# US 12,215,072 B2 · Method and system for the synthesis of methanol

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- Number: US 12,215,072 B2
- Document ID: US12215072B2
- Status: Granted
- Kind: B2
- Application number: 17/613,702
- Filed: 2020-05-26
- Published: 2022-07-14
- Granted: 2025-02-04
- Earliest claimed: 2019-05-28
- Assignees: Gascontec GmbH; Thyssenkrupp Uhde GmbH
- Applicants: Gascontec GmbH; thyssenkrupp Uhde GmbH
- Inventors: Alexander Schulz
- Web page: https://patentgrep.com/patent/US12215072B2

## CPC

- C01B 3/36: using oxygen; using mixtures containing oxygen as gasifying agents
- C07C 29/152: characterised by the reactor used
- B01J 19/2465: {externally, i.e. the mixture leaving the vessel and subsequently re-entering it}
- C01B 3/382: Processes with two or more reaction steps, of which at least one is catalytic, e.g. steam reforming and partial oxidation
- C01B 3/56: by contacting with solids; Regeneration of used solids
- C07C 29/15: by reduction of oxides of carbon exclusively
- C07C 29/1518: {one step being the formation of initial mixture of carbon oxides and hydrogen for synthesis}
- C01B 2203/0244: the reforming step being an autothermal reforming step, e.g. secondary reforming processes
- C01B 2203/025: containing a partial oxidation step
- C01B 2203/043: Regenerative adsorption process in two or more beds, one for adsorption, the other for regeneration
- C01B 2203/061: Methanol production
- Y02E 60/32: Hydrogen storage
- Y02P 20/50: Improvements relating to the production of bulk chemicals
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A method for the synthesis of methanol, wherein a carbonaceous energy source flow is supplied to a synthesis gas reactor arrangement for obtaining a synthesis gas flow having hydrogen and carbon oxides, wherein the synthesis gas flow is supplied to a thermal recovery apparatus for recovering heat from the synthesis gas flow and then to a synthesis gas compressor for pressure increase. The synthesis gas flow is supplied at least in part to a first reactor stage of a methanol reactor arrangement for partial conversion to methanol, a residual gas flow having unreacted carbon oxides being obtained from the methanol reactor arrangement, which residual gas flow is supplied to a recycling compressor for increasing its pressure, the pressure-increased gas flow being supplied to the methanol reactor arrangement for partial conversion to methanol, a recovery flow from an unreacted residual gas being supplied to the first reactor stage of a hydrogen recovery arrangement to obtain a H-recycling flow. The

## Claims

### Claim 1

A method for the synthesis of methanol, wherein a carbon-containing energy carrier stream is fed to a synthesis gas reactor arrangement for obtaining a synthesis gas stream with hydrogen and oxides of carbon, wherein the synthesis gas stream is fed to a heat recovery device for recovering heat from the synthesis gas stream and thereafter to a synthesis gas compressor for increasing pressure, wherein at least a portion of the pressure-increased synthesis gas stream is fed to a first reactor stage of a methanol reactor arrangement for partial conversion into methanol, wherein a residual gas stream with unreacted oxides of carbon is obtained from the methanol reactor arrangement, the residual gas stream being fed to a recycle compressor for increasing the pressure of the residual gas stream, wherein the pressure-increased residual gas stream is fed to the methanol reactor arrangement for partial conversion into methanol, wherein a recovery stream from an unreacted residual gas from the first reactor stage is fed to a hydrogen recovery arrangement for obtaining a H recycle stream, the H recycle stream having unreacted hydrogen from the unreacted residual gas, the unreacted hydrogen of the H recycle stream being fed again to the first reactor stage for at least partial conversion into methanol, wherein the pressure of at least a portion of the unreacted hydrogen of the H recycle stream from the first reactor stage up to its feed again into the first reactor stage is increased along with the unreacted oxides of carbon by means of the recycle compressor.

### Claim 2 (depends on 1)

The method according to claim 1, wherein the methanol reactor arrangement comprises a methanol separation device for obtaining the unreacted residual gas from the first reactor stage and a raw methanol stream from the first reactor stage, wherein the methanol separation device comprises a condensation device for obtaining the unreacted residual gas from the first reactor stage and the raw methanol stream from the first reactor stage by condensation.

### Claim 3 (depends on 1)

The method according to claim 1, wherein a portion of the pressure-increased residual gas stream is diverted and fed to the synthesis gas reactor arrangement, wherein the diverted portion of the pressure-increased residual gas stream is fed to the energy carrier stream.

### Claim 4 (depends on 1)

The method according to claim 1, wherein the methanol reactor arrangement has a plurality of reactor stages for the synthesis of methanol which are operationally connected in series, wherein the recycle compressor is operationally disposed between two reactor stages, wherein by the methanol separation device, a respective unreacted residual gas is obtained from each of the plurality of reactor stages.

### Claim 5 (depends on 4)

The method according to claim 4, wherein the H recycle stream is fed to the unreacted residual gas a reactor stage which is operationally downstream of the first reactor stage, wherein the H recycle stream is fed to the recycle compressor together with the residual gas stream for increasing pressure.

### Claim 6 (depends on 4)

The method according to claim 4, wherein the residual gas stream is obtained from a reactor stage which is operationally downstream of the first reactor stage, wherein the recycle compressor feeds the pressure-increased residual gas stream to the first reactor stage.

### Claim 7 (depends on 6)

The method according to claim 6, wherein the residual gas stream is obtained from a reactor stage of the plurality of reactor stages which is in the last operational position.

### Claim 8 (depends on 1)

The method according to claim 1, wherein at least a portion of the recovery stream is diverted from the unreacted residual gas of the first reactor stage, wherein at least a portion of the recovery stream is diverted operationally upstream of the recycle compressor.

### Claim 9 (depends on 8)

The method according to claim 8, wherein the recovery stream is fed to the hydrogen recovery arrangement at a feed pressure which is higher than a residual gas pressure at which the residual gas stream is obtained from the methanol reactor arrangement, wherein at least a portion of the recovery stream is diverted out of the residual gas stream operationally downstream of the recycle compressor.

### Claim 10 (depends on 1)

The method according to claim 1, wherein the H recycle stream is fed to the synthesis gas stream which has been pressure-increased.

### Claim 11 (depends on 1)

The method according to claim 1, characterized in that for obtaining the synthesis gas stream, an oxygen-containing stream is fed to the synthesis gas reactor arrangement, in wherein in the synthesis gas reactor arrangement, the synthesis gas stream is obtained by means of autothermal reforming or a partial oxidation of the carbon-containing energy carrier stream, wherein the oxygen-containing stream is obtained from an air separation device for obtaining a stream of oxygen from ambient air.

### Claim 12 (depends on 1)

The method according to claim 1, wherein the H recycle stream is fed to the energy carrier stream, operationally upstream of the synthesis gas reactor arrangement, in that the hydrogen recovery arrangement outputs a purge stream which is discharged for combustion.

### Claim 13 (depends on 1)

The method according to claim 1, wherein the H recycle stream has a higher molar proportion of hydrogen than the recovery stream, wherein the H recycle stream has a higher molar proportion of hydrogen than the purge stream.

### Claim 14 (depends on 1)

The method according to claim 1, wherein the hydrogen recovery arrangement has a pressure swing adsorption device for obtaining the H recycle stream from the recovery stream.

### Claim 15 (depends on 1)

The method according to claim 1, characterized in that the pressure of the unreacted hydrogen of the recovery stream from the first reactor stage up to its feed again into the first reactor stage is increased exactly once along with the unreacted oxides of carbon by means of the recycle compressor.

### Claim 16

A plant for the synthesis of methanol, with a synthesis gas reactor arrangement for obtaining a synthesis gas stream with hydrogen and oxides of carbon from a carbon-containing energy carrier stream, with a synthesis gas compressor for increasing the pressure of the synthesis gas stream, with a methanol reactor arrangement which has a first reactor stage, with a heat recovery device for recovering heat from the synthesis gas stream, with a hydrogen recovery arrangement and with a recycle compressor, wherein at least a portion of the pressure-increased synthesis gas stream is fed to the first reactor stage for partial conversion into methanol, wherein a residual gas stream with unreacted oxides of carbon is obtained from the methanol reactor arrangement, the residual gas stream being fed to the recycle compressor for increasing the pressure of the residual gas stream, wherein the pressure-increased residual gas stream is fed to the methanol reactor arrangement for partial conversion into methanol, wherein the synthesis gas stream is fed to the heat recovery device and thereafter to the synthesis gas compressor, wherein a recovery stream from an unreacted residual gas from the first reactor stage is fed to the hydrogen recovery arrangement for obtaining a H recycle stream, the H recycle stream having unreacted hydrogen from the unreacted residual gas, the unreacted hydrogen of the H recycle stream being fed again to the first reactor stage for at least partial conversion into methanol, wherein the pressure of at least a portion of the unreacted hydrogen of the H recycle stream from the first reactor stage up to its feed again into the first reactor stage is increased along with the unreacted oxides of carbon by means of the recycle compressor.
