The small pore Cu-CHA zeolite is attracting increasing attention as a versatile platform to design novel single-site catalysts for deNOx applications and for the direct conversion of methane to methanol. Understanding at the atomic scale how the catalyst composition influences the Cu-species formed during thermal activation is a key step to unveil the relevant composition-activity relationships. Herein, we explore by in situ XAS the impact of Cu-CHA catalyst composition on temperature-dependent Cu-speciation and reducibility. Advanced multivariate analysis of in situ XANES in combination with DFT-assisted simulation of XANES spectra and multi-component EXAFS fits as well as in situ FTIR spectroscopy of adsorbed N2 allow us to obtain unprecedented quantitative structural information on the complex dynamics during the speciation of Cu-sites inside the framework of the CHA zeolite.

Composition-driven Cu-speciation and reducibility in Cu-CHA zeolite catalysts: A multivariate XAS/FTIR approach to complexity

MARTINI, ANDREA;BORFECCHIA, ELISA;Pankin, I. A.;NEGRI, CHIARA;BERLIER, Gloria;BORDIGA, Silvia;LAMBERTI, Carlo
2017

Abstract

The small pore Cu-CHA zeolite is attracting increasing attention as a versatile platform to design novel single-site catalysts for deNOx applications and for the direct conversion of methane to methanol. Understanding at the atomic scale how the catalyst composition influences the Cu-species formed during thermal activation is a key step to unveil the relevant composition-activity relationships. Herein, we explore by in situ XAS the impact of Cu-CHA catalyst composition on temperature-dependent Cu-speciation and reducibility. Advanced multivariate analysis of in situ XANES in combination with DFT-assisted simulation of XANES spectra and multi-component EXAFS fits as well as in situ FTIR spectroscopy of adsorbed N2 allow us to obtain unprecedented quantitative structural information on the complex dynamics during the speciation of Cu-sites inside the framework of the CHA zeolite.
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http://pubs.rsc.org/en/Content/ArticleLanding/2017/SC/C7SC02266B#!divAbstract
X-RAY-ABSORPTION; IN SITU XAS; FTIR, MULTIVARIATE CURVE RESOLUTION; CU-ZEOLITE; CU-CHA; CATALYSIS
Martini, Andrea; Borfecchia, Elisa; Lomachenko, K. A.; Pankin, I. A.; Negri, Chiara; Berlier, Gloria; Beato, P.; Falsig, H.; Bordiga, Silvia; Lamberti, Carlo
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2318/1651332
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