CN114777420A - System and method for recovering argon and high-purity methane in hydrogen system - Google Patents

System and method for recovering argon and high-purity methane in hydrogen system Download PDF

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Publication number
CN114777420A
CN114777420A CN202210330253.XA CN202210330253A CN114777420A CN 114777420 A CN114777420 A CN 114777420A CN 202210330253 A CN202210330253 A CN 202210330253A CN 114777420 A CN114777420 A CN 114777420A
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methane
argon
pipeline
gas
purity
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张武
丁胜军
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Zhongke Ruiao Energy Technology Co ltd
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Zhongke Ruiao Energy Technology Co ltd
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  • Separation By Low-Temperature Treatments (AREA)

Abstract

The system and method for recovering argon and high purity methane in a hydrogen system of the present invention, wherein the system of the present invention comprises: a heat exchange device; a liquid nitrogen washing device; a demethanizer unit; a crude argon plant; an argon refining device; methane rectifying device. The method for recovering argon and high-purity methane in the hydrogen system comprises the following steps: cooling the raw material gas; removing high boiling point components in the raw material gas; removing methane in the raw material gas; removing high boiling point substances in the raw material gas; purifying the raw material gas into a high-purity liquid argon product; and purifying the methane-rich gas separated from the raw material gas into a high-purity methane product. The technology of the invention can lead the hydrogen recovery rate to reach more than 99 percent on the premise of not reducing the pressure of hydrogen and nitrogen, and can also produce high-purity liquid argon, LNG and high-purity methane products. The technology of the invention has the advantages of high recovery rate, less investment and energy consumption saving.

Description

System and method for recovering argon and high-purity methane in hydrogen system
Technical Field
The invention relates to liquefaction and recycling of gas, in particular to a system and a method for recycling argon and high-purity methane in a hydrogen system.
Background
In the process of synthesizing ammonia, inert gases are circularly accumulated in the reaction system and need to be continuously discharged. A large amount of hydrogen and nitrogen is discharged simultaneously with the discharge of the inert gas. The conventional technical scheme is to adopt membrane separation to recover hydrogen, so that the hydrogen becomes low pressure, energy consumption loss of repeated compression is caused, and the recovery rate is not high.
Disclosure of Invention
The invention aims to solve the technical problem of providing a system and a method for recovering argon and high-purity methane in a hydrogen system, which can ensure that the hydrogen recovery rate reaches more than 99 percent and can also produce high-purity liquid argon, LNG and high-purity methane products.
The system for recovering argon and high-purity methane in the hydrogen system comprises:
the heat exchange device is used for exchanging heat of two or more cold and hot streams;
the liquid nitrogen washing device is used for removing high-boiling-point components in the feed gas and is connected with the heat exchange device through a pipeline;
the demethanizer is used for removing methane in the high boiling point components pumped out by the liquid nitrogen washing device and is connected with the liquid nitrogen washing device through a pipeline;
the crude argon device is connected with the demethanizer, is used for removing high boiling point substances in the argon-rich gas discharged by the demethanizer, and is connected with the demethanizer through a pipeline;
the fine argon device is connected with the crude argon device through a pipeline and is used for purifying an argon-rich stream discharged by the crude argon device into a high-purity liquid argon product;
and the methane rectifying device is used for purifying a methane product and is connected with the methane removing device through a pipeline.
The system for recovering argon and high-purity methane in the hydrogen system comprises the following components: the device comprises a water washing device for removing ammonia in the raw gas and an adsorption device for removing moisture and other high-freezing-point components in the raw gas, wherein the water washing device is connected with the adsorption device through a pipeline, and the adsorption device is connected with the heat exchange device through a pipeline.
The system for recovering argon and high-purity methane in the hydrogen system further comprises a methane refining device, wherein the methane refining device is connected with the methane rectifying device through a first pipeline, and the first pipeline passes through the heat exchange device.
The system for recovering argon and high-purity methane in the hydrogen system comprises a liquid nitrogen washing device, a heat exchange device, a gas phase recovery device and a gas phase recovery device, wherein a gas phase outlet of the liquid nitrogen washing device is connected with a second pipeline; the tail gas outlet of the demethanizer is connected with a third pipeline, and the third pipeline passes through a heat exchange device so as to rewarm the gas phase in the third pipeline; and a bottom liquid phase outlet of the crude argon device is connected with an inlet of the demethanizer through a fourth pipeline, and the fourth pipeline is provided with a booster pump.
The system for recovering argon and high-purity methane in the hydrogen system comprises a water washing device, a water washing device and a water purifying device, wherein the water washing device comprises one or more towers, and the towers are one or more of pressure containers, plate towers and packed towers; the adsorption device comprises one or more pressure containers, wherein each pressure container is filled with a certain amount of adsorbent for adsorbing water and other high-boiling-point substances in the feed gas, and the adsorbent is one or more of a molecular sieve, activated carbon, activated alumina and ceramic balls; the heat exchange device comprises one or more heat exchangers, each heat exchanger at least comprises two flow channels for fluid heat exchange, and the heat exchanger is one or more of a shell-and-tube type, a plate-fin type and a wound tube type; the liquid nitrogen washing device is one or more of a pressure container, a plate tower and a packed tower; the demethanizer is one or more of a pressure vessel, a plate tower and a packed tower; the crude argon device is one or more of a pressure vessel, a plate tower and a packed tower; the argon refining device is one or more of a pressure vessel, a plate tower and a packed tower; the methane rectifying device is one or more of a pressure vessel, a plate tower and a packed tower; the methane refining device comprises one or more pressure vessels, wherein each pressure vessel is filled with a certain amount of adsorbent for adsorbing impurities in the raw material gas, and the adsorbent is one or more of a molecular sieve, activated carbon, activated alumina, a catalyst and ceramic balls.
The system for recovering argon and high-purity methane in the hydrogen system further comprises a refrigerating device, wherein the refrigerating device is connected with the heat exchange device and used for providing cold energy for the heat exchange device, and the refrigerating device is an expansion refrigerating device or a liquid throttling refrigerating device.
The system for recovering argon and high-purity methane in the hydrogen system comprises a first methane rectifying device, a second methane rectifying device, a heat exchange device and a third pipeline, wherein a gas phase outlet of the first methane rectifying device is connected with the third pipeline, and the third pipeline passes through the heat exchange device to rewarm a gas phase in the third pipeline.
The method for recovering argon and high-purity methane in a hydrogen system comprises the following steps:
cooling the raw material gas;
removing high boiling point components in the raw material gas;
removing methane in the raw material gas;
removing high boiling point substances in the raw material gas;
purifying the raw material gas into a high-purity liquid argon product;
and purifying the methane-rich gas separated from the raw material gas into a high-purity methane product.
The method for recovering argon and high-purity methane in the hydrogen system comprises the following steps before cooling the raw material gas: removing ammonia in the raw gas and removing water and other high freezing point components in the raw gas.
By adopting the technical scheme of the invention, the hydrogen recovery rate can reach more than 99% on the premise of not reducing the pressure of hydrogen and nitrogen, and high-purity liquid argon, LNG and high-purity methane products can be produced. The technology of the invention has the advantages of high recovery rate, less investment and energy consumption saving.
Drawings
FIG. 1 is a schematic diagram of a system for recovering argon and high purity methane in a hydrogen system according to the present invention;
FIG. 2 is a schematic diagram of the configuration of a system for recovering argon and high purity methane in a hydrogen system according to the present invention;
FIG. 3 is a schematic structural diagram of a first refrigeration device;
fig. 4 is a schematic structural diagram of a second refrigeration device.
Detailed Description
As shown in fig. 1, 2, 3 and 4, the system for recovering argon and high purity methane in a hydrogen system according to the present invention comprises:
the heat exchange device 201 is used for exchanging heat of two or more cold and hot streams;
the liquid nitrogen washing device 202 is used for removing high-boiling-point components in the feed gas and is connected with the heat exchange device through a pipeline;
the demethanizer 203 is used for removing methane in the high boiling point components extracted by the liquid nitrogen washing device 202 and is connected with the liquid nitrogen washing device through a pipeline;
the crude argon device 204 is connected with the demethanizer 203, is used for removing high boiling point substances in the argon-rich gas discharged from the demethanizer 203, and is connected with the demethanizer 203 through a pipeline;
the fine argon plant 205 is connected with the crude argon plant 204 through a pipeline and is used for purifying the argon-rich stream discharged from the crude argon plant 204 into a high-purity liquid argon product;
and the methane rectifying device 206 is used for purifying the methane product and is connected with the demethanizer 203 through a pipeline.
The system for recovering argon and high-purity methane in the hydrogen system comprises the following components: an ammonia water washing device 101 for removing ammonia in the raw gas and an adsorption device 102 for removing moisture and other high freezing point components in the raw gas, wherein the ammonia water washing device 101 is connected with the adsorption device 102 through a pipeline, and the adsorption device 102 is connected with a heat exchange device 201 through a pipeline.
The system for recovering argon and high-purity methane in the hydrogen system further comprises a methane refining device 207 which is connected with a methane rectifying device 206 through a first pipeline, and the first pipeline passes through a heat exchange device 201.
The system for recovering argon and high-purity methane in the hydrogen system comprises a liquid nitrogen washing device 202, a gas phase outlet of which is connected with a second pipeline, wherein the second pipeline passes through a heat exchange device 201 so as to rewarm the gas phase in the second pipeline; a tail gas outlet of the demethanizer 203 is connected with a third pipeline, and the third pipeline passes through the heat exchanger 201 to rewarm a gas phase in the third pipeline; the bottom liquid phase outlet of the crude argon plant 204 is connected to one inlet of the demethanizer 203 via a fourth line on which a booster pump is installed.
The system for recovering argon and high-purity methane in the hydrogen system comprises a water washing device 101, wherein the water washing device comprises one or more towers, and the towers are one or more of pressure containers, plate towers and packed towers; the adsorption device 102 comprises one or more pressure vessels, each pressure vessel is filled with a certain amount of adsorbent for adsorbing water and other high boiling point substances in the feed gas, and the adsorbent can be one or more of molecular sieve, activated carbon, activated alumina and ceramic balls; the heat exchange device 201 comprises one or more heat exchangers, each heat exchanger at least comprises two flow channels for fluid heat exchange, and the heat exchanger is one or more of a shell-and-tube type, a plate-fin type and a wound tube type; the liquid nitrogen washing device 202 is one or more of a pressure vessel, a plate tower and a packed tower; the demethanizer 203 is one or more of a pressure vessel, a plate column, a packed column; the crude argon unit 204 is one or more of a pressure vessel, a tray column, a packed column; the argon refining device 205 is one or more of a pressure vessel, a plate tower and a packed tower; the methane rectification device 206 is one or more of a pressure vessel, a plate column and a packed column; the methane refining device 207 comprises one or more pressure vessels, each pressure vessel is filled with a certain amount of adsorbent for adsorbing impurities in the raw material gas, and the adsorbent can be one or more of molecular sieve, activated carbon, activated alumina, catalyst and ceramic balls.
The system for recovering argon and high-purity methane in the hydrogen system further comprises a refrigerating device, wherein the refrigerating device is connected with the heat exchange device and used for providing cold energy for the heat exchange device, and the refrigerating device is an expansion refrigerating device or a liquid throttling refrigerating device.
The system for recovering argon and high-purity methane in the hydrogen system comprises a first methane rectifying device 206, wherein a gas phase outlet of the first methane rectifying device is connected with a fifth pipeline, and the fifth pipeline passes through a heat exchange device 201 so as to rewarm the gas phase in the fifth pipeline.
The method for recovering argon and high-purity methane in a hydrogen system comprises the following steps:
cooling the raw material gas;
removing high boiling point components in the raw material gas;
removing methane in the raw material gas;
removing high boiling point substances in the raw material gas;
purifying the raw material gas into a high-purity liquid argon product;
and purifying the methane-rich gas separated from the raw material gas into a high-purity methane product.
The method for recovering argon and high-purity methane in the hydrogen system comprises the following steps before cooling the raw material gas: removing ammonia in the raw gas, and removing water and other high freezing point components in the raw gas.
The first refrigeration device 301A and the second refrigeration device 301B may be one or more sets of refrigeration devices, respectively, and the refrigeration devices may be expansion refrigeration devices or liquid throttling refrigeration devices;
the technology of the invention can lead the hydrogen recovery rate to reach more than 99 percent on the premise of not reducing the pressure of hydrogen and nitrogen, and can produce high-purity liquid argon, LNG and high-purity methane products.
The main purpose of using the system shown in figure 2 is to recover the hydrogen, nitrogen, methane and argon from the blowing gas of the ammonia synthesis plant. The device comprises: the system comprises a water washing device 101, an adsorption device 102, a heat exchange device 201, a liquid nitrogen washing device 202, a demethanizer 203, a crude argon device 204, an argon refining device 205, a methane rectifying device 206, a methane refining device 207, a first refrigerating device 301A and a second refrigerating device 301B.
The specific process flow is as follows: the system raw material gas is the blowing gas of the ammonia synthesis device, and mainly comprises hydrogen (H)2) Nitrogen (N)2) Methane (CH)4) Argon (Ar), and the like. Firstly, blowing gas S01 from an ammonia synthesis device enters a water washing device (101), a water washing tower of the water washing device adopts regular packing, the blowing gas S01 enters from the bottom of the tower and then reversely contacts washing water S02 sprayed from the top of the tower, ammonia in the blowing gas is absorbed, and finally the ammonia content at the outlet of the washing tower is less than or equal to 10 ppm. The washed feed gas S03 enters an adsorption device (102), and the adsorption device adsorbs moisture and residual trace ammonia in the feed gas through a molecular sieve so as to meet the cryogenic requirement. The raw gas S05 passing through the adsorption device enters a heat exchange device 201, the heat exchange device adopts a plate-fin heat exchanger, and the raw gas in the plate-fin heat exchangerThe raw material gas is cooled by heat exchange with the cold flow strand of the return flow. The other stream S25 is low-pressure nitrogen, is pressurized by a compressor, enters a heat exchange device to be cooled to liquid nitrogen, and then enters a liquid nitrogen washing device 202 together with the stream S06, and in the liquid nitrogen washing device, a liquid nitrogen stream S27 is used for separating high-boiling-point components (such as CH) in a stream S064Ar, etc.) was flushed to liquid phase stream S09. The component of the gas-phase stream S07 of the liquid nitrogen washing device 202 is N2And H2(wherein CO + CO)2≤5ppm、CH4Less than or equal to 1ppm and Ar less than or equal to 20 ppm). And the stream S07 returns to the heat exchange device 201 for rewarming and then is sent out of the system to be used as a raw material of the ammonia synthesis device. The liquid phase stream S09 of the liquid nitrogen washing device 202 enters a demethanizer 203, methane is extracted from the bottom of a rectifying tower in the demethanizer in a liquid phase form, the stream S12 enters a methane rectifying device 206 to obtain a methane product S18 with the concentration of 99.99% or more, the stream S18 enters a heat exchange device 201 to be subcooled and then enters a methane refining device 207, and finally an electronic-grade methane product S20 is obtained. The top of the demethanizer in the demethanizer takes nitrogen as the tail gas S11 mainly containing a small amount of hydrogen, and the tail gas enters the heat exchange device 201 for rewarming and then is sent out of the system. And pumping a stream of argon-rich gas S10 from the demethanizer to enter a crude argon plant 204, pumping an argon-rich stream S13 containing methane from the crude argon plant, returning the argon-rich stream S14 containing no methane to the refined argon plant 205 after being pressurized by a booster pump, separating the argon-rich stream S16 from the refined argon plant 205 to obtain high-purity argon S16 and waste nitrogen gas S15, sending the high-purity argon S16 out of the system to enter a storage tank for storage, and sending the waste nitrogen gas S15 back to the heat exchange device 201 for reheating and then out of the system.
The refrigeration capacity of the system shown in fig. 3 and 4 is derived from two sets of refrigeration apparatuses, namely, a first refrigeration apparatus 301A and a second refrigeration apparatus 301B. The refrigerating device consists of a refrigerating compressor, a cooler, a separator, a buffer tank and the like. The refrigerant medium of the first refrigeration apparatus 301A is a mixed refrigerant composed of methane (CH)4) Ethylene (C)2H4) Propane (C)3H8) Isopentane (i-C)5H12) Nitrogen (N)2) And (4) forming. The mixed refrigerant enters a compressor for pressurization after passing through a buffer tank, the pressurized refrigerant enters the heat exchange device 201, is cooled to liquid, throttles by a throttle valve JT-1a and a throttle valve JT-1b and then returns to the heat exchange device 201And (4) providing cold energy, and finally rewarming the cold energy into a gas phase to return to the inlet buffer tank of the compressor and further return to the inlet of the compressor. The refrigerant medium of the second refrigeration device 301B is nitrogen, the low-pressure nitrogen enters the nitrogen compressor through the buffer tank to be pressurized, the pressurized nitrogen enters the heat exchange device 201, is throttled by the throttle valve JT-2 after being cooled to liquid and is sent to the demethanizer 203, the crude argon device 204, the fine argon device 205 and the methane rectification device 206 to provide condensation cold, and finally is reheated to a gaseous phase to be returned to the buffer tank at the inlet of the nitrogen compressor and further returned to the inlet of the nitrogen compressor.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that those skilled in the art can make various improvements and modifications without departing from the principle of the present invention, and these improvements and modifications should also be construed as the protection scope of the present invention.

Claims (9)

1. A system for recovering argon and high purity methane in a hydrogen system, comprising:
a heat exchange device (201) for exchanging heat between two or more cold and hot streams;
the liquid nitrogen washing device (202) is used for removing high boiling point components in the feed gas and is connected with the heat exchange device through a pipeline;
the demethanizer (203) is used for removing methane in the high boiling point components pumped out by the liquid nitrogen washing device (202) and is connected with the liquid nitrogen washing device through a pipeline;
the crude argon device (204) is connected with the demethanizer (203) and is used for removing high boiling point substances in the argon-rich gas discharged from the demethanizer (203) and is connected with the demethanizer (203) through a pipeline;
the fine argon device (205) is connected with the crude argon device (204) through a pipeline and is used for purifying an argon-rich stream discharged from the crude argon device (204) into a high-purity liquid argon product;
and the methane rectifying device (206) is used for purifying the methane product and is connected with the demethanizer (203) through a pipeline.
2. The system for recovering argon and high purity methane from a hydrogen system of claim 1, further comprising: the device comprises a water washing device (101) for removing ammonia in raw gas and an adsorption device (102) for removing moisture and other high-freezing-point components in the raw gas, wherein the water washing device (101) is connected with the adsorption device (102) through a pipeline, and the adsorption device (102) is connected with a heat exchange device (201) through a pipeline.
3. The system for recovering argon and high-purity methane in a hydrogen system according to claim 2, further comprising a methane refining device (207) connected to the methane rectifying device (206) through a first pipe, wherein the first pipe passes through the heat exchange device (201).
4. The system for recovering argon and high-purity methane in a hydrogen system as claimed in claim 3, wherein a gas phase outlet of the liquid nitrogen washing device (202) is connected with a second pipeline, and the second pipeline passes through the heat exchange device (201) so as to rewarming a gas phase in the second pipeline; a tail gas outlet of the demethanizer (203) is connected with a third pipeline, and the third pipeline passes through a heat exchange device (201) so as to rewarm a gas phase in the third pipeline; the bottom liquid phase outlet of the crude argon device (204) is connected with one inlet of the demethanizer (203) through a fourth pipeline, and the fourth pipeline is provided with a booster pump.
5. The system for recovering argon and high-purity methane in a hydrogen system according to claim 4, wherein the water washing device (101) comprises one or more towers, and the towers comprise one or more of a pressure vessel, a plate tower and a packed tower; the adsorption device (102) comprises one or more pressure vessels, wherein each pressure vessel is filled with a certain amount of adsorbent for adsorbing water and other high-boiling-point substances in the feed gas, and the adsorbent is one or more of molecular sieve, activated carbon, activated alumina and ceramic balls; the heat exchange device (201) comprises one or more heat exchangers, each heat exchanger at least comprises two flow channels for fluid heat exchange, and the heat exchanger is one or more of a shell-and-tube type, a plate-fin type and a wound tube type; the liquid nitrogen washing device (202) is one or more of a pressure vessel, a plate tower and a packed tower; the demethanizer (203) is one or more of a pressure vessel, a plate column, a packed column; the crude argon device (204) is one or more of a pressure vessel, a plate tower and a packed tower; the argon refining device (205) is one or more of a pressure vessel, a plate tower and a packed tower; the methane rectifying device (206) is one or more of a pressure vessel, a plate tower and a packed tower; the methane refining device (207) comprises one or more pressure vessels, each pressure vessel is filled with a certain amount of adsorbent for adsorbing impurities in the feed gas, and the adsorbent is one or more of a molecular sieve, activated carbon, activated alumina, a catalyst and a ceramic ball.
6. The system for recovering argon and high purity methane from a hydrogen system of claim 5, further comprising a refrigeration unit coupled to the heat exchange unit for providing refrigeration to the heat exchange unit, the refrigeration unit being an expansion refrigeration unit or a liquid throttling refrigeration unit.
7. The system for recovering argon and high-purity methane in a hydrogen system according to claim 6, wherein the gas phase outlet of the first methane rectifying device (206) is connected to a fifth pipeline, and the fifth pipeline passes through the heat exchange device (201) to rewet the gas phase in the fifth pipeline.
8. A method for recovering argon and high-purity methane in a hydrogen system is characterized by comprising the following steps:
cooling the raw material gas;
removing high boiling point components in the raw material gas;
removing methane in the raw material gas;
removing high boiling point substances in the raw material gas;
purifying the raw material gas into a high-purity liquid argon product;
and purifying the methane-rich gas separated from the raw material gas into a high-purity methane product.
9. The method for recovering argon and high purity methane from a hydrogen system of claim 8 further comprising, prior to cooling the feed gas: removing ammonia in the raw gas and removing water and other high freezing point components in the raw gas.
CN202210330253.XA 2022-03-31 2022-03-31 System and method for recovering argon and high-purity methane in hydrogen system Pending CN114777420A (en)

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