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EP0021445A2 Expired / Lapsed EP ⏱️ 0.0 years remaining

Method for preparing zeolites, zeolites obtained by such method and their use for the conversion of hydrocarbons

Assignee: Montedison SpA
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Filing: 1980-06-27
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Granted: —
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Expires: 2000-06-27
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Abstract

Abstract Preparation of zeolites having the formula: wherein Y ranges from 20 to 90, Z ranges from 2 to 12, M is at least one cation and n ist the valence of M; said preparation comprises the admixing of diethyl-piperidinium hydroxide [(DEPP) + OH-] or of a salt thereof with water and with: a) at least one sodium compound; b) at least one compound of aluminium; c) at least one compound of silicon; the respective molar ratios, expressed as ratios of oxides, being comprised in the following ranges: SiO 2 :Al 2 O 3 = from 20 to 120 Na 2 0:Si0 2 = from 0.07 to 0.50 (DEPP) 2 O:SiO 2 = from 0.05 to 0.50 H 2 0:Na 2 0 = from 50 to 600. The invention concerns also zeolites obtained by said preparation and their use for some acid-catalyzed conversions of hydrocarbons.

Inventors

  • 👤 Raymond Le Van Mao
  • 👤 Orlando Pilati
  • 👤 Enrico Moretti
  • 👤 Romano Covini
  • 👤 Fausto Genoni

Bibliographic Details

Application Number —
Jurisdiction EP
Data Source google_patents
Last Synchronized 2026-10-25 21:04
CPC Classifications
C; C07; C07C; C07C6/00; B; B01; B01J; B01J29/00; B01J29/04; B01J29/06; B01J29/70; B01J29/7049; B01J29/72; B01J29/76; C01; C01B; C01B39/00; C01B39/02; C01B39/023; C07C2/00; C07C2/54; C07C4/00; C07C4/02; C07C4/06; C07C4/08; C07C5/00; C07C5/22; C07C5/27; C07C5/2729; C07C5/2732; C07C5/2737; C07C5/32; C07C5/373; C07C5/393; C07C5/41; C07C2529/00; C07C2529/04; C07C2529/06; Y; Y02; Y02P; Y02P20/00; Y02P20/50; Y02P20/52

Claims Analysis

Total Claims: 20
Claim 1
Independent Claim 205 words
1) A method for preparing zeolites having the formula: wherein Y ranges from 20 to 90, preferably from 50 to 80, Z ranges from 2 to 12, preferably from 3 to 8, M is at least one cation and n is the valence of cation M, and wherein aluminium and silicon can be optionally replaced, at least partially, by gallium and germanium respectively, said method comprising the admixing of diethyl-piperidinium hydroxide / (DEPP) OH ]or of a salt thereof with water and with: a) at least one sodium compound; b) at least one compound of a metal selected from the group comprising aluminium, gallium and mixtures thereof; c) at least one compound of an element selected from the group comprising silicon, germanium and mixture thereof, the respective molar ratios, expressed as ratios of oxides, being comprised in the following ranges: SiO 2 : Al 2 O 3 = from 20 to 120 (preferably from 50 to 85) Na 2 0 : SiO 2 = from 0.07 to 0.50 (preferably from 0.07 to 0.25) (DEPP) 0 : SiO 2 = from 0.05 to 0.50 (preferably from 0.10 to 0.20) H 2 O : Na 2 0 = from 50 to 600 (preferably from 150 to 400).
Claim 2
Dependent Claim 205 words
1) A method for preparing zeolites having the formula: wherein Y ranges from 20 to 90, preferably from 50 to 80, Z ranges from 2 to 12, preferably from 3 to 8, M is at least one cation and n is the valence of cation M, and wherein aluminium and silicon can be optionally replaced, at least partially, by gallium and germanium respectively, said method comprising the admixing of diethyl-piperidinium hydroxide / (DEPP) OH ]or of a salt thereof with water and with: a) at least one sodium compound; b) at least one compound of a metal selected from the group comprising aluminium, gallium and mixtures thereof; c) at least one compound of an element selected from the group comprising silicon, germanium and mixture thereof, the respective molar ratios, expressed as ratios of oxides, being comprised in the following ranges: SiO 2 : Al 2 O 3 = from 20 to 120 (preferably from 50 to 85) Na 2 0 : SiO 2 = from 0.07 to 0.50 (preferably from 0.07 to 0.25) (DEPP) 0 : SiO 2 = from 0.05 to 0.50 (preferably from 0.10 to 0.20) H 2 O : Na 2 0 = from 50 to 600 (preferably from 150 to 400).
Claim 3
Dependent Claim 67 words
2) A method according to claim 1, wherein the cationic dilution ratios, namely the molar ratios: r1 = H 2 O : (DEPP) 2 O r2 = H 2 O : [(DEPP) 2 O + Na 2 O] are defined as follows: r1 = equal to or higher than 180 and preferably than 225 , r2 = equal to or higher than 100 and preferably than 110.
Claim 4
Dependent Claim 20 words
3) A method according to claim 1, wherein the sodium factor SF, namely the ratio r2:r1 is lower than 0.50.
Claim 5
Dependent Claim 41 words
4) A method according to claim 1, wherein the start mixture is heated, until crystallization, in at least one step, at a temperature from 130 to 200°C and preferably from 160 to 200°C, for at least 24 and preferably 48 hours.
Claim 6
Dependent Claim 41 words
5) A method according to claim 1, wherein first an aqueous solution is prepared, which contains the DEPP salt, sodium aluminate and NaOH, secondly the solution is heated, preferably between 60 and 70°C and thirdly a solution containing Si02 is added.
Claim 7
Dependent Claim 41 words
6) A method according to claim 1, characterized in that the crystallized zeolite is washed, dried and activated by means of heating in the air at high temperature, preferably ranging from 450°C to the temperature at which the structural collapse starts.
Claim 8
Dependent Claim 32 words
7) A method according to claim 1, characterized in that the diethyl-piperidinium salt is diethyl-piperidinium-bromide, compound a) is sodium hydroxide, compound b) is sodium aluminate and compound c) is a silica sol.
Claim 9
Dependent Claim 51 words
8) A method according to claim 1, characterized in that said cation M is selected, from amongst the monovalent cations, the ions of the elements of the rare earths, the ions of the elements belonging to the 2nd and 8th Groups of the Periodic System of the elements and mixtures thereof.
Claim 10
Dependent Claim 35 words
9) A method according to claim 9, characterized in that said monovalent cations are selected from the group comprising the alkaline ions, the hydrogen ion, the ammonium ion, the diethyl-piperidinium ion (DEPP) and mixtures thereof.
Claim 11
Dependent Claim 39 words
10) Use of the zeolites obtained according to the method of claim 1 in a process for converting hydrocarbons by means of reactions usually catalyzed by acids, such as cracking, hydrocracking, isomerization, aromatization, polymerization, alkylation, disproportionation, reforming and dealkylation.
Claim 12
Dependent Claim 30 words
11) The use according to claim 10, characterized in that said isomerization is an isomerization to para- and/ or ortho-xylene of meta-xylene or of mixtures of meta-xylene with its isomers.
Claim 13
Dependent Claim 63 words
12) The use according to claim 11, characterized in that said isomerization is effected in the vapour phase, in the presence of hydrogen, at temperatures ranging from 250°C to 450°C, preferably from 275° to 400°C, at pressures ranging from 1000 to 2000 Kilopascal and at space velocities of from 1 to 10 volumes of liquid hydrocarbons per volume of catalyst and per hour.
Claim 14
Dependent Claim 15 words
13) The use according to claim 11, wherein the zeolites are in the acid form.
Claim 15
Dependent Claim 20 words
14) The use according to claim 11, wherein the zeolite catalysts contain nickel or other metals of the VIII group.
Claim 16
Dependent Claim 31 words
15) The use according to claim 11 wherein the zeolites are admixed with a binder, preferably selected from the group comprising silica, alumina, clays like for instance bentonite, and mixtures thereof.
Claim 17
Dependent Claim 19 words
16) The use according to claim 11, wherein the zeolites have the X-ray diffraction pattern reported on Table 8.
Claim 18
Dependent Claim 24 words
17) New zeolites, defined as zeolites MB28, having the formula reported in claim 1 and showing the X-ray diffraction pattern reported on Table 8.
Claim 19
Dependent Claim 21 words
18) New zeolites MB 28 according to claim 17, as prepared according to the methods of claims 3, 4 and 5.
Claim 20
Dependent Claim 28 words
19) New zeolites, defined as zeolites MB28, having the formula reported in claim 1 and showing the X-ray diffraction pattern reported on the Tables from 1 to 6.

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