# US 8,785,708 B2 · Process for preparing C2- to C4- olefins from a feed stream comprising oxygenates and steam

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- Number: US 8,785,708 B2
- Document ID: US8785708B2
- Status: Granted
- Kind: B2
- Application number: 11/909,629
- Filed: 2006-02-28
- Published: 2010-09-16
- Granted: 2014-07-22
- Earliest claimed: 2005-04-06
- Assignees: Lurgi GmbH
- Applicants: Martin Rothaemel; Walter Boll; Gerhard Birke; Harald Koempel; Waldemar Liebner; Hermann Bach
- Inventors: Martin Rothaemel; Walter Boll; Gerhard Birke; Harald Koempel; Waldemar Liebner; Hermann Bach
- Web page: https://patentgrep.com/patent/US8785708B2

## CPC

- C07C 1/20: starting from organic compounds containing only oxygen atoms as heteroatoms
- C07C 2529/70: of types characterised by their specific structure not provided for in groups C07C2529/08 - C07C2529/65
- Y02P 20/52: using catalysts, e.g. selective catalysts
- Y02P 30/20: using bio-feedstock
- Y02P 30/40: Ethylene production
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

In a process for the preparation of C2- to C4-olefins, a feed stream comprising oxygenates and steam is passed through at least one fixed-bed zone comprising zeolite catalyst, where the oxygenates are converted catalytically into olefins with high selectivity for lower olefins, and the reaction mixture leaving the fixed-bed zone is separated into a first product stream comprising C2- to C3-olefins and inert gas components, at least one second product stream comprising C4+-olefins, and a third product stream consisting of aqueous phase. In order to improve the yield of lower olefins, the aim is to regulate the temperature of the catalytic reaction in accordance with a target temperature value in the range from 440 to 520° C. specified for the reaction mixture exiting the fixed-bed zone by means of a supplementary stream consisting of olefins and inert gas components fed into the feed stream.

## Claims

### Claim 1

Process for the preparation of C2- to C4-olefins from a feed stream comprising vapor-form oxygenates and steam and having a temperature of from 280 to 480° C., which is passed through at least one fixed-bed zone (3) arranged in a reactor (2) and formed from a bed of granular, shape-selective zeolite catalyst of the pentasil type, and the oxygenates are converted catalytically into olefins with high selectivity for lower olefins at a reaction temperature of from 350 to 550° C. and the reaction mixture exiting the reactor is separated into a first product stream comprising C2- to C3-olefins and inert gas components, at least one further, second product stream comprising C4+-olefins, and a third product stream consisting of aqueous phase, characterized in that a reaction pressure of from 1.0 to 3.0 bara prevails at the entry of the feed stream into the fixed-bed zone (3) and a reaction pressure of from 0.5 to 2.0 bara prevails at the exit of the reaction mixture from the fixed-bed zone, and the temperature of the catalytic reaction is regulated in accordance with a target temperature value in the range from 440 to 520° C. specified for the reaction mixture exiting the fixed-bed zone by means of a supplementary stream comprising C4+ olefins and inert gas components fed into the feed stream, wherein the target temperature value for the reaction mixture exiting the reactor is measured by means of a temperature sensor beneath the catalyst fixed bed and the temperature of the feed stream entering the reactor and flowing through the catalyst fixed bed is measured by means of a temperature sensor arranged above the catalyst mixed bed.

### Claim 2 (depends on 1)

Process according to claim 1, wherein the target temperature value is in the range from 480 to 495° C.

### Claim 3 (depends on 1)

Process according to claim 1 wherein, the C4+-olefins in the second product stream together with the inert gas components and the ethylene in the first product stream are recycled into the feed stream as supplementary stream.

### Claim 4 (depends on 1)

Process according to claim 1 wherein the inert gas components employed comprise steam, nitrogen, helium, neon, argon, hydrogen, carbon monoxide, carbon dioxide, C1- to C4-paraffins and mixtures thereof.

### Claim 5 (depends on 1)

Process according to claim 1 wherein the supplementary stream comprises C2- to C8-olefins.

### Claim 6 (depends on 5)

Process according to claim 5 wherein the supplementary stream further comprises C2-olefins and C4- to C6-olefins.

### Claim 7 (depends on 5)

Process according to claim 5 wherein the supplementary stream further comprises C1- to C8-paraffins.

### Claim 8 (depends on 5)

Process according to claim 5 wherein the supplementary stream further comprises C5- to C8-naphthenes.

### Claim 9 (depends on 5)

Process according to claim 5 wherein the supplementary stream further comprises C6- to C7 aromatic compounds.

### Claim 10 (depends on 1)

Process according to claim 1 wherein by-product streams arising in thermal cracking, catalytic cracking or similar processes are employed as supplementary stream.

### Claim 11 (depends on 1)

Process according to claim 1 wherein process-inherent recycling streams are employed as supplementary stream.

### Claim 12 (depends on 1)

Process according to claim 1 wherein the throughput of the oxygenates present in the feed stream is from 0.1 to 10 kg, per hour and per kg of catalyst employed.

### Claim 13 (depends on 12)

Process according to claim 12 wherein the throughput of the oxygenates is from about 0.3 to 1.5 kg/her per kg of catalyst used.

### Claim 14 (depends on 1)

Process according to claim 1 wherein the feed stream fed to a reactor having a plurality of fixed-bed zones is split into a number of feed sub-streams corresponding to the number of fixed-bed zones, and each feed sub-stream is fed to a corresponding fixed-bed zone, the reaction mixture discharged from a fixed-bed zone is fed to the subsequent fixed-bed zone, and the reaction mixture discharged from the final fixed-bed zone in the downstream direction is fed to a separation unit, a supplementary stream comprising olefins and inert gas components is split into a number of supplementary sub-streams corresponding to the number of feed sub-streams, and each supplementary sub-stream is fed into a corresponding feed sub-stream or into the reaction mixture exiting a fixed-bed zone and fed to the subsequent fixed-bed zone.

### Claim 15 (depends on 14)

Process according to claim 14 wherein the reactor has between two to six fixed bed zones.

### Claim 16 (depends on 1)

Process according to claim 1 wherein the oxygenates are selected from methanol, dimethyl ether and mixtures thereof.

### Claim 17 (depends on 1)

Process according to claim 1 wherein the reaction temperature is in the range of about 420° C. to about 490° C.

### Claim 18 (depends on 1)

Process according to claim 1 wherein the C2- to C4-olefin that is produced in the process is propylene.

### Claim 19 (depends on 1)

Process according to claim 1 wherein the inert gas components in the supplementary stream comprise one or more of steam, nitrogen, helium, neon, argon, hydrogen, carbon monoxide and carbon dioxide.
