Conversion of methane to aromatic compounds using UZM-39 aluminosilicate zeolite

摘要

A new family of coherently grown composites of TUN and IMF zeotypes has been synthesized and shown to be effective catalysts in processes for converting at least one aliphatic hydrocarbon having from 1 to about 4 carbon atoms in a feedstream to provide at least one aromatic hydrocarbon. These zeolites are represented by the empirical formula.
NanMmk+TtAl1-xExSiyOz
where M represents zinc or a metal or metals from Group 1, Group 2, Group 3 or the lanthanide series of the periodic table, T is the organic structure directing agent or agents and E is a framework element such as gallium. The process involves contacting a low carbon number aliphatic hydrocarbon with the coherently grown composite of TUN and IMF zeotypes to produce at least an aromatic.

主权项

1. A process for converting at least one low carbon number aliphatic hydrocarbon in a feedstream to provide at least one aromatic hydrocarbon, the process comprising contacting the feedstream at reaction conditions with a catalyst to generate at least one aromatic hydrocarbon, the catalyst comprising a coherently grown composite of TUN and IMF zeotypes having a three-dimensional framework of at least AlO2 and SiO2 tetrahedral units and an empirical composition in the as synthesized and anhydrous basis expressed by an empirical formula of:
NanMmk+TtAl1-xExSiyOz where “n” is the mole ratio of Na to (Al+E) and has a value from approximately 0.05 to 0.5, M represents at least one metal selected from the group consisting of zinc, Group 1 (IUPAC 1), Group 2 (IUPAC 2), Group 3 (IUPAC 3), and the lanthanide series of the periodic table, and any combination thereof, “m” is the mole ratio of M to (Al+E) and has a value from 0 to 0.5, “k” is the average charge of the metal or metals M, T is the organic structure directing agent or agents derived from reactants R and Q where R is an A,Ω-dihalogen substituted alkane having from 3 to 6 carbon atoms and Q is at least one neutral monoamine having 6 or fewer carbon atoms, “t” is the mole ratio of N from the organic structure directing agent or agents to (Al+E) and has a value of from about 0.5 to about 1.5, E is an element selected from the group consisting of gallium, iron, boron and combinations thereof, “x” is the mole fraction of E and has a value from 0 to about 1.0, “y” is the mole ratio of Si to (Al+E) and varies from greater than 9 to about 25 and “z” is the mole ratio of O to (Al+E) and has a value determined by the equation:
z=(n+k·m+3+4·y)/2 and is characterized by a characteristic selected from the group consisting of (a) it has TUN regions and IMF regions that are coherently aligned so that the [010]TUN zone axis and the [001]IMF zone axis are parallel to each other and there is continuity of crystal planes of type (002)TUN and (060)IMF, where the indexing is referred to monoclinic C2/m and orthorhombic Cmcm unit cells for TUN and IMF respectively, (b) it has the x-ray diffraction pattern having at least the d-spacings and intensities set forth in Table A1:TABLE A12θd (Å)I/Io %7.17-7.2112.25-12.31vw-m 7.5-8.1*11.78-10.91w-m8.889.95m9.179.63w-m12.47-12.627.09-7.00w-m17.75.01vw-m22.8-23.23.90-3.83vs23.39-23.493.80-3.78m-s25.01-25.313.56-3.52m28.74-29.253.10-3.05w-m45.08-45.292.01-2.00w*composite peak consisting of multiple overlapping reflections and (c) combinations thereof.