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  • Both the laboratory synthesized zeolites with tailored distribution of framework Al atoms and commercial ZSM-5 zeolites of various proveniences were investigated in a broad region of Si/Al ratio with respect to the distribution of Al atoms in the framework. The analysis of the distribution of framework Al atoms was done by using strictly defined conditions of Co(II) ion exchange and UV-Vis, 27Al and 29Si (CP) MAS NMR experiments. Evidence has been found that the distribution of framework Al atoms in ZSM-5, and in Si-rich zeolites in general, is not random and is not controlled by statistics, but occurs between the most populated Al pairs (Al-Si-Si-Al sequences in 6MRs) and single far distant Al atoms (Al-Sin>2-Al sequences) located in different rings. Depending on the type of Si- and Al-reactants and presence of TPA+/Na+ in gels, a broad distribution of Al atoms (from 5 to 85% of Al atoms in Al pairs) for Si/Al 12-20 can be achieved. At Si/Al > 20, the population of Al pairs decreases, but 90% of single Al atoms can be obtained in the whole range of Si/Al compositions. The local negative charge of the framework governed by the distribution of framework Al atoms inevitably controls the structure of the counter metal ion species, which is reflected in the catalytic properties of metallo-zeolites in redox reactions requiring different types of counter ion species. A high population of Al pairs in the framework is required for stabilization of divalent bare Cu(II), Co(II) and Fe(II) ions both in ZSM-5 and the beta zeolite, representing the active sites for C10H22-SCR-NOx, CH4- and C3H8-SCR-NOx, and for N2O decomposition, respectively.
  • Both the laboratory synthesized zeolites with tailored distribution of framework Al atoms and commercial ZSM-5 zeolites of various proveniences were investigated in a broad region of Si/Al ratio with respect to the distribution of Al atoms in the framework. The analysis of the distribution of framework Al atoms was done by using strictly defined conditions of Co(II) ion exchange and UV-Vis, 27Al and 29Si (CP) MAS NMR experiments. Evidence has been found that the distribution of framework Al atoms in ZSM-5, and in Si-rich zeolites in general, is not random and is not controlled by statistics, but occurs between the most populated Al pairs (Al-Si-Si-Al sequences in 6MRs) and single far distant Al atoms (Al-Sin>2-Al sequences) located in different rings. Depending on the type of Si- and Al-reactants and presence of TPA+/Na+ in gels, a broad distribution of Al atoms (from 5 to 85% of Al atoms in Al pairs) for Si/Al 12-20 can be achieved. At Si/Al > 20, the population of Al pairs decreases, but 90% of single Al atoms can be obtained in the whole range of Si/Al compositions. The local negative charge of the framework governed by the distribution of framework Al atoms inevitably controls the structure of the counter metal ion species, which is reflected in the catalytic properties of metallo-zeolites in redox reactions requiring different types of counter ion species. A high population of Al pairs in the framework is required for stabilization of divalent bare Cu(II), Co(II) and Fe(II) ions both in ZSM-5 and the beta zeolite, representing the active sites for C10H22-SCR-NOx, CH4- and C3H8-SCR-NOx, and for N2O decomposition, respectively. (en)
Title
  • Critical evaluation of the role of the distribution of Al atoms in the framework for the activity of metallo-zeolites in redox N2O/NOx reactions
  • Critical evaluation of the role of the distribution of Al atoms in the framework for the activity of metallo-zeolites in redox N2O/NOx reactions (en)
skos:prefLabel
  • Critical evaluation of the role of the distribution of Al atoms in the framework for the activity of metallo-zeolites in redox N2O/NOx reactions
  • Critical evaluation of the role of the distribution of Al atoms in the framework for the activity of metallo-zeolites in redox N2O/NOx reactions (en)
skos:notation
  • RIV/61388955:_____/14:00427597!RIV15-GA0-61388955
http://linked.open...avai/riv/aktivita
http://linked.open...avai/riv/aktivity
  • I, P(GAP106/11/0624)
http://linked.open...iv/cisloPeriodika
  • MAR 2014
http://linked.open...vai/riv/dodaniDat
http://linked.open...aciTvurceVysledku
http://linked.open.../riv/druhVysledku
http://linked.open...iv/duvernostUdaju
http://linked.open...titaPredkladatele
http://linked.open...dnocenehoVysledku
  • 9204
http://linked.open...ai/riv/idVysledku
  • RIV/61388955:_____/14:00427597
http://linked.open...riv/jazykVysledku
http://linked.open.../riv/klicovaSlova
  • Cu-zeolite; Co-zeolite; Fe-zeolite (en)
http://linked.open.../riv/klicoveSlovo
http://linked.open...odStatuVydavatele
  • NL - Nizozemsko
http://linked.open...ontrolniKodProRIV
  • [2C16B1AAB2CF]
http://linked.open...i/riv/nazevZdroje
  • Applied Catalysis A - General
http://linked.open...in/vavai/riv/obor
http://linked.open...ichTvurcuVysledku
http://linked.open...cetTvurcuVysledku
http://linked.open...vavai/riv/projekt
http://linked.open...UplatneniVysledku
http://linked.open...v/svazekPeriodika
  • 474
http://linked.open...iv/tvurceVysledku
  • Dědeček, Jiří
  • Sazama, Petr
  • Sobalík, Zdeněk
  • Wichterlová, Blanka
http://linked.open...ain/vavai/riv/wos
  • 000336005800022
issn
  • 0926-860X
number of pages
http://bibframe.org/vocab/doi
  • 10.1016/j.apcata.2013.07.033
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