期刊
JOURNAL OF PHYSICAL CHEMISTRY B
卷 108, 期 28, 页码 10002-10011出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp048368w
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The valence and local symmetry of iron in framework-substituted FeZSM-5 with a high Fe dilution (Si/Fe = 360) was studied by means of Kbeta-detected X-ray absorption spectroscopy. This technique combines high-resolution (DeltaE similar to1 eV) fluorescence detection of the 3p to 1s (Kbeta) transition with the X-ray absorption near-edge structure (XANES) at the Fe K-edge. An absorption-like spectrum is recorded by detecting the Kbeta fluorescence intensity as a function of the incident energy that is scanned through the K absorption edge. Kbeta-detected XANES spectra allow for a more precise separation of the weak K pre-edge structure from the main edge as compared to conventional absorption spectroscopy. Subsequent analysis and interpretation of the pre-edge spectral features therefore is more accurate. The pre-edge is sensitive to changes in the local coordination and oxidation state of Fe. Using this technique we were able to quantitatively determine the degree of iron extraction out of a zeolite framework upon steaming. With the use of appropriate reference compounds, the pre-edge analysis was used to monitor the activation of low-loaded, framework-substituted FeZSM-5 (0.3 wt % Fe). Template removal and calcination distort the zeolite framework and induce a deviation from T-d symmetry for incorporated iron. The (deliberate) presence of water at high temperature (T > 500 degreesC) facilitates the hydrolysis of the Si-O-Fe bonds and increases the formation of extraframework iron species. The amount of Fe-III occupying tetrahedral sites in the MFI-type zeolite decreases to 32% and 19%, respectively, for mild- and hard-steamed samples.
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