Method for producing zeolites and zeotypes

Patent metadata

Field	Value
Publication number	US-2016137516-A1
Application number	US-201414898656-A
Country	US
Kind code	A1
Filing date	Jul 7, 2014
Priority date	Jul 5, 2013
Publication date	May 19, 2016
Grant date	—

Abstract

The invention relates to a method for producing zeolite, zeolite-like or zeotype particles comprising the steps of: 1) Adding one or more metal precursors to a silica or alumina source; 2) Reducing the one or more metal precursors to form metal nanoparticles on the surface of the silica or alumina source; 3) Passing a gaseous hydrocarbon, alkyl alcohol or alkyl ether over the silica or alumina supported metal nanoparticle to form a carbon template coated zeolite, zeolite-like or zeotype precursor composition; 4a) Adding a structure directing agent to the carbon template coated zeolite, zeolite-like or zeotype precursor composition thereby creating a zeolite, zeolite-like or zeotype gel composition; 4b) Crystallising the zeolite, zeolite-like or zeotype gel composition by subjecting said composition to a hydrothermal treatment; 5) Removing the carbon template and structure directing agent and isolating the resulting zeolite, zeolite-like or zeotype particles.

First claim

1 . A method for producing zeolite, zeolite-like or zeotype particles comprising:
1) Adding one or more metal precursors to a silica or alumina source; 2) Reducing the one or more metal precursors to form metal nanoparticles on the surface of the silica or alumina source; 3) Passing a gaseous hydrocarbon, alkyl alcohol or alkyl ether over the silica or alumina supported metal nanoparticle to form a carbon template coated zeolite, zeolite-like or zeotype precursor composition; 4a) Adding a structure directing agent to the carbon template coated zeolite, zeolite-like or zeotype precursor thereby creating a zeolite, zeolite-like or zeotype gel composition; 4b) Crystallising the zeolite, zeolite-like or zeotype gel composition by subjecting said composition to a hydrothermal treatment; and 5) Removing the carbon template and structure directing agent and isolating the resulting zeolite, zeolite-like or zeotype particles; wherein the carbon template coated zeolite, zeolite-like or zeotype precursor composition of step 3 is used directly in step 4a without removing the silica or alumina source.

2 - 16 . (canceled)

17 . The method for producing zeolite, zeolite-like or zeotype particles according to claim 1 , wherein the one or more metal(s) is selected from the group consisting of group 4 elements, group 6 elements, group 7 elements, group 8 elements, group 9 elements, group 10 elements, group 11 elements and group 12 elements or mixtures thereof.

18 . The method for producing zeolite, zeolite-like or zeotype particles according to claim 1 , wherein the one or more metal(s) is selected from the group consisting of titanium, osmium, iridium, platinum, ruthenium, palladium, rhodium, rhenium, copper, nickel, iron, cobalt, silver, gold, cadmium, and molybdenium or mixtures thereof.

19 . The method of producing a zeolite, zeolite-like or zeotype particle according to claim 1 , the method further comprising adding an Al, Sn Ti, Zr or Ge source during step 4a.

20 . The method for producing zeolite, zeolite-like or zeotype particles according to claim 1 , wherein the hydrocarbon is selected from the group consisting of aliphatic hydrocarbons having 1 to 8 carbon atoms, aliphatic hydrocarbons having 1 to 3 carbon atoms, alkenes having 2 to 6 carbon atoms, aromatic hydrocarbons having 6 to 10 carbon atoms and cyclic hydrocarbons having 3 to 8 carbon atoms.

21 . The method for producing zeolite, zeolite-like or zeotype particles according to claim 20 , wherein the hydrocarbon is methane, propene, xylene or benzene.

22 . The method for producing zeolite, zeolite-like or zeotype particles according to claim 1 , wherein the hydrothermal treatment comprises that the zeolite, zeolite-like or zeotype gel composition is heated to temperatures between 70 and 300° C., or at 180° C., under an autogeneous pressure in an autoclave or open flask for 24 hours or more.

23 . The method for producing zeolite, zeolite-like or zeotype particles according to claim 1 , wherein the one or more metal metals precursors is added to the silica or alumina source in an amount of 5 to 20 wt %, from 0.5 to 5 wt %, from 0.5 to 2 wt %, or 1 wt % during step 1.

24 . The zeolite, zeolite-like or zeotype particle manufactured by the method according to claim 1 with a crystal structure comprising one or more encapsulated metal nanoparticles.

25 . The zeolite, zeolite-like or zeotype particle according to claim 24 , wherein the particle is a hierarchical mesoporous zeolite or zeotype particle.

26 . The zeolite, zeolite-like or zeotype particle according to claim 24 , wherein the amount of metal nanoparticles are in the range from 0.1 to 25 wt %, 0.5 to 20 wt %, 0.5 to 10 wt %, 0.5 to 5%, 1.0 to 5 wt %, 1 to 2 wt %, or 1 wt %.

27 . The zeolite, zeolite-like or zeotype particle according to claim 24 , wherein the one or more encapsulated metal nanoparticles comprise one or more metal(s) selected from the group consisting of group 4 elements, group 6 elements, group 7 elements, group 8 elements, group 9 elements, group 10 elements, group 11 elements and group 12 elements or mixtures thereof.

28 . The zeolite, zeolite-like or zeotype particle according to claim 24 , wherein the one or more encapsulated metal nanoparticles comprise one or more metal(s) selected from the group consisting of titanium, osmium, iridium, platinum, ruthenium, palladium, rhodium, rhenium, copper, nickel, iron, cobalt, silver, gold, cadmium, and molybdenum or mixtures thereof.

29 . The zeolite, zeolite-like or zeotype particle according to claim 24 , the zeolite, zeolite-like or zeotype particle comprising an Al, Sn, Ti, Zr or Ge source in the framework of the crystal structure.

30 . A method of using the zeolite particle according to claim 24 in Catalytic Cracking, hydrocracking, hydroconversion, paraffin isomerisation, paraffin aromatisation, olefin oligomerisation, aromatic alkylation, aromatic disproportionation, aromatic isomerisation, MTG-MTO, hydration, hydrogenation, benzene hydroxylation, phenol hydroxylation, DeNOx stationary sources or synthesis of fine chemicals comprising providing the zeolite particle according to claim 24 and subjecting said zeolite particle to a process selected from the group consisting of Catalytic Cracking, hydrocracking, hydroconversion, paraffin isomerisation, paraffin aromatisation, olefin oligomerisation, aromatic alkylation, aromatic disproportionation, aromatic isomerisation, MTG-MTO, hydration, hydrogenation, benzene hydroxylation, phenol hydroxylation, DeNOx stationary sources and synthesis of fine chemicals.

Assignees

• Univ Danmarks Tekniske

Inventors

• Kegnæs Søren
• Abildstrøm Jacob Oskar
• Mielby Jerrik Jørgen

Classifications

• C07C2529/89

  Silicates, aluminosilicates or borosilicates of titanium, zirconium or hafnium · CPC title

• C01B39/08 Primary

  the aluminium atoms being wholly replaced · CPC title

• C07C2/66

  Catalytic processes · CPC title

• B01J29/89

  Silicates, aluminosilicates or borosilicates of titanium, zirconium or hafnium {(B01J29/005 takes precedence)} · CPC title

• C07C5/2772

  with metal oxides · CPC title