TY - JOUR A1 - Heinrich, F. A1 - Schmidt, C. A1 - Löffler, E. A1 - Menzel, Michael A1 - Grünert, W. T1 - Fe-ZSM-5 Catalysts for the Selective Reduction of NO by Isobutane - The Problem of the Active Sites JF - Journal of catalysis N2 - 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 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. KW - deNOx KW - Hydrocarbons KW - Isobutane KW - Fe-ZSM-5 KW - EXAFS KW - Mössbauer spectroscopy KW - Temperature-programmed reduction PY - 2002 DO - https://doi.org/10.1006/jcat.2002.3775 SN - 0021-9517 SN - 1090-2694 VL - 212 SP - 157 EP - 172 PB - Acad. Press CY - San Diego, Calif. AN - OPUS4-2258 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Grünert, W. A1 - Heinrich, F. A1 - Schmidt, C. A1 - Löffler, E. A1 - Menzel, Michael T1 - Fe_ZSM-5 - Katalisatoren für die SCR von NO durch Kohlenwasserstoffe: Katalysatorstruktur und katalytische Eigenschaften T2 - 35. Jahrestreffen deutscher Katalytiker T2 - 35. Jahrestreffen deutscher Katalytiker CY - Weimar, Germany DA - 2002-03-20 PY - 2002 AN - OPUS4-4883 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -