DE1468748C3 - Crystalline, zeolitic, decomposed aluminosilicates precipitated from 1184743 - Google Patents

Crystalline, zeolitic, decomposed aluminosilicates precipitated from 1184743

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Publication number
DE1468748C3
DE1468748C3 DE1468748A DE1468748A DE1468748C3 DE 1468748 C3 DE1468748 C3 DE 1468748C3 DE 1468748 A DE1468748 A DE 1468748A DE 1468748 A DE1468748 A DE 1468748A DE 1468748 C3 DE1468748 C3 DE 1468748C3
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Prior art keywords
crystalline
aluminosilicates
zeolitic
decomposed
precipitated
Prior art date
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Expired
Application number
DE1468748A
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German (de)
Other versions
DE1468748A1 (en
DE1468748B2 (en
Inventor
James Edward Buffalo Boyle
Paul Eugene North Tonawanda Pickert
Jule Antone Buffalo Rabo
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Union Carbide Corp
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Union Carbide Corp
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Priority claimed from US862764A external-priority patent/US3130006A/en
Application filed by Union Carbide Corp filed Critical Union Carbide Corp
Publication of DE1468748A1 publication Critical patent/DE1468748A1/en
Publication of DE1468748B2 publication Critical patent/DE1468748B2/en
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Publication of DE1468748C3 publication Critical patent/DE1468748C3/en
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
    • B01J20/16—Alumino-silicates
    • B01J20/18—Synthetic zeolitic molecular sieves
    • B01J20/186—Chemical treatments in view of modifying the properties of the sieve, e.g. increasing the stability or the activity, also decreasing the activity
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
    • B01J29/084—Y-type faujasite
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2/00—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
    • C07C2/02—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition between unsaturated hydrocarbons
    • C07C2/04—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition between unsaturated hydrocarbons by oligomerisation of well-defined unsaturated hydrocarbons without ring formation
    • C07C2/06—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition between unsaturated hydrocarbons by oligomerisation of well-defined unsaturated hydrocarbons without ring formation of alkenes, i.e. acyclic hydrocarbons having only one carbon-to-carbon double bond
    • C07C2/08—Catalytic processes
    • C07C2/12—Catalytic processes with crystalline alumino-silicates or with catalysts comprising molecular sieves
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2/00—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
    • C07C2/54—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition of unsaturated hydrocarbons to saturated hydrocarbons or to hydrocarbons containing a six-membered aromatic ring with no unsaturation outside the aromatic ring
    • C07C2/64—Addition to a carbon atom of a six-membered aromatic ring
    • C07C2/66—Catalytic processes
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C4/00—Preparation of hydrocarbons from hydrocarbons containing a larger number of carbon atoms
    • C07C4/02—Preparation of hydrocarbons from hydrocarbons containing a larger number of carbon atoms by cracking a single hydrocarbon or a mixture of individually defined hydrocarbons or a normally gaseous hydrocarbon fraction
    • C07C4/06—Catalytic processes
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/02—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils characterised by the catalyst used
    • C10G11/04—Oxides
    • C10G11/05—Crystalline alumino-silicates, e.g. molecular sieves
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G35/00—Reforming naphtha
    • C10G35/04—Catalytic reforming
    • C10G35/06—Catalytic reforming characterised by the catalyst used
    • C10G35/095—Catalytic reforming characterised by the catalyst used containing crystalline alumino-silicates, e.g. molecular sieves
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G47/00—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions
    • C10G47/02—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions characterised by the catalyst used
    • C10G47/10—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions characterised by the catalyst used with catalysts deposited on a carrier
    • C10G47/12—Inorganic carriers
    • C10G47/16—Crystalline alumino-silicate carriers
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2529/00—Catalysts comprising molecular sieves
    • C07C2529/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites, pillared clays
    • C07C2529/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • C07C2529/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2529/00—Catalysts comprising molecular sieves
    • C07C2529/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites, pillared clays
    • C07C2529/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • C07C2529/60—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the type L

Description

Die Erfindung betrifft kristalline, zeoüthische AIummosilikate und deren Verwendung als Katalysator für die Spaltung von Kohlenwasserstoffen.The invention relates to crystalline, zeolite gummosilicates and their use as a catalyst for the splitting of hydrocarbons.

Zeoliihisehe Molekularsiebe sind natürliche oder synthetische kristalline Metallaluminosilikate mit weitgehend geordneten AlO1- und SiO4-Tetraedern, die über Sauerstoffatome vernetzt sind. Die Zwischenräume zwischen den Tetraedern sind vorder Entwässerung durch Wassermoleküle besetzt. Durch Entwässerung werden Kristalle erhalten, die von Kanälen von molekularen Abmessungen durchzogen sind. Die«; Kanäle bieten sehr große Oberflächen für die Adsorption von Frenidmolekülen, vorausgesetzt, daß die Kristallstruktur und damit die Öffnungen zu den inneren ^dsorptionsbereichen erhalten bleiben.Zeolite molecular sieves are natural or synthetic crystalline metal aluminosilicates with largely ordered AlO 1 and SiO 4 tetrahedra, which are cross-linked via oxygen atoms. The spaces between the tetrahedra are occupied by water molecules before drainage. By dewatering crystals are obtained, which are crisscrossed by channels of molecular dimensions. The"; Channels offer very large surfaces for the adsorption of frenid molecules, provided that the crystal structure and thus the openings to the inner areas of absorption are preserved.

Die Elektrovalenz des Aluminiums in der Struktur ist durch Einbeziehung eines Kations in den Kristall abgesältigt. In synthetischen zeolithischen Molekularsieben ist dieses Kation meistens ein Alkalimetallkation, z. B. Natrium oder Kalium oder deren Gemische. Die Kationen der synthetischen oder natürlichen Zeolithe können gegen andere mono-, di- oder trivalente Kationen ausgetauscht werden, deren physikalische Größe und Gestalt derart sind, daß sie in die intrakristallinen Durchgänge in der Aiuminosilikatstruktur diffundieren. In diesen Fällen wurde stets das ursprüngliche Metallkation entweder durch ein anderes Metallkation oder bei der Behandlung mit Säuren durch Wasserstoffkation ersetzt.The electrovalence of the aluminum in the structure is due to the inclusion of a cation in the crystal peeled off. In synthetic zeolitic molecular sieves this cation is mostly an alkali metal cation, z. B. sodium or potassium or mixtures thereof. The cations of synthetic or natural zeolites can be exchanged for other mono-, di- or trivalent cations, their physical size and shape are such that they diffuse into the intracrystalline passages in the aluminum inosilicate structure. In these cases the original metal cation was always replaced by another metal cation or replaced by a hydrogen cation when treated with acids.

Gegenstand der Erfindung sind kristalline, zeolithische, dekationisierte Aluminosilikate mit einem SiO2-A LOj-Molverhältnis von mehr als 3, Vorzugsweise mehr als 4,5, einem Verhältnis von monovalenten Kationen zu Aluminiumatomen von weniger als 0,9, vorzugsweise weniger als 0,7, einem Aluminosilikalgerüst, dessen Menge an Sauerstoffatomen um eine den entfernten Kationen äquivalente Menge vermindert worden ist und mit einer zur Adsorption von Benzol ausreichenden Porengröße.The invention relates to crystalline, zeolitic, decationized aluminosilicates with an SiO 2 -A LOj molar ratio of more than 3, preferably more than 4.5, a ratio of monovalent cations to aluminum atoms of less than 0.9, preferably less than 0, 7, an aluminosilical skeleton, the amount of oxygen atoms of which has been reduced by an amount equivalent to the removed cations and with a pore size sufficient for the adsorption of benzene.

Diese dekationisierlen zeolithischen Molekularsiebe werden beispielsweise nach dem Verfahren der deutschen Patentschrift 1 184 743 in der Weise hergestellt, daß man wenigstens 10% der Metallkationen eines Molekularsicbes mit einem SiO2-Al2O3-Verhältnis von mehr als 3 und einer zur Adsorption von Benzol ausreichenden Porengröße gegen Ammoniumionen austauscht und das Ammonium-ausgetauschte Molekularsieb auf Temperaturen zwischen 350 und 6000C, insbesondere 475 und 600°C, erhitzt. Als zeolithisches Molekularsieb wird hierbei bevorzugt von Zeolith Y (deutsche Patentschrift 1 089 929), Zeolith L (deutsche Patentschrift 1 100 009) oder dem natürlichen Zeolith Faujasit ausgegangen.These dekationisierlen zeolitic molecular sieves are produced, for example, according to the method of German patent specification 1,184,743 in such a way that at least 10% of the metal cations of a molecular sieve with an SiO 2 -Al 2 O 3 ratio of more than 3 and one for the adsorption of benzene exchanging pore size sufficient for ammonium ions and the ammonium-exchanged molecular sieve at temperatures between 350 and 600 0 C, in particular 475 and 600 ° C heated. Zeolite Y (German Patent 1 089 929), Zeolite L (German Patent 1 100 009) or the natural zeolite faujasite are preferably used as the zeolite molecular sieve.

In den neuen dekationisierten zeolithischen MoIekularsieben ist wenigstens ein Teil der Aluminiumatome nicht mehr durch kationische Substanzen abgesättigt. Trotzdem behalten überraschenderweise auch diese dekationisierten Molekularsiebe ihre Kristallstruktur bei. Ebenso wie die ihnen zugrunde lie-In the new decationized zeolitic molecular sieves there is at least some of the aluminum atoms no longer saturated by cationic substances. Still surprisingly retained these decationized molecular sieves also contribute their crystal structure. Just like the underlying

ao genden bekannten Molekularsiebtypen besitzen sie eine zur Adsorption von Benzol ausreichende Porengröße und sind infolgedessen in der Lage, größerc Moleküle beispielsweise Kohlenwasserstoffe zu adsorbieren. Das Siliziumdioxyd-Aluminiumtrioxyd-Moi-Ao lowing known molecular sieve types they have a sufficient pore size for the adsorption of benzene and are consequently able to adsorb larger molecules, for example hydrocarbons. The silicon dioxide-aluminum trioxide moi-

IS verhältnis dieser neuen Molekularsiebe beträgt melir als 3. vorzugsweise mehr als 4,5, ihr Verhältnis vn-i monovaleiv ι Metallkationen zu Aluminiumatomen ist kleiner s 0,9, zweckmäßig kleiner als 0,7, und vorzugsweise kleiner als 0,3.IS ratio of these new molecular sieves is melir as 3rd, preferably more than 4.5, their ratio vn-i monovaleiv ι metal cations to aluminum atoms is less than 0.9, suitably less than 0.7, and preferably less than 0.3.

Aus den vorstehenden Ausführungen ist klar ersichtlich, daß der Ausdruck «dekationisiert« sich auf de-i einzigartigen Zustand bezieht, in dem eine wesentliche Menge, d.h. wenigstens 10°',,, der Aluminiumatoie der Aluminosilicatstruktur nicht mit Kationen ass;>ziiert sind oder, anders ausgedrückt, in dem weniger als 90°/0 der Muminiumatome eines Metallalumii.nsilicats mit Kationen assoziiert sind. Zur Erzielung der besten katalytischen Wirksamkeit muß der Grad der Dekationisierung wenigstens 30°/0, vorzugsweise mehr.From the foregoing it is clear that the term "decationized" refers to the unique state in which a substantial amount, ie at least 10%, of the aluminum atom of the aluminosilicate structure is not cationic ; > are ciated or in other words, where less 90 ° / 0 of Muminiumatome a Metallalumii.nsilicats associated with cations. To achieve the best catalytic effectiveness, the degree of decationization must be at least 30 ° / 0 , preferably more.

betragen.be.

Gegenstand der Erfindung ist ferner die Verwendung dieser kristallinen zeolithischen dekationisierten AIuminosilikate als Katalysator für die Spaltung von Kohlenwasserstoffen. Weil die Poren der neuen dekationisierten Molekularsiebe gemäß der Erfindung groß genug sind, um die Kohlenwasserstoffmolekiilc zu adsorbieren und die umgelagerten Kohlenwasserstoffmoleküle zu desorbieren, eignen sie sich für die Spaltung sämtlicher Kohlenwasserstoffe, die ganzThe invention also relates to the use of these crystalline zeolitic decationized aluminosilicates as a catalyst for the splitting of hydrocarbons. Because the pores of the new Decationized molecular sieves according to the invention are large enough to remove the hydrocarbon molecules to adsorb and desorb the rearranged hydrocarbon molecules, they are suitable for the Splitting of all hydrocarbons, the whole

■i" oder teilweise von den Poren der Molekularsiebe der neuen Katalysatoren adsorbiert werden. Vor allem bei der hydrierenden Spaltung sind sie den bekannten Katalysatoren überlegen, da sie bei hohen Umsätzen vorwiegend zu den sehr erwünschten C3- und C1-Kohlenwasserstoffen führen.■ i "or partially adsorbed by the pores of the molecular sieves of the new catalysts. Especially in the case of hydrogenative cleavage, they are superior to the known catalysts, since at high conversions they predominantly lead to the very desirable C 3 and C 1 hydrocarbons.

Die Wärmebehandlung des Ammonium-ausgetauschten Molekularsiebs als letzten Schritt des Verfahrens zur Herstellung der neuen dekationisierten zeolithischen Molekularsiebe ks.in in situ bei der Spaltung der Kohlenwasserstoffe vorgenommen werden. Heat treatment of the ammonium-exchanged molecular sieve as the final step in the process for the production of the new decationized zeolitic molecular sieves ks.in in situ at the Cleavage of the hydrocarbons can be made.

An Hand des Beispieles sei die Erfindung näher erläutert:The invention is explained in more detail using the example:

Beispielexample

n-Heptan wurde bei den für die katalytische hydrierende Spaltung üblichen Reaktionstemperaturen einerseits mit einem dekationisierten Zeolith Y, andererseits mit einem handelsüblichen Katalysator umgesetzt. Beide Katalysatoren wurden vorher in Wasserstoff aktiviert. Die Ergebnisse sind in der nachstehenden Tabelle zusammengefaßt.n-Heptane was at the reaction temperatures customary for the catalytic hydrogenative cleavage reacted on the one hand with a decationized zeolite Y, on the other hand with a commercially available catalyst. Both catalysts were previously activated in hydrogen. The results are in the following Table summarized.

Diese Resultate lassen erkennen, daß der dekationisierte Zeolith Y bei niedrigerer Temperatur aktiver war als der handelsübliche Spaltkatalysator. Ferner bestand das Produkt aus den erwünschteren Propan- und Butankomponenten. Die Butanfraktion bestand zum großen Teil aus dem erwünschten Isobutan.These results indicate that the decationized zeolite Y is more active at the lower temperature was than the commercially available cracking catalyst. Furthermore, the product consisted of the more desirable propane and butane components. The butane fraction consisted largely of the desired isobutane.

33 1 4681 468 748748 üü
44th ito rito r 550550 Dekationisierter
Zeolith
Na(20)Y
450Decationized
Zeolite
Na (20) Y
450 lysator
ndelsüblicher Katalys:
peratur," C
500lyser
Customary catalyst:
temperature, "C
500 42
1242
12th Gebildete Produkte, Molprozent
0 „ C1 +- C, in C, — C4 Products formed, mole percent
0 "C 1 + - C, in C, - C 4 75
375
3 Kata
Ha
Reaktionstem
450Kata
Ha
Reaction stem
450 8
108th
10 4343 ' η Ci in Ci — C. ' η Ci in Ci - C. 4343 4
04th
0 4545 4040 11 „ C. in C1 — C1 11 "C. in C 1 - C 1 54
T> 54
T> 5050 45
4945
49 5555 0 „ IsO-C1 in C. 0 "IsO-C 1 in C. 1414th 50
4550
45 9292 5555 " „ nicht umgesetztes n-C7 " " Unconverted nC 7 9696

Claims (2)

Patentansprüche:Patent claims: 1. Kristalline, /eolithische liekationisierte AIuminosilikate mit einem SiOo-AI203-Mol\erhältnis ' >n mehr als 3. vorzugsweise mehr als 4,5, einem Verhältnis von monovalenten Kationen zu Aluminiumatomen von weniger als 0,9, vorzugsweise weniger als 0,7, einem Aluminosilikatgerüst. dessen Menge an Sauerstoffatomen um eine den entfernten Kationen äquivalente Menge vermindert worden ist und mit einer zur Adsorption von Benzol ausreichenden Porengröße.1. Crystalline, / eolithic, cationized aluminosilicates with an SiOo-Al 2 O 3 molar ratio> n more than 3. preferably more than 4.5, a ratio of monovalent cations to aluminum atoms of less than 0.9, preferably less than 0.7, an aluminosilicate framework. whose amount of oxygen atoms has been reduced by an amount equivalent to the removed cations and with a pore size sufficient for the adsorption of benzene. 2. Verwendung kristalliner, zeolithischer dekatlonisierter Aluminosilikate gemäß Anspruch 1 als Katalysatoren für die Spaltung von Kohlcnwasserstoffen. 2. Use of crystalline, zeolitic decatlonized Aluminosilicates according to Claim 1 as catalysts for the cleavage of hydrocarbons.
DE1468748A 1959-12-30 1960-12-29 Crystalline, zeolitic, decomposed aluminosilicates precipitated from 1184743 Expired DE1468748C3 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US862764A US3130006A (en) 1959-12-30 1959-12-30 Decationized molecular sieve compositions
DE1184743 1960-12-29

Publications (3)

Publication Number Publication Date
DE1468748A1 DE1468748A1 (en) 1970-06-18
DE1468748B2 DE1468748B2 (en) 1973-04-26
DE1468748C3 true DE1468748C3 (en) 1973-11-08

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DE1468748B2 (en) 1973-04-26

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SH Request for examination between 03.10.1968 and 22.04.1971
C3 Grant after two publication steps (3rd publication)
E77 Valid patent as to the heymanns-index 1977