CN113148967A - Method and device for recovering helium from natural gas in pipeline - Google Patents
Method and device for recovering helium from natural gas in pipeline Download PDFInfo
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- CN113148967A CN113148967A CN202110513014.3A CN202110513014A CN113148967A CN 113148967 A CN113148967 A CN 113148967A CN 202110513014 A CN202110513014 A CN 202110513014A CN 113148967 A CN113148967 A CN 113148967A
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- C01B2210/00—Purification or separation of specific gases
- C01B2210/0001—Separation or purification processing
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- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
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- C01B2210/0021—Temperature swing adsorption
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Abstract
The invention discloses a method and a device for recovering helium from pipeline natural gas, which are characterized in that the pipeline natural gas is concentrated by a concentration process, and the pipeline natural gas with the helium content of 200-500 ppm can be concentrated to the helium content of more than 20%; and then purifying the concentrated raw material crude helium gas by a purification recovery process. The invention aims at the natural gas of the pipeline with the helium content of more than or equal to 300ppm in China, and high-purity helium is directly obtained from the natural gas of the pipeline through a multistage membrane separation component, a pressure swing adsorption purification device, a hydrogen-helium separation device, a temperature swing adsorption purification device and the like. The invention is different from a low-temperature fractionation process, adopts a composite process, has strong adaptability to the helium content in natural gas, and can be directly used for processing pipeline natural gas with the content of more than 300ppm and obtaining high-purity helium. The invention relates to the technical field of natural gas recovery helium, and can be applied to natural gas pipelines, natural gas purification stations, natural gas pressurization stations, natural gas regulation transmission stations, well mouth natural gas and the like for recovering and preparing high-purity helium.
Description
Technical Field
The invention belongs to the technical field of helium recovery, and particularly relates to a method and a device for recovering helium from natural gas in a pipeline.
Background
Helium is a colorless and tasteless inert gas, is widely applied to the fields of optical fibers, semiconductors, medical treatment, national defense and the like, and is a non-renewable scarce strategic resource. Helium has wide application and large consumption, but the acquisition source is limited, the content of helium in the air is about 5ppm, and the helium has no extraction value and is mainly recovered from associated helium in natural gas exploitation at present.
China is a typical poor helium country, the content of associated helium of natural gas is generally 200-600 ppm, and the problem that the technology is complex, the cost is high, the economy is not outstanding and the like is faced when helium is directly recovered and extracted from the natural gas, so that the dependence of helium used in China on import exceeds 95%, the helium is imported by more than 3000 million cubic meters every year after 2018, and the current situation of poor helium in China severely restricts the development of national defense and national economy.
Compared with the helium content of natural gas in America, Katalr, Russia and other countries which is generally over 1000ppm, the helium content of natural gas in China is generally lower. However, China is a typical country with large energy consumption, and has typical elm-inner Mongolia, Qinghai, Xinjiang, Sichuan Yu and other atmospheric regions, and the natural gas reserves and the exploitation amount are huge.
The technology and the device for recovering helium from BOG gas in the LNG liquefaction process developed in China have 2-3 sets of start-up and produce qualified high-purity helium, and a low-temperature fractionation process is generally adopted. However, the helium content in the BOG gas is concentrated by more than ten times, and the related technology is simpler. More importantly, the LNG liquefaction plants in China account for a small amount of large natural gas production, and even if helium produced by helium recovery projects of all domestic liquefaction plants only accounts for 20-30% of helium consumed by China every year, gaps are still large. Therefore, the research on helium recovery from natural gas in pipelines is significant, and the method and the device are the only method and way for solving the self-sufficiency of helium supply in China.
Disclosure of Invention
The invention aims to provide a method and a device for recovering helium from pipeline natural gas, which can be directly used for processing the pipeline natural gas with more than 300ppm and obtaining high-purity helium from the pipeline natural gas.
The invention provides a method for recovering helium from natural gas of a pipeline, which is characterized in that the natural gas of the pipeline is concentrated by a concentration process, and the concentration is from 300-500 ppm to more than 20% (volume); and then purifying the concentrated natural gas of the pipeline by a purification and recovery process.
The invention also provides a device for recovering helium from the pipeline natural gas, which comprises a helium concentration system and a helium purification and recovery system; the helium concentration system comprises a primary membrane separation assembly connected with a natural gas outlet pipe of the pipeline and a multi-stage membrane separation assembly connected with the primary membrane separation assembly; a packed tower for removing heavy hydrocarbons is arranged between the pipeline natural gas outlet pipe and the primary membrane separation component; the helium purification and recovery system comprises a pressure swing adsorption purification device, a hydrogen-helium separation device, a dehydrogenation device and a Temperature Swing Adsorption (TSA) purification device which are sequentially connected through a gas pipeline; the pressure swing adsorption purification device is connected with the multi-stage membrane separation assembly.
The invention relates to a method for regulating pressure of raw material natural gas from a natural gas pipeline to enter a primary membrane separation component after heavy hydrocarbon removal treatment. The non-permeate tail gas of the primary membrane separation assembly has a small pressure drop relative to the raw natural gas and can be directly returned to the pipeline and conveyed to downstream gas utilization. The first-stage membrane separation component is connected with the compressor, and enters the multistage membrane separation component after being pressurized by the compressor. And the permeation gas of the multistage membrane separation assembly is pressurized by a booster pump and then sent into a pressure swing adsorption purification device, the crude helium gas which is discharged from the pressure swing adsorption purification device enters a hydrogen helium separation device, an outlet of the hydrogen helium separation device is connected with a dehydrogenation device and a Temperature Swing Adsorption (TSA) purification device, and the high-purity helium gas is obtained by the Temperature Swing Adsorption (TSA) purification device. The tail gas or the regenerated gas generated by the multistage membrane separation component, the pressure swing adsorption purification device and the hydrogen-helium separation device returns to the storage tank, and returns to the gas transmission pipeline after being pressurized and regulated by the compressor, so that the loss of the gas transmission quantity of the pipeline is reduced.
Aiming at the pipeline natural gas with the helium content of more than or equal to 300ppm in China, the pipeline natural gas is concentrated to the helium content of more than 20% (volume ratio) through the multistage membrane separation assembly, so that the source of helium is greatly expanded, and the method is not limited to the recovery of helium from the non-condensable gas or BOG gas of a cold box with high helium content formed in the LNG liquefaction process at present. The invention directly obtains high-purity helium from the natural gas in the pipeline by a pressure swing adsorption purification device, a hydrogen-helium separation device, a temperature swing adsorption purification device and the like. The invention is different from a low-temperature fractionation process, adopts a composite process, has strong adaptability to helium content fluctuation in natural gas, is a universal helium concentration and purification process, and can be directly used for processing pipeline natural gas with the content of more than 300ppm and obtaining high-purity helium. The invention relates to the technical field of natural gas recovery helium, and can be applied to natural gas pipelines, natural gas purification stations, natural gas pressurization stations, natural gas regulation transmission stations, well mouth natural gas and the like for recovering and preparing high-purity helium.
Drawings
FIG. 1 is a schematic diagram of a helium concentration system.
FIG. 2 is a schematic diagram of the overall configuration of an apparatus for recovering helium from pipeline natural gas.
In the figure: 601 one-stage membrane separation component, 602 compressor, 603, 605 multi-stage membrane separation components, 604 compressor, 606 compressor, 607 pressure swing adsorption purification device, 608 hydrogen helium separation device, 609 dehydrogenation device, 610 temperature swing adsorption purification device, T611 storage tank, 612 packed tower.
Detailed Description
The following is a further description of the present invention as an illustration of the technical contents of the present invention, but the essential contents of the present invention are not limited to the following, and one of ordinary skill in the art can and should understand that any simple changes or substitutions based on the essential spirit of the present invention should fall within the protection scope of the present invention as claimed.
The invention adopts a method for recovering helium from pipeline natural gas, which is to concentrate the pipeline natural gas by a concentration process, wherein the pipeline natural gas with the helium content of 300-500 ppm can be concentrated to the helium content of more than 20% (volume); and then purifying the concentrated natural gas of the pipeline by a purification and recovery process.
The invention adopts a device for realizing the method for recovering helium, which comprises a helium concentration system and a helium purification and recovery system; the helium concentration system comprises a first-stage membrane separation component 601 connected with a natural gas outlet pipe of the pipeline and a multi-stage membrane separation component connected with the first-stage membrane separation component 601; wherein, the multistage membrane separation component adopts a two-stage membrane separation component 603 and a three-stage membrane separation component 605 which are connected in series. The gas inlet end of the secondary membrane separation module 603 is connected with the permeate gas outlet end of the primary membrane separation module 601, and the permeate gas outlet end of the secondary membrane separation module 603 is connected with the gas inlet end of the tertiary membrane separation module 605. Meanwhile, a packed tower for removing heavy hydrocarbon is arranged between the pipeline natural gas outlet pipe and the primary membrane separation component 601; the device also comprises a helium purification and recovery system, which specifically comprises a pressure swing adsorption purification device 607, a hydrogen-helium separation device 608, a dehydrogenation device 609 and a temperature swing adsorption TSA purification device 610 which are sequentially connected through a gas pipeline; wherein, the inlet end of the pressure swing adsorption purification device 607 is connected to the permeate gas outlet end of the three-stage membrane separation component 605.
Specifically, as shown in fig. 2, the method firstly separates out and removes C from the pipeline natural gas by treating the pipeline natural gas through a packed tower6After the heavy hydrocarbon is treated, the pressure is regulated and the heavy hydrocarbon is sent to a first-stage membrane separation component 601 for first-stage separation. Packed column removal of C6The heavy hydrocarbon is treated through common heavy hydrocarbon eliminating adsorption process, and the stuffing may be molecular sieve, silica gel, active alumina, etc. The pressure difference between the non-permeate gas and the inlet raw material gas of the primary membrane separation module 601 is not more than 0.5Mpa, and the inlet pressure of the primary membrane separation module 601 is more than 5 times of the pressure of the permeate gas side. The permeate from the first-stage membrane separation module 601 is pressurized by a compressor 604 and then sequentially sent to a second-stage membrane separation module 603 and a third-stage membrane separation module 605 for multi-stage membrane separation, so that the helium content of the crude helium feed gas permeated after the final membrane separation reaches more than 20%. The tail gas of the secondary membrane separation component 603 and the tail gas of the tertiary membrane separation component 605 return to T611 and are pressurized by the compression pump 602 and return to a gas pipeline. Wherein, the second-stage membrane separation component 603 and the third-stage membrane separation component 605 are organic cascade technology, and a first-stage compression pump can be added between the second-stage membrane separation component 603 and the third-stage membrane separation component 605 or not. The first-stage membrane separation assembly 601, the compressor 604, the second-stage membrane separation assembly 603, the third-stage membrane separation assembly 605 and the compressor 606 are organically coupled, and the pressure ratio of the inlet side and the permeate side of each stage of membrane separation assembly is adjusted by means of a back pressure valve or other pressure adjusting devices arranged at the tail gas end of each stage of membrane separation assembly through pressure adjustment. The inlet pressure and the side pressure ratio of the permeate gas of the primary membrane separation assembly 601, the secondary membrane separation assembly 603 and the tertiary membrane separation assembly 605 are controlled to be more than or equal to 5 (the higher the pressure ratio is, the more easily the permeate gas is obtained, the pressure ratio can be generally selected to be between 5 and 30), so that the raw crude helium with the helium content of more than or equal to 20 percent can be concentrated from more than or equal to 300ppm in the pipeline natural gas. The concentration system is used for obtaining highPure helium provides a base feed gas with a higher helium content, expanding the source of helium.
The membrane separation component adopted by the invention adopts a common high-molecular hollow fiber membrane, and the membrane material is usually a high-molecular polymer material such as polysulfone, polyamide and the like. The pretreated raw gas is sent into a first-stage membrane separation component under high pressure, small molecules such as helium and hydrogen can pass through a membrane to form permeation gas at an outlet at a low pressure side, large molecules such as methane and nitrogen can be retained to form non-permeation gas at an outlet at a high pressure side, and the non-permeation gas can return to a pipeline due to small pressure drop. Of course, the membrane separation module of the present invention is not limited to the three-stage series connection method used in the present embodiment, and more stages of membrane separation modules may be used to obtain a higher crude helium content, but the three-stage series connection method is preferable in view of economy. In addition, if the temperature of the primary membrane separation module 601 can be maintained at 50 to 60 ℃, the increase of the crude helium content of the raw material finally obtained can be facilitated, and the temperature of the secondary membrane separation module 603 and/or the tertiary membrane separation module 605 maintained at 50 to 60 ℃ is not apparently increased.
The raw material crude helium obtained after the multi-stage membrane separation is pressurized by a booster pump 606 and then sent to a Pressure Swing Adsorption (PSA) purification device 607 for adsorption and purification, and crude helium (including hydrogen) with the purity of more than or equal to 98 percent can be obtained. The crude helium obtained by adsorption purification is sent to a hydrogen-helium separation device 608 for hydrogen-helium separation, and then sent to a dehydrogenation device 609 for dehydrogenation treatment. The crude helium enters a hydrogen-helium separation device 608 to separate out most of hydrogen, and returns to a storage tank T611, and a small amount of hydrogen is further converted into water in a dehydrogenation device 609, so that the purpose of deep dehydrogenation is achieved. And finally, sending the helium to a temperature swing adsorption TSA purification device 610 to obtain the recovered high-purity helium. The tail gas or the regenerated gas generated by the secondary membrane separation component 603, the tertiary membrane separation component 605, the pressure swing adsorption purification device 607 and the hydrogen helium separation device 608 returns to the storage tank T611, and returns to the gas transmission pipeline after being pressurized and regulated by the compressor 602, thereby reducing the loss of the pipeline gas transmission quantity.
The pressure swing adsorption purification device 607 adopts a common double-tower form, ensures the desorption state of one tower when the other tower is in the adsorption state, porous adsorption materials such as active carbon are arranged in the tower, other impurities are adsorbed on the porous adsorption materials by pressurization, the impurities can be desorbed from the adsorbent again by decompression to complete the regeneration of the adsorbent, helium hydrogen micromolecules are purified, a series of impurities such as nitrogen, oxygen, argon and the like can be effectively removed by pressure swing adsorption purification, and the pressure swing adsorption purification device works under the normal temperature environment; the hydrogen-helium separation device 608 employs a commonly used palladium membrane separator for hydrogen separation; the outlet of the hydrogen-helium separation device 608 is connected with a dehydrogenation device 609; the dehydrogenation device 609 adopts a common catalytic dehydrogenation mode, common dehydrogenation catalysts such as Pt-based catalysts, ceramic-loaded Pt catalysts and the like are filled in the dehydrogenation device 609, a small amount of hydrogen can be converted into water by the catalysts in the presence of oxygen or air, and the removal depth of the hydrogen is less than or equal to 2 ppm. The dehydrogenation unit 609 can treat the crude helium containing a small amount of hydrogen from the hydrogen-helium separation unit 608; the dehydrogenation device 609 can adopt external or internal heating, and the internal working temperature is generally 200-300 ℃; the Temperature Swing Adsorption (TSA) purification device 610 adopts a common double-tower design, and ensures that one tower is in a desorption state while the other tower is in an adsorption state, porous adsorption materials such as activated carbon and molecular sieve are filled in the tower, other impurities except helium are adsorbed on the porous adsorption materials through temperature reduction, the impurities can be desorbed from the adsorbent again through temperature rise to complete the regeneration of the adsorbent, the helium is purified, and other gas impurities are discharged along with the regeneration process. A plurality of adsorption cylinders soaked by cold sources are arranged inside each adsorption tower of the Temperature Swing Adsorption (TSA) purification device 610, and a plurality of adsorbent fillers such as molecular sieves, activated carbon and the like are filled in the adsorption cylinders; the Temperature Swing Adsorption (TSA) purification device 610 can adopt a cold source (cold liquid) such as liquid nitrogen or a refrigerating unit, and the temperature of the cold source is less than or equal to minus 20 ℃; and finally, the purity of helium at the outlet of the Temperature Swing Adsorption (TSA) purification device is more than or equal to 99.999 percent.
The basic working principle of the invention is as follows:
the raw material natural gas from a natural gas pipeline enters a first-stage membrane separation assembly after passing through a packed tower and being subjected to pressure regulation. The non-permeate tail gas of the primary membrane separation assembly has a small pressure drop relative to the raw natural gas and can be directly returned to the pipeline and conveyed to downstream gas utilization. The first-stage membrane separation component is connected with the compressor, and the permeate gas enters the second-stage membrane separation component and the third-stage membrane separation component in sequence after being pressurized by the compressor. And the permeation gas of the three-stage membrane separation component is pressurized by a booster pump and then sent into a pressure swing adsorption purification device, the crude helium gas which is discharged from the pressure swing adsorption purification device enters a hydrogen helium separation device, an outlet of the hydrogen helium separation device is connected with a dehydrogenation device and a Temperature Swing Adsorption (TSA) purification device, and the high-purity helium gas is obtained by the Temperature Swing Adsorption (TSA) purification device. The tail gas or regenerated gas generated by the secondary membrane separation component, the tertiary membrane separation component, the pressure swing adsorption purification device and the hydrogen-helium separation device returns to the storage tank and returns to the gas transmission pipeline after being pressurized and regulated by the compressor, so that the loss of the gas transmission and supply amount of the pipeline is reduced. The invention aims at the natural gas of the pipeline with helium content more than or equal to 300ppm in China, and high-purity helium is directly obtained from the natural gas of the pipeline through a membrane separation component, a pressure swing adsorption purification device, a hydrogen-helium separation device, a temperature swing adsorption purification device and the like.
It should be noted that the technical contents described above are only explained and illustrated to enable those skilled in the art to know the technical spirit of the present invention, and therefore, the technical contents are not to limit the scope of the present invention. The scope of the invention is defined by the appended claims. It should be understood by those skilled in the art that any modification, equivalent replacement, and improvement made based on the spirit of the present invention should be considered to be within the spirit and scope of the present invention.
Claims (11)
1. A method for recovering helium from pipeline natural gas is characterized in that the pipeline natural gas is concentrated to more than 20% through a concentration process; and purifying the concentrated natural gas of the pipeline by a purification and recovery process.
2. The method of claim 1, wherein the concentration process comprises the steps of: the method comprises the following steps of (1) carrying out pressure regulation on the pipeline natural gas, sending the pipeline natural gas into a first-stage membrane separation component (601) for first-stage separation, and then sending the pipeline natural gas into a multi-stage membrane separation component for multi-stage membrane separation after pressurization, wherein the multi-stage membrane separation component at least comprises a second-stage membrane separation component (603) and a third-stage membrane separation component (605) which are connected in series; a compressor is arranged or not arranged between the secondary membrane separation component (603) and the tertiary membrane separation component (605); the pressure ratio of the gas inlet pressure to the permeate gas outlet side of the first-stage membrane separation assembly (601), the second-stage membrane separation assembly (603) and the third-stage membrane separation assembly (605) is not less than 5; the concentration process also comprises the step of carrying out primary separation after carrying out heavy hydrocarbon removal treatment on the pipeline natural gas.
3. The method of claim 1, wherein the purification recovery process comprises the steps of: pressurizing the concentrated natural gas of the pipeline, then sending the pressurized natural gas into a pressure swing adsorption purification device (607) for adsorption purification, sending the crude helium obtained through adsorption purification into a hydrogen helium separation device (608) for hydrogen helium separation, then sending the crude helium into a dehydrogenation device (609) for dehydrogenation treatment, and finally sending the crude helium into a temperature swing adsorption purification device (610) to obtain high-purity helium.
4. The method according to claim 2, wherein the gas temperature of the primary membrane separation module (601) is maintained between 50 ℃ and 60 ℃; and tail gas or regenerated gas generated by the multistage membrane separation assembly returns to the gas transmission pipeline.
5. The method of claim 3, wherein the tail gas or the regeneration gas generated by the pressure swing adsorption purification device (607) and the hydrogen-helium separation device (608) is returned to the storage tank (T611), pressurized by the compressor (602), and pressure-regulated and then returned to the gas transmission pipeline.
6. The device for recovering helium from natural gas in the pipeline is characterized by comprising a helium concentration system and a helium purification and recovery system;
the helium concentration system comprises a first-stage membrane separation component (601) connected with a natural gas outlet pipe of the pipeline and a multi-stage membrane separation component connected with the first-stage membrane separation component (601); a packed tower for removing heavy hydrocarbon is arranged between the pipeline natural gas outlet pipe and the primary membrane separation component (601);
the helium purification and recovery system comprises a pressure swing adsorption purification device (607), a hydrogen-helium separation device (608), a dehydrogenation device (609) and a temperature swing adsorption purification device (610) which are sequentially connected through a gas pipeline; the pressure swing adsorption purification device (607) is connected with a multi-stage membrane separation component.
7. The apparatus according to claim 6, wherein the multistage membrane separation module comprises at least a secondary membrane separation module (603) and a tertiary membrane separation module (605) in series; a compressor is arranged or not arranged between the secondary membrane separation assembly (603) and the tertiary membrane separation assembly (605).
8. The apparatus of claim 6, wherein a compressor is disposed between the one-stage membrane separation module (601) and the multi-stage membrane separation module, and a compressor is disposed between the multi-stage membrane separation module and the pressure swing adsorption purification apparatus (607).
9. The apparatus of claim 6, wherein said primary membrane separation module (601) is provided with a non-permeate outlet line connected to a return line.
10. The apparatus of claim 6, wherein the multi-stage membrane separation module, the pressure swing adsorption purification unit (607), and the hydrogen helium separation unit (608) are each provided with a tail gas or regeneration gas outlet line connected to a return line.
11. The apparatus according to claim 10, characterized in that the off-gas or regeneration gas outlet line is connected to a storage tank (T611), the other end of the storage tank (T611) being connected by a line to a return conduit.
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| CN202110513014.3A CN113148967A (en) | 2021-05-11 | 2021-05-11 | Method and device for recovering helium from natural gas in pipeline |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN115140718A (en) * | 2022-07-20 | 2022-10-04 | 大连理工大学 | Helium separation and recovery system and method based on membrane separation, pressure swing adsorption and electrochemical hydrogen pump coupling |
| CN115872371A (en) * | 2021-09-26 | 2023-03-31 | 中国石油化工股份有限公司 | Method and system for purifying ultrapure helium |
| CN116281896A (en) * | 2022-12-01 | 2023-06-23 | 煤炭科学技术研究院有限公司 | Helium extraction method for helium-containing coal bed gas concentration at low temperature |
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| CN209554793U (en) * | 2019-01-09 | 2019-10-29 | 北京石油化工工程有限公司 | Helium recovery unit in a kind of hydrogen-containing gas |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN115872371A (en) * | 2021-09-26 | 2023-03-31 | 中国石油化工股份有限公司 | Method and system for purifying ultrapure helium |
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| CN115140718A (en) * | 2022-07-20 | 2022-10-04 | 大连理工大学 | Helium separation and recovery system and method based on membrane separation, pressure swing adsorption and electrochemical hydrogen pump coupling |
| CN116281896A (en) * | 2022-12-01 | 2023-06-23 | 煤炭科学技术研究院有限公司 | Helium extraction method for helium-containing coal bed gas concentration at low temperature |
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