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GB2151603A - Modified clay - Google Patents

Modified clay Download PDF

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Publication number
GB2151603A
GB2151603A GB8431326A GB8431326A GB2151603A GB 2151603 A GB2151603 A GB 2151603A GB 8431326 A GB8431326 A GB 8431326A GB 8431326 A GB8431326 A GB 8431326A GB 2151603 A GB2151603 A GB 2151603A
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United Kingdom
Prior art keywords
beryllium
layered clay
pillared
process according
clay
Prior art date
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GB8431326A
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GB2151603B (en
GB8431326D0 (en
Inventor
Martin Philip Atkins
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BP PLC
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BP PLC
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Publication of GB8431326D0 publication Critical patent/GB8431326D0/en
Publication of GB2151603A publication Critical patent/GB2151603A/en
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00Catalysts comprising molecular sieves
    • B01J29/04Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/049Pillared clays
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • B01J20/10Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
    • B01J20/16Alumino-silicates
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C41/00Preparation of ethers; Preparation of compounds having groups, groups or groups
    • C07C41/01Preparation of ethers
    • C07C41/02Preparation of ethers from oxiranes
    • C07C41/03Preparation of ethers from oxiranes by reaction of oxirane rings with hydroxy groups

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Catalysts (AREA)
  • Silicates, Zeolites, And Molecular Sieves (AREA)
  • Inorganic Chemistry (AREA)
  • Analytical Chemistry (AREA)
  • Dispersion Chemistry (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)

Abstract

A novel pillared layered clay having beryllium-containing pillars is produced by in a first step hydrolysing a hydrolysable compound of beryllium, for example a salt, and thereafter in a second step cation-exchanging a cation-exchangeable layered clay, for example a smectite, with the hydrolysate so- obtained. Pillared clays so produced are useful as catalysts, catalyst supports and adsorbents.

Description

SPECIFICATION Novel pillared layered clays, process for their production, and uses thereof The present invention relates to novel pillared layered clays or, as they are sometimes referred to, crosslinked interlayered clays, a process for their production and their use as catalysts, catalyst supports or sorbents.
Layered clays, that is clays having a lamellar structure with interlamellar spaces disposed therebetween in which pillars or crosslinks are substantially absent, are well-known as catalysts in organic reactions which are catalysed by protons. See for example our European patent publications Nos. 0031252 and 0031687. It is generally recognised that such clays when heated in air suffer irreversible collapse of their layered structures at temperatures of 180"C and above, the actual value of this temperature depending upon the nature of the exchangeable cation present in the interlamellar region of the structure. The collapse of the layered structure is associated with a loss in the catalytic activity of the clay.
Layered clays can also suffer from the disadvantage that they suffer particle/granule instability in the presence of polar liquids such as methanol or ethanol. This does not impair catalytic activity in batch or continuous reactions in which the catalyst particles are subject to agitation, thereby maintaining them in suspension. However, the catalyst particles have at some stage to be separated from the reactor product by filtration, centrifugation or other solid/liquid separation methods. For fixed bed operation, the layered clay catalyst must be mixed with suitable binders to ensure granule or pellet stability.
Also known from, for example, US Patents No. 4216188 and 4248739 are stabilised pillared layered clays, sometimes referred to as crosslinked interlayered clays in which the layers are separated and supported by "pillars" of monomeric, oligomeric or polymeric species derived from metal hydroxides. Such clays can inherently possess a higher degree of thermal stability and improved hydrothermal stability when compared with non-pillared layered clays. In USP 4248739 the use of the pillared layered clays as sorbents, catalysts and catalytic supports is described. The clays are said to be useful as hydrocarbon conversion catalysts for use in conventional catalytic cracking, hydrocracking, hydrotreating, isomerisation and reforming processes. Similar uses are described for the pillared clays of USP 4216188.Our published European Application No. 83970 describes their use as catalysts in a number of different reactions catalysed by protons, for example the production of esters by reaction of an olefin with a carboxylic acid and the production of alkylaromatic compounds by reaction of an aromatic compound with an olefin or an alcohol.
The present invention provides a pillared layered clay having beryllium-containing pillars.
The beryllium-containing pillars suitably may comprise oligomeric beryllium species.
In another aspect the present invention provides a process for the production of a pillared layered clay having beryllium-containing pillars which process comprises in a first step hydrolysing a hydrolysable compound of beryllium and thereafter in a second step cationexchanging a cation-exchangeable layered clay with the hydrolysate so-obtained.
The compound of beryllium which is to be hydrolysed may suitabley be a beryllium salt, for example beryllium sulphate, beryllium chloride or beryllium nitrate.
Hydrolysis of the beryllium compound may suitably be effected by reaction with either an aqueous or an aqueous alcoholic solution of an inorganic base. Suitable inorganic bases include oxides and hydroxides of metals of Groups I and II of the Periodic Table, for example sodium hydroxide. Other inorganic bases such as sodium carbonate may also be employed.
The ratio of the concentration of base, expressed in terms of moles of hydroxide per litre, to the concentration of beryllium, expressed in terms of gm ions of beryllium per litre, may suitably be in the range from 20:1 to 1:20, preferably in the range from 5:1 to 1:5, even more preferably about 2.5:1.
The hydrolysis may suitably be effected at ambient temperature, but elevated temperatures, suitably in the range from 30 to 90"C may be employed.
It is believed that the hydrolysis produces monomeric, dimeric and polymeric beryllium cations, the distribution of which in the hydrolysis can be influenced by the nature of the base and the ratio of the hydroxyl ion concentration to the beryllium ion concentration.
The layered clay as used in the second step of the process may be a natural layered clay or a synthetic layered clay. Of the many types of layered clays available (see for example 'Encyclopedia of Chemical Technology' [Kirk Othmer], 3rd Edition, published by John Wiley and Sons, pages 190-206) it is preferred to use the smectite class of layered clays, which may be either dioctahedral or trioctahedral. For an explanation as to the difference between dioctahedral and trioctahedral type clays reference is made to the book entitled 'The Chemistry of Clay-Organic Reactions' by B.K.G. Theng, published by John Wiley and Sons, New York-Toronto, at page 2. Examples of suitable smectite-type layered clays include montmorillonite, bentonite, belidellite, nontronite and hectorite.
Examples of suitable synthetic smectite-type layered clays and methods for their prepara tion are described in US Patent No. 3855147 (NL Industries). It is also possible to use a pillared layered clay in which the pillars are derived from other materials, for example those of US Patents Nos. 4216188 and 4248739.
The layered clay may be cation-exchanged with the hydrolysate using any technique known in the art, preferably at a temperature below 100"C, even more preferably at a tem- perature less than 50"C, most preferably at a temperaure about ambient. It will usually be found convenient to add the clay to the hydrolysate and leave it in contact therewith, preferably with stirring, for a period of from a few minutes to several days, preferably from 30 minutes to 6 hours.
The pillared clay so-obtained may thereafter be separated from the hydrolysate by conventional means, such as by centrifugation or filtration.
It is preferred in a final step to heat the pillared clay to a temperature suitably in the range from 250 to 450"C, preferably about 400on, for a period of, for example, from i to 1 2 hours to drive off water. The heating may suitably be carried out in air, oxygen or an inert gas, such as nitrogen.
Pillared layered clays in which the pillars contain beryllium may be used as catalysts in a wide variety of chemical reactions, for example reaction which are catalysed by protons. Example of reactions which are catalysed by protons include: (i) a process for the production of an ether by reacting either an olefin or an olefin oxide with an alcohol, (ii) a process for the production of an ether by conversion of either a primary or secondary aliphatic alcohol, a polyol or an olefin oxide, (iii) a process for the production of an alkyl aromatic compound by reacting an aromatic compound with either an alcohol or an olefin, (iv) a process for the production of an alcohol by reacting an olefin with water, (v) a process for the production of an ester by reacting either an olefin or an olefin oxide with a carboxylic acid, (vi) a process for the decomposition of hydroperoxides, (vii) a process for the production of alkylphenols by the alkylation of phenol, and (viii) a process for the transalkylation or dealkylation of alkyl aromatic hydrocarbons.
Further details of processes (i) to (vii) may be found in our copending European patent application Publication No. 83970 (BP Case No. 5306) and of process (viii) in our copending European Application No. 83307022.0 (BP Case No 5445), which are incorporated herein by reference.
Because the pillared interlayered clays according to the invention have a characteristic interlayer spacing and a substantiai micropore structure, they are also useful as adsorbents and as catalyst supports.
The invention will now be further illustrated by reference to the following Examples: Example 1 (i) Hydrolysis of beryllium sulphate Beryllium sulphate (8.89; 0.05 mole) was hydrolysed at 60"C in the presence of base (sodium carbonate or potassium hydroxide).
Samples were taken during the course of the hydrolysis and examined by beryllium NMR spectroscopy. Samples were taken: A. before addition of base, B. after addition of an amount of base corresponding to about 20% hydrolysis, and C. after addition of 2.5 mole equivalents of base (i.e. 13.149 Na2COX or 24.89 KOH) corresponding to substantially complete hydrolysis.
The NMR signal of aqueous beryllium (11) (Sample A) was assigned as reference (0 ppm). The partially hydrolysed sample (B) contained a small peak at 0.1 5 ppm assigned to the dimeric species and a large peak at Oppm assigned to the unreacted beryllium monomer. The substantially hydrolysed sample (C)- showed a large peak at 0.57 ppm which was assigned to the trimeric species with a small shoulder at Oppm indicating a trace of unreacted beryllium (11) monomer.
= = [mole equivalent of base]/[moles of be- ryllium= 2.5 (ii) Preparation of beryllium pillared layered clay The substantially hydrolysed beryllium solution (C) (500 ml, 0.5 molar) prepared as described in (i) above was added to a portion of natural sodium montmorillonite (Wyoming) (1009) at 60"C for 1 hour accompanied by rapid stirring. The suspension was cooled to room temperature and the clay decanted from the aqueous media. The clay was washed with deionised water (4 x 500 ml), dried in an oven at 80 to 100"C and subsequently calcined at 350"C.
XRD analysis showed the material to have a basal doo, spacing of about 1 3 Angstroms.
Example 2 The beryllium pillared layered clay (20 ml) obtained in Example 1 was charged to a reactor in a small continuous flow unit and ethanol/ethylene oxide (10:1 wt) was passed over the catalyst at 90 C with a contact time of about 1 5 minutes. A 63% conversion of ethylene oxide was obtained under these conditions. The percentage ratio of mono-: diglycol ether was 92:8 (wt).

Claims (9)

1. A pillared layered clay having beryllium-containing pi!lars.
2. A pillared layered clay according to claim 1 wherein the beryllium-containing pil lars comprise oligomeric beryllium species.
3. A process for the production of a pillared layered clay having beryllium-containing pillars which process comprises in a first step hydrolysing a hydrolysable compound of beryllium and thereafter in a second step cationexchanging a cation-exchangeable layered clay with the hydrolysate so-obtained.
4. A process according to claim 3 wherein the hydrolysable compound of beryllium is a beryllium salt.
5. A process according to either claim 3 or claim 4 wherein hydrolysis of the hydrolysable beryllium compound is effected by reaction with either an aqueous or an aqueous alcoholic solution of an inorganic base.
6. A process according to claim 5 wherein the ratio of the concentration of base, expressed in terms of moles of hydroxide per litre, to the concentration of beryllium, expressed in terms of g ions of beryllium per litre is in the range from 5:1 to 1:5.
7. A process according to any one of claims 3 to 6 wherein the layered clay is a smectite.
8. A process according to any one of claims 3 to 6 wherein the layered clay is a pillared clay in which the pillars are derived from another material.
9. A process according to any one of claims 3 to 8 wherein the layered clay is cation-exchanged with the hydrolysate at a temperature less than 50"C.
1 0. A process according to any one of claims 3 to 9 wherein the pillared clay is separated from the hydrolysate and heated to a temperature in the range from 250 to 450"C to drive off water.
GB8431326A 1983-12-16 1984-12-12 Modified clay Expired GB2151603B (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
GB8333614A GB8333614D0 (en) 1983-12-16 1983-12-16 Pillared layered clays

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GB2151603A true GB2151603A (en) 1985-07-24
GB2151603B GB2151603B (en) 1987-04-08

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4866020A (en) * 1987-03-26 1989-09-12 The British Petroleum Company P.L.C. Lithiated clays and uses thereof
EP0240359A3 (en) * 1986-04-04 1989-10-25 Exxon Research And Engineering Company A method of pillaring micas and the resulting pillared micas
US4952544A (en) * 1987-03-05 1990-08-28 Uop Stable intercalated clays and preparation method
US4957889A (en) * 1987-03-05 1990-09-18 Uop Stable intercalated clays and preparation method
US4980047A (en) * 1987-03-05 1990-12-25 Uop Stable intercalated clays and preparation method
US4995964A (en) * 1987-03-05 1991-02-26 Uop Midbarrel hydrocracking process employing rare earth pillared clays

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0240359A3 (en) * 1986-04-04 1989-10-25 Exxon Research And Engineering Company A method of pillaring micas and the resulting pillared micas
US4952544A (en) * 1987-03-05 1990-08-28 Uop Stable intercalated clays and preparation method
US4957889A (en) * 1987-03-05 1990-09-18 Uop Stable intercalated clays and preparation method
US4980047A (en) * 1987-03-05 1990-12-25 Uop Stable intercalated clays and preparation method
US4995964A (en) * 1987-03-05 1991-02-26 Uop Midbarrel hydrocracking process employing rare earth pillared clays
US4866020A (en) * 1987-03-26 1989-09-12 The British Petroleum Company P.L.C. Lithiated clays and uses thereof

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Publication number Publication date
GB2151603B (en) 1987-04-08
GB8431326D0 (en) 1985-01-23
GB8333614D0 (en) 1984-01-25

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