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Fe-ZSM-5 Catalysts for the Selective Reduction of NO by Isobutane - The Problem of the Active Sites

  • Relations between the structure of Fe–ZSM-5 catalysts prepared by interaction of FeCl3 with H–ZSM-5 and their catalytic behavior in the SCR of NO by isobutane were investigated by combining results of catalytic studies (1000 ppm NO, 1000 ppm isobutane, and 2% O2 in He, 30,000 h-1) and of physicochemical characterization (XRD, EXAFS, Mössbauer spectroscopy, TPR, IR, XPS). By variation of the preparation conditions (method of FeCl3 introduction—chemical vapor deposition or solid-state ion exchange, washing intensity, calcination regime) and of the matrix (H–ZSM-5 with normal and high defect density), Fe–ZSM-5 materials with strongly varying properties (aggregation degree of the Fe phase, acidity) were obtained. Significant discrepancies between conclusions derived from EXAFS, TPR, and Mössbauer spectroscopy were ascribed to a preference of Mössbauer spectroscopy for the detection of aggregated phases and a high defectivity of Fe oxide clusters formed upon calcination. The critical stepRelations between the structure of Fe–ZSM-5 catalysts prepared by interaction of FeCl3 with H–ZSM-5 and their catalytic behavior in the SCR of NO by isobutane were investigated by combining results of catalytic studies (1000 ppm NO, 1000 ppm isobutane, and 2% O2 in He, 30,000 h-1) and of physicochemical characterization (XRD, EXAFS, Mössbauer spectroscopy, TPR, IR, XPS). By variation of the preparation conditions (method of FeCl3 introduction—chemical vapor deposition or solid-state ion exchange, washing intensity, calcination regime) and of the matrix (H–ZSM-5 with normal and high defect density), Fe–ZSM-5 materials with strongly varying properties (aggregation degree of the Fe phase, acidity) were obtained. Significant discrepancies between conclusions derived from EXAFS, TPR, and Mössbauer spectroscopy were ascribed to a preference of Mössbauer spectroscopy for the detection of aggregated phases and a high defectivity of Fe oxide clusters formed upon calcination. The critical step for the preparation of a highly disperse Fe phase is extensive washing after Fe introduction. The catalytic behavior of overexchanged Fe–ZSM-5 materials prepared by interaction of FeCl3 with H–ZSM-5 of normal defect density was not influenced by aggregation of a significant part of the Fe phase. The comparison of their catalytic properties with those of a Fe2O3/H–ZSM-5 mechanical mixture and of catalysts prepared by aqueous ion exchange or by CVD of FeCl3 into H–ZSM-5 of high defect density implies that the particular activity of overexchanged Fe–ZSM-5 arises from minority sites. In these, the Fe ions are probably isolated. Other Fe sites of low nuclearity appear to add to the activity. The poor SCR performance (at a given ability for isobutane activation) of Fe–ZSM-5 prepared with a defective ZSM-5 matrix may indicate that the Fe sites which provi de the particular activity of overexchanged Fe–ZSM-5 require the cooperation of acidic sites.zeige mehrzeige weniger

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Metadaten
Autor*innen:F. Heinrich, C. Schmidt, E. Löffler, Michael Menzel, W. Grünert
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):Journal of catalysis
Jahr der Erstveröffentlichung:2002
Verlag:Acad. Press
Verlagsort:San Diego, Calif.
Jahrgang/Band:212
Erste Seite:157
Letzte Seite:172
Freie Schlagwörter:EXAFS; Fe-ZSM-5; Hydrocarbons; Isobutane; Mössbauer spectroscopy; Temperature-programmed reduction; deNOx
DOI:10.1006/jcat.2002.3775
ISSN:0021-9517
ISSN:1090-2694
Verfügbarkeit des Dokuments:Physisches Exemplar in der Bibliothek der BAM vorhanden ("Hardcopy Access")
Bibliotheksstandort:Sonderstandort: Publica-Schrank
Datum der Freischaltung:19.02.2016
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:03.02.2003
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