directing agent N,N,N-trimethyl-1-adamantanimonium hydroxide and functionalization of the SSZ-13 framework through the introduction of Cu and Fe via ion exchange have been carried out. The prepared samples were characterized by XRD, SEM, and UV-vis spectroscopy, N2 sorption, XRF and NH3-TPD. It was found that relativ...
متن کاملStructural snapshots of the SCR reaction mechanism on Cu-SSZ-13.
The structure of copper sites in Cu-SSZ-13 during NH3-SCR was unravelled by a combination of novel operando X-ray spectroscopic techniques. Strong adsorption of NH3 on Cu, its reaction with weakly adsorbed NO from the gas phase, and slow re-oxidation of Cu(I) were proven. Thereby the SCR reaction mechanism is significantly different to that observed for Fe-ZSM-5.
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عنوان ژورنال:
دوره 6 شماره
صفحات -
تاریخ انتشار 2015