Abstract
The effect of introducing extra-framework Ga on the local structure of the metal sites in Fe/ZSM-5, resulting in enhanced reactivity toward N2O, was investigated using a combination of Raman and X-ray absorption spectroscopies. The Raman spectra indicate an increased abundance of oxo- and/or hydroxo-bridged diiron sites, whereas the Fe K-edge XANES reveals more extensive reduction of Fe(III) to Fe(II). Curvefits of the EXAFS at both the Ga and Fe K-edges are consistent with heterometallic oxo-clusters containing both Ga−Fe and Fe−Fe paths. The spectroscopic evidence suggests a tetranuclear [Fe2Ga2O42+] core, possessing an open dicubane structure.
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