CN116286107A - Multistage membrane separation carbon capture process applied to synthesis gas - Google Patents
Multistage membrane separation carbon capture process applied to synthesis gas Download PDFInfo
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- CN116286107A CN116286107A CN202310303218.3A CN202310303218A CN116286107A CN 116286107 A CN116286107 A CN 116286107A CN 202310303218 A CN202310303218 A CN 202310303218A CN 116286107 A CN116286107 A CN 116286107A
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
- C10K1/00—Purifying combustible gases containing carbon monoxide
- C10K1/002—Removal of contaminants
- C10K1/003—Removal of contaminants of acid contaminants, e.g. acid gas removal
- C10K1/005—Carbon dioxide
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/504—Carbon dioxide
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
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Abstract
A multistage membrane separation carbon capture process applied to synthesis gas belongs to the field of coal gasification decarburization hydrogen production, and can solve the problems of overhigh energy consumption and complex system of the existing carbon capture. Is realized by equipment such as a hydrogen film, a carbon film, a compressor, a cooler, a pipeline and the like. The synthesis gas containing hydrogen and carbon dioxide firstly enters the carbon film after being cooled, the residual gas of the carbon film is sent out as a hydrogen product, and the gas of the permeation side enters the secondary hydrogen film after being compressed. Pressurizing the permeation side of the second-stage hydrogen membrane, then entering the third-stage hydrogen membrane, sending out the material flow of the permeation side of the third-stage hydrogen membrane as a carbon dioxide product, and returning the permeation sides of the second-stage hydrogen membrane and the third-stage hydrogen membrane to the feeding side after compression. The invention gives play to the advantages of membrane technology by reasonably matching different membranes, ensures that the circulating gas flow is controlled in a smaller range, hydrogen and carbon dioxide products are obtained from the residual permeation side, has energy consumption far lower than that of a membrane separation technology using a single membrane type, and can simultaneously realize higher CO 2 Purity and higher CO 2 The recovery rate is high, and the recovery rate is high,the carbon capture cost is lower than 15$/t and is far lower than that of the conventional absorption method.
Description
Technical Field
The invention belongs to the field of coal gasification hydrogen production, and particularly relates to a membrane separation carbon capture process applied to synthesis gas, which is suitable for carbon dioxide capture and hydrogen purification in the situations of coal-to-hydrogen production, natural gas-to-hydrogen production, coal gasification combined cycle power plants and the like. By reasonably selecting the hydrogen preferential osmosis membrane and the carbon dioxide preferential osmosis membrane,and the operating parameters are reasonably controlled, the purity of over 96 percent and the recovery rate of over 90 percent can be realized on the basis of the prior commercial membrane material, and the recovery cost is reduced to 15$/t CO under the condition of considering the liquefaction of carbon dioxide 2 。
Background
With the increasing consumption of fossil energy, CO 2 Environmental problems such as greenhouse effect caused by emission are attracting more and more attention, wherein CO discharged by power plant flue gas 2 Global CO 2 Over 70% of emissions, which plays a key role in global warming. As a large country for producing and consuming coal, the 2021-year coal resource yield of China reaches 41.3 hundred million tons, and the coal occupies 56% of the total energy consumption of China. Coal resources mined every year in China are 60% used in the power generation field, but CO caused by coal-fired power plants 2 Emission is currently the main problem restricting the traditional thermal power generation mode. Under the large background of energy conservation and emission reduction, the CO aiming at the traditional thermal power generation is researched 2 The emission reduction method is more and more paid attention to all countries in the world, but the existing absorption method which can be applied on a large scale has complex working steps, so that the investment is high, the energy consumption in the regeneration process after absorption is very large, and the development of the carbon capture technology of the absorption method is severely restricted.
In terms of the carbon capture pathway, CO is captured from coal-fired power plants 2 There are three potential approaches, post-combustion capture, pre-combustion capture, and oxygen-enriched fuel combustion. Post-combustion capture allows for retrofitting already operating plants, but at near atmospheric pressure, CO 2 The concentration is only 10-20%, and an additional pressurizing process is required for the low driving force of the capturing process, thereby resulting in high energy consumption. In oxyfuel combustion, by using O 2 Instead of air, almost pure CO can be obtained 2 The key problem to be solved is to produce pure O prior to combustion of the fuel for separation 2 . The pre-combustion is typically performed in an IGCC power plant, which has the advantages of higher energy production efficiency, low pollutant emissions and high fuel flexibility. In pre-combustion capture, the coal is first transformed into H by gasification 2 And CO 2 H and H 2 0、H 2 S mixture, thenBy removal of CO 2 Pure H after waiting for substances 2 And enters the gas turbine engine. Due to the higher pressure of the synthesis gas and the CO 2 The concentration is about 40%, and is considered to be the most potential carbon capture mode of the power plant. In IGCC plants, the gas leaving the shift reactor is typically at a pressure of 30-50Bar, containing about 40% CO 2 . Separation of CO from the gas stream, as compared to separation from flue gas 2 Easier and lower cost, pre-combustion carbon capture is the most promising carbon emission reduction approach.
Several CO's currently available 2 The separation technology can be divided into an absorption method, an adsorption method, a membrane separation method and a low-temperature condensation method, wherein the membrane separation method has the advantages of simple operation, low energy consumption, no pollution and the like, and is regarded as a carbon capturing mode with the most development prospect.
Although various kinds of CO having excellent properties 2 N 2 、CO 2 /H 2 H and H 2 /CO 2 Separation membrane polymeric materials are continually being proposed and improved, but due to the Trade-off effect between permeability coefficient and selectivity, it is difficult to rely solely on single stage membranes to function in the carbon capture field. Researchers have achieved CO by increasing the number of membrane separation stages 2 The product achieves the aim of higher purity and recovery rate at the same time, but the excessive number of stages is limited in energy consumption reduction, and the complexity is increased, so that the product is difficult to be applied to actual industrial production. Meanwhile, different membrane materials are different in permeation rate for different gases, different components are required to be separated by means of pressure difference at two sides in a membrane separation device, obvious pressure difference exists between a permeation side and a feeding end, the permeation side pressure is always normal pressure, and therefore if a permeation side material flow has higher pressure requirement, the problem of higher compression energy consumption of subsequent products can be caused. Therefore, how to design the process flow with the highest competitiveness by adopting a high-efficiency and reliable design method is the key for realizing carbon capture of the membrane process.
In view of the above, it is desirable to design a process with low energy consumption and moderate process complexity to meet the practical industrial requirements of decarbonizing and producing hydrogen from synthesis gas.
Disclosure of Invention
In order to solve the problems of high energy consumption and large environmental pollution of the existing carbon capture technology, the invention discloses a process for realizing high-efficiency and low-energy-consumption decarburization of synthesis gas by utilizing different membrane combinations, and hydrogen and carbon dioxide are obtained from the residual permeation side in the process, so that the process has the advantages of low energy consumption and low cost.
In order to achieve the above purpose, the invention adopts the following technical scheme:
a multistage membrane separation carbon capture process applied to synthesis gas, wherein the main components in the gasified synthesis gas are hydrogen with the volume fraction of 50-70% and carbon dioxide with the volume fraction of 30-50%. The process is realized by a multistage membrane separation carbon capture system, and the multistage membrane separation carbon capture system comprises a first cooler, a first stage membrane separation unit, a first compressor, a second cooler, a second stage membrane separation unit, a second compressor, a third cooler, a third stage membrane separation unit, a third compressor, a fourth cooler and a fourth compressor.
In the invention, after the synthesis gas S1 and the recycle gas S8 are mixed, the mixture is firstly cooled by a first cooler 1 and then enters a first-stage membrane separation unit 2 for hydrogen product purification, carbon dioxide preferentially permeates in the first-stage membrane separation unit 2, the high-purity hydrogen product S2 is arranged on the permeation side, and the gas S3 with higher carbon dioxide concentration is arranged on the permeation side. The gas S3 on the permeation side of the primary membrane enters a second cooler 4 after being pressurized by a first compressor 3, and enters a secondary membrane separation unit 5 to further purify CO2 after being cooled by the second cooler 4, at the moment, hydrogen in the secondary membrane separation unit is permeated preferentially, the gas S5 on the permeation side of the secondary membrane is taken as recycle gas, and the residual side of the permeation side of the secondary membrane contains higher concentration CO 2 The residual gas S4 after being compressed by the second compressor 6 and cooled by the third cooler 7 enters the three-stage membrane separation unit 8. The hydrogen in the three-stage membrane separation unit 8 is preferentially permeated to obtain three-stage membrane permeation side gas S7, the final purification of the carbon dioxide product is completed, and the high-purity hydrogen product S6 on the permeation side is sent out after being pressurized by the third compressor 9 and cooled by the fourth cooler 10. Finally, the second-stage membrane permeation side gas S5 and the third-stage membrane permeation side gas S7 are mixed to form a recycle gas S8, and the recycle gas is pressurized by the fourth compressor 11 and returned to the raw material side to be mixed with the raw material gas S1.
Furthermore, the membranes in each stage of membrane separation units in the process can be flat plates, spiral rolls or hollow fiber type. Two different types of membrane materials are selected for process design aiming at the performances of components in the synthesis gas and the existing membrane materials, wherein the two membrane materials are a carbon dioxide preferential permeation membrane (also a carbon membrane) and a hydrogen preferential permeation membrane (also a hydrogen membrane), namely carbon dioxide is more preferential permeation in the carbon membrane than hydrogen, and hydrogen is preferential permeation in the hydrogen membrane as a rapid permeation body.
Furthermore, the primary membrane separation unit adopts a carbon dioxide preferential permeation membrane, and the secondary and tertiary membrane separation units adopt a hydrogen preferential permeation membrane.
Further, the pressure of the synthesis gas is 2.0-6.0MPa, and the composition is 50-70% of hydrogen and 30-50% of carbon dioxide. Wherein H in hydrogen film 2 /CO 2 Selectivity is 5-20, CO in carbon film 2 /H 2 The selectivity is 10-14. The inlet pressure of the second-stage membrane separation unit 5 is 1-3MPa, the inlet pressure of the third-stage membrane separation unit 8 is 2-5MPa, and the outlet pressure of each stage of membrane separation unit is close to atmospheric pressure. For reasonably collocating membrane materials, firstly, a relatively high hydrogen product with components accounting for relatively high is obtained from the high-pressure permeation residual side of the first-stage membrane separation unit 2, and the rest gas enters the second-stage membrane separation unit and the third-stage membrane separation unit after being compressed, and CO 2 The product is obtained from high-pressure osmosis measurement, the smaller circulating gas flow determines the lower energy consumption of the system, and the energy consumption is lower than 1GJ/t CO 2 。
Further, in the first, second, third and fourth compressors: each compressor system at least comprises one compressor, when the pressure is higher, a plurality of compressors and coolers among the compressors are adopted, and redundant compression heat in the compression process is taken out in time, so that the compression energy consumption is saved.
The beneficial effects of the invention are as follows:
the process flow provided by the invention can solve the problems of overhigh energy consumption and complex system of the existing carbon capture. The invention gives play to the advantages of membrane technology by reasonably matching different membranes, so that the circulating gas flow is controlled in a smaller range, and hydrogen and carbon dioxide products are obtained from the residual side, so that the energy consumption is far lower than that of a membrane separation technology using a single membrane type, and the invention can simultaneously realizeHigher CO 2 Purity and higher CO 2 The recovery rate is lower than 15$/t carbon capture cost and is far lower than that of the conventional absorption method.
Drawings
Fig. 1 shows a process principle flow chart of the carbon capture membrane separation process in the invention.
Reference numerals: 1 a first cooler; a first-stage membrane separation unit; 3 a first compressor; 4 a second cooler; a 5-stage membrane separation unit; 6 a second compressor; 7 a third cooler; a third-stage membrane separation unit; 9 a third compressor; a fourth cooler 10; 11 a fourth compressor; s1 raw material gas, S2 hydrogen product, S3 first-stage membrane permeation gas, S4 second-stage membrane permeation residual gas, S5 second-stage membrane permeation gas, S6 third-stage membrane permeation residual gas, S7 third-stage membrane permeation gas and S8 circulating flow.
Detailed Description
Preferred embodiments of the present invention are described below with reference to the accompanying drawings. It should be understood by those skilled in the art that these embodiments are merely for explaining the technical principles of the present invention, and are not intended to limit the scope of the present invention.
Example 1
In the synthesis gas feed gas, H 2 Content of 60%, CO 2 Content 40%, flow 28390kmol/h, CO by adopting the membrane separation carbon capture process 2 The separation requirement is 96% purity and 90% recovery rate, after the synthetic gas raw material is mixed with circulating gas, the mixture is firstly cooled to room temperature by a cooler, then is fed into a primary carbon film at 3.0MPa pressure, and CO 2 The components permeate preferentially, and CO is obtained on the low-pressure permeation side of the primary membrane separation unit 2 73% primary permeate gas and residual non-permeate CO 2 The high-pressure residual permeate gas with the content of 6% is sent out as a hydrogen product, the first-stage permeate gas enters a first compressor for compression, is pressurized to 2.0MPa, is cooled to room temperature by a first cooler and enters a second-stage hydrogen membrane, hydrogen is preferentially permeated, and CO is obtained at the low-pressure permeate side of a second-stage membrane separation unit 2 A second-level permeation gas with the content of 20 percent, and CO is obtained at the high-pressure permeation residual side 2 Higher purity CO at 78% 2 The material flow is cooled after being pressurized to 3.6MPa by a second compressorCooling the reactor to room temperature, entering a three-stage hydrogen membrane, allowing hydrogen to permeate preferentially, and obtaining CO on the low-pressure permeation side of the three-stage membrane separation unit 2 Three-stage permeation gas with 37% content, and measuring CO under high pressure 2 High CO content of 96% 2 A purity stream. Mixing the secondary permeation air and the tertiary permeation air, pressurizing to 3MPa by a fourth compressor, mixing with synthesis gas, mixing with CO 2 The 33% gas was cooled to room temperature in the feed cooler and returned to the feed side. Can simultaneously realize 96 percent of purity and 90 percent of recovery rate.
The logistics details are given below:
TABLE 5 Process flow information
When the method is implemented, the higher recovery rate can be realized at the same time of higher purity, and compared with the current situation of high energy consumption of the existing carbon capture process, the method has remarkable improvement effect.
The examples described above represent only embodiments of the invention and are not to be understood as limiting the scope of the patent of the invention, it being pointed out that several variants and modifications may be made by those skilled in the art without departing from the concept of the invention, which fall within the scope of protection of the invention.
Claims (7)
1. The multistage membrane separation carbon capture process applied to the synthesis gas is characterized by being realized by a multistage membrane separation carbon capture system, wherein the multistage membrane separation carbon capture system comprises a first cooler (1), a first-stage membrane separation unit (2), a first compressor (3), a second cooler (4), a second-stage membrane separation unit (5), a second compressor (6), a third cooler (7), a third-stage membrane separation unit (8), a third compressor (9), a fourth cooler (10) and a fourth compressor (11); the specific process flow is as follows:
after being mixed with the recycle gas S8, the synthesis gas S1 is firstly cooled by a first cooler (1) and then enters a first-stage membrane separation unit(2) Purifying a hydrogen product, wherein carbon dioxide preferentially permeates in a primary membrane separation unit (2), the high-purity hydrogen product S2 is arranged on the permeate side, and the gas S3 with higher carbon dioxide concentration is arranged on the permeate side; the gas S3 on the permeation side of the primary membrane enters a second cooler (4) after being pressurized by a first compressor (3), and enters a secondary membrane separation unit (5) to further purify CO2 after being cooled by the second cooler (4), at the moment, hydrogen in the secondary membrane separation unit is preferentially permeated, the gas S5 on the permeation side of the secondary membrane is taken as circulating gas, and the residual side of the secondary membrane contains higher concentration CO 2 The residual gas S4 after the filtration is compressed by a second compressor (6) and cooled by a third cooler (7) enters a three-stage membrane separation unit (8); the hydrogen in the three-stage membrane separation unit (8) is preferentially permeated to obtain three-stage membrane permeation side gas S7, the final purification of the carbon dioxide product is completed, and the high-purity hydrogen product S6 on the permeation side is sent out after being pressurized by a third compressor (9) and cooled by a fourth cooler (10); finally, the second-stage membrane permeation-side gas S5 and the third-stage membrane permeation-side gas S7 are mixed to form a recycle gas S8, and the recycle gas is returned to the raw material side after being pressurized by the fourth compressor (11) and mixed with the raw material gas S1.
2. The multistage membrane separation carbon capture process for synthesis gas according to claim 1, wherein the membranes in each stage of membrane separation unit in the process can be flat plate, spiral wound or hollow fiber.
3. The multistage membrane separation carbon capture process for synthesis gas according to claim 1, wherein the membrane materials in each stage of membrane separation units in the process comprise two types of carbon dioxide preferential permeation membranes and hydrogen preferential permeation membranes.
4. The multistage membrane separation carbon capture process for synthesis gas according to claim 1, wherein the primary membrane separation unit adopts a carbon dioxide preferential permeation membrane, and the secondary and tertiary membrane separation units adopt hydrogen preferential permeation membranes.
5. A according to claim 1The multistage membrane separation carbon trapping process for the synthesis gas is characterized in that the pressure of the synthesis gas is 2.0-6.0MPa, and the synthesis gas comprises 50-70% of hydrogen and 30-50% of carbon dioxide; wherein hydrogen preferentially permeates H in the membrane 2 /CO 2 The selectivity is 5-20, and carbon dioxide preferentially permeates CO in the membrane 2 /H 2 The selectivity is 10-14.
6. The multistage membrane separation carbon capture process for synthesis gas according to claim 1, wherein the inlet pressure of the secondary membrane separation unit (5) is 1-3MPa, the inlet pressure of the tertiary membrane separation unit (8) is 2-5MPa, and the outlet pressure of each stage of membrane separation unit is close to atmospheric pressure.
7. The multistage membrane separation carbon capture process for synthesis gas according to claim 1, wherein the first, second, third and fourth compressors: each compressor system at least comprises one compressor, when the pressure is higher, a plurality of compressors and coolers among the compressors are adopted, and redundant compression heat in the compression process is taken out in time, so that the compression energy consumption is saved.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN116462158A (en) * | 2023-04-20 | 2023-07-21 | 大连理工大学 | Synthetic gas component membrane separation process based on waste heat recovery |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116462158A (en) * | 2023-04-20 | 2023-07-21 | 大连理工大学 | Synthetic gas component membrane separation process based on waste heat recovery |
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