# US 8,772,192 B2 · Germanium silicalite catalyst and method of preparation and use

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- Number: US 8,772,192 B2
- Document ID: US8772192B2
- Status: Granted
- Kind: B2
- Application number: 13/537,184
- Filed: 2012-06-29
- Published: 2014-01-02
- Granted: 2014-07-08
- Earliest claimed: 2012-06-29
- Assignees: Saudi Basic Industries Corporation
- Applicants: Alla Khanmamedova; Scott Stevenson; Dustin Farmer; Mike Mier
- Inventors: Alla Khanmamedova; Scott Stevenson; Dustin Farmer; Mike Mier
- Web page: https://patentgrep.com/patent/US8772192B2

## CPC

- B01J 23/42: Platinum
- B01J 29/047: {Germanosilicates; Aluminogermanosilicates (B01J29/005 takes precedence)}
- C07C 2/76: by condensation of hydrocarbons with partial elimination of hydrogen
- C07C 2523/42: Platinum
- C07C 2529/035: Crystalline silica polymorphs, e.g. silicalites
- Y02P 20/52: using catalysts, e.g. selective catalysts
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A catalyst and its preparation and use are disclosed. The catalyst is a silicalite having germanium (Ge) included within the framework of the silicalite prepared in a particular manner. The catalyst may be used in a method of converting hydrocarbons wherein a hydrocarbon feed is contacted with the catalyst. The catalyst may be formed by preparing an aqueous reaction mixture of a silica-containing silicalite precursor material and a germanium source. The reactants of the reaction mixture are allowed to react. The reacted reaction mixture is heated under conditions to form crystals of a silicalite having germanium included within the framework of the silicalite. The crystals are then calcined to form the catalyst. In certain embodiments, a noble metal may be deposited upon the germanium-containing silicalite.

## Claims

### Claim 1

A catalyst comprising:
a silicalite having germanium (Ge) in a amount if from about 8% or less by weight included within the framework of the silicalite prepared by:
preparing an aqueous reaction mixture of a silica-containing silicalite precursor material and a germanium source;
allowing the reactants of the reaction mixture to react while maintaining a temperature of 55° C. or less;
adjusting the pH of the reacted reaction mixture, if necessary, so that the reacted reaction mixture has a pH of 12 or less;
heating the reacted reaction mixture under conditions to form crystals of a silicalite having germanium included within the framework of the silicalite; and
calcining the crystals.

### Claim 2 (depends on 1)

The catalyst of claim 1, wherein:
the germanium is present within the framework of the silicalite in an amount of from about 3% or less by weight.

### Claim 3 (depends on 1)

The catalyst of claim 1, wherein:
the germanium is present within the framework of the silicalite in an amount of at least about 0.05% by weight.

### Claim 4 (depends on 1)

The catalyst of claim 1, wherein:
any aluminum content of the silicalite provides a silica/alumina molar ratio of about 450:1 or greater.

### Claim 5 (depends on 1)

The catalyst of claim 1, wherein:
any aluminum content of the silicalite provides a silica/alumina molar ratio of about 1000:1 or greater.

### Claim 6 (depends on 1)

The catalyst of claim 1, further comprising:
a noble metal deposited upon the germanium-containing silicalite.

### Claim 7 (depends on 6)

The catalyst of claim 6, wherein:
the noble metal is present in an amount of from about 0.05% to about 3% by weight of the catalyst.

### Claim 8 (depends on 6)

The catalyst of claim 6, wherein:
the noble metal is present in an amount of from about 0.1% to about 2% by weight of catalyst.

### Claim 9 (depends on 6)

The catalyst of claim 6, wherein:
the noble metal is platinum.

### Claim 10 (depends on 1)

The catalyst of claim 1, wherein:
the catalyst contains no or less than 0.01% by weight of any fluorine.

### Claim 11 (depends on 1)

The catalyst of claim 1, wherein:
the pH of the reacted reaction mixture is adjusted to a pH of from about 9 to less than 12 prior to heating the reacted reaction mixture.

### Claim 12 (depends on 1)

The catalyst of claim 1, wherein:
the reactants of the reaction mixture are allowed to react while maintaining a temperature that does not exceed a temperature range of from about 30° C. to about 45° C.