CN108441261B - Nitrogen-containing methane-rich gas separation system and separation method based on argon circulation refrigeration - Google Patents

Nitrogen-containing methane-rich gas separation system and separation method based on argon circulation refrigeration Download PDF

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CN108441261B
CN108441261B CN201810437481.0A CN201810437481A CN108441261B CN 108441261 B CN108441261 B CN 108441261B CN 201810437481 A CN201810437481 A CN 201810437481A CN 108441261 B CN108441261 B CN 108441261B
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argon
methane
cold energy
gas
nitrogen
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CN108441261A (en
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舒伟
张敏卿
毛文军
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream
    • F25J3/0228—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream
    • F25J3/0233—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream separation of CnHm with 1 carbon atom or more
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G70/00—Working-up undefined normally gaseous mixtures obtained by processes covered by groups C10G9/00, C10G11/00, C10G15/00, C10G47/00, C10G51/00
    • C10G70/04—Working-up undefined normally gaseous mixtures obtained by processes covered by groups C10G9/00, C10G11/00, C10G15/00, C10G47/00, C10G51/00 by physical processes
    • C10G70/043—Working-up undefined normally gaseous mixtures obtained by processes covered by groups C10G9/00, C10G11/00, C10G15/00, C10G47/00, C10G51/00 by physical processes by fractional condensation
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D3/00—Distillation or related exchange processes in which liquids are contacted with gaseous media, e.g. stripping
    • B01D3/14—Fractional distillation or use of a fractionation or rectification column
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D5/00—Condensation of vapours; Recovering volatile solvents by condensation
    • B01D5/0003—Condensation of vapours; Recovering volatile solvents by condensation by using heat-exchange surfaces for indirect contact between gases or vapours and the cooling medium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D5/00—Condensation of vapours; Recovering volatile solvents by condensation
    • B01D5/0057—Condensation of vapours; Recovering volatile solvents by condensation in combination with other processes
    • B01D5/006—Condensation of vapours; Recovering volatile solvents by condensation in combination with other processes with evaporation or distillation
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G70/00—Working-up undefined normally gaseous mixtures obtained by processes covered by groups C10G9/00, C10G11/00, C10G15/00, C10G47/00, C10G51/00
    • C10G70/04—Working-up undefined normally gaseous mixtures obtained by processes covered by groups C10G9/00, C10G11/00, C10G15/00, C10G47/00, C10G51/00 by physical processes
    • C10G70/041—Working-up undefined normally gaseous mixtures obtained by processes covered by groups C10G9/00, C10G11/00, C10G15/00, C10G47/00, C10G51/00 by physical processes by distillation
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    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream
    • F25J3/0204—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the feed stream
    • F25J3/0209—Natural gas or substitute natural gas
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    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream
    • F25J3/0204—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the feed stream
    • F25J3/0219—Refinery gas, cracking gas, coke oven gas, gaseous mixtures containing aliphatic unsaturated CnHm or gaseous mixtures of undefined nature
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    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream
    • F25J3/0228—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream
    • F25J3/0257—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream separation of nitrogen
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00—Processes or apparatus using separation by rectification
    • F25J2200/02—Processes or apparatus using separation by rectification in a single pressure main column system
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00—Processes or apparatus using separation by rectification
    • F25J2200/50—Processes or apparatus using separation by rectification using multiple (re-)boiler-condensers at different heights of the column
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00—Processes or apparatus using separation by rectification
    • F25J2200/74—Refluxing the column with at least a part of the partially condensed overhead gas
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2210/00—Processes characterised by the type or other details of the feed stream
    • F25J2210/12—Refinery or petrochemical off-gas
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/12—External refrigeration with liquid vaporising loop
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/14—External refrigeration with work-producing gas expansion loop
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/58—Quasi-closed internal or closed external argon refrigeration cycle
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/10—Greenhouse gas [GHG] capture, material saving, heat recovery or other energy efficient measures, e.g. motor control, characterised by manufacturing processes, e.g. for rolling metal or metal working

Abstract

The invention relates to a separation system and a separation method based on argon circulation refrigeration of nitrogen-containing methane-rich gas, wherein the separation system comprises a methane separation system and an argon circulation refrigeration system, after the nitrogen-containing methane-rich gas enters the methane separation system, the separated liquid methane enters a liquid methane-argon heat exchanger in the argon circulation refrigeration system, cold energy of the liquid methane is transferred to circulation argon, and the circulation argon is used for providing cold energy for a tower top condenser in the methane separation system, so that the cold energy recovery process is realized. The separation method is that the cold energy of the liquid methane is transferred to the circulating argon, and the circulating argon in turn provides cold energy for separating the liquid methane from the nitrogen-containing methane-rich gas. The separation system of the invention takes circulating argon as working medium, recovers the cold energy of methane and nitrogen of the separation system through a heat pump and a cold energy heat exchanger, supplements the cold energy through partial argon expansion refrigeration, and then utilizes the argon Joule-Thomson effect to improve the cold energy grade and then transmits the cold energy grade to the nitrogen-containing methane-rich gas separation system, thereby realizing high-efficiency separation with lower refrigeration energy consumption.

Description

Nitrogen-containing methane-rich gas separation system and separation method based on argon circulation refrigeration
Technical Field
The invention belongs to the technical field of product recovery in nitrogen-containing and methane-rich industrial tail gas, and relates to a nitrogen-containing and methane-rich gas separation system based on argon circulation refrigeration and a separation method.
Background
The refinery dry gas mainly comes from the processes of heavy oil catalytic cracking, delayed coking, hydrocracking, catalytic reforming and the like in petroleum processing, and the main components of the refinery dry gas comprise hydrogen, nitrogen, methane, ethylene, ethane, propane and the like, wherein the values of the hydrogen, the ethylene, the ethane and the like are higher. Ethylene is a high-value product, hydrogen can be recycled for hydrocracking or sold as a product, and light hydrocarbons such as ethane, propane and the like can be recycled for an ethylene device as high-quality cracking raw materials. However, most refineries use dry gas as fuel gas except for the fact that few refineries with associated ethylene units use ethylene feed recovery processes. The main components of the purge gas for methanol synthesis comprise hydrogen, nitrogen, methane and the like, part of manufacturers convert the purge gas into LNG through an expensive methanation process, and the other parts of the purge gas fuel gas are still used. The dry gas and the purge gas are directly used as fuel, and the low-value use of high-price products exists, so that the resource waste is caused.
The separation and recovery of the high-valence products in the dry gas usually adopts one or a combination of adsorption, absorption, membrane and cryogenic separation. The adsorption method utilizes the selective adsorbent to realize the cycle of adsorption and desorption through pressure and temperature changes, and a certain component which is relatively pure is obtained. For example, patent CN201410220850.2, hydrogen and ethylene in dry gas are recovered by light cold adsorption. The yield and purity of the adsorption method are relatively low, and the investment and occupation of the device are large. The absorption rule adopts solvent absorption to carry out selective absorption, and then the high-purity product can be obtained through rectification separation. For example, patent CN201410220882.2 and CN201410359774.3 respectively adopt butane, pentane, aromatic hydrocarbon or acetonitrile and other solvents to make selective absorption, and recover hydrogen and ethylene in the dry gas. Because of the solvent characteristics, the absorption has the defects of low selectivity and low separation yield, and cold energy is still required to be provided for precise separation, so that the application of the method is limited. The membrane separation realizes the separation of the components by utilizing the permeability difference of different components in the dry gas in the special membrane, and is suitable for recycling hydrogen in the dry gas with low pressure and low hydrogen content, but the purity is not high. The cryogenic separation generally uses methane and ethylene propylene propane as refrigerants, and the required low-temperature cold energy is obtained through the compression, condensation, throttling and expansion processes. The cryogenic separation can ensure the purity and high yield of the product, can obtain polymerization-grade ethylene for dry gas separation, and can improve the recovery rate of methane when used for purge gas separation, but the conventional cryogenic method has high operating pressure and high energy consumption, and the expensive refrigeration cost restricts the wide application of the method, so that the method is only suitable for large-scale treatment.
Natural gas is a high-quality environment-friendly fuel, and is transported in a Liquid (LNG) mode generally, the liquid cryogenic (normal pressure-162 ℃) is required to be changed into a gaseous state before the natural gas is combusted, and the gasification cold energy of the LNG is used for dry gas separation, so that the dry gas separation cost can be greatly reduced. The normal pressure gasification temperature of methane is only minus 162 ℃, and the methane is difficult to separate with nitrogen in dry gas or oilfield associated gas at the temperature in a high-definition way, so that the recovery rate of methane is low, and meanwhile, methane is entrained in light component hydrogen and nitrogen, so that the hydrogen recovery is influenced.
Disclosure of Invention
The invention aims to solve the technical problem of providing a nitrogen-containing methane-rich gas separation system and a separation method based on argon circulation refrigeration aiming at the defects of the prior art. According to the argon circulation refrigerating system, argon is used as a circulation working medium, methane and nitrogen cold energy of a separating system is recovered through a heat pump and a cold energy heat exchanger, the cold energy is supplemented through partial argon expansion refrigeration, then the cold energy grade is improved through an argon Joule-Thomson effect and then is transmitted to a nitrogen-containing methane-rich gas separating system, high-efficiency separation is realized through lower refrigeration energy consumption, high-price utilization of industrial resources such as dry gas, purge gas, land and ocean oilfield associated gas, coal bed gas, shale gas and the like is realized, and the methane recovery rate in the above gases can reach more than 99%.
In order to solve the problems, the invention adopts the following technical scheme:
the nitrogen-containing methane-rich gas separation system based on argon circulation refrigeration comprises a methane separation system and an argon circulation refrigeration system, wherein after nitrogen-containing methane-rich gas enters the methane separation system, separated liquid methane flows out of the bottom of a methane rectifying tower and enters a liquid methane-argon heat exchanger in the argon circulation refrigeration system, cold energy of the liquid methane is transferred to circulating argon, and the circulating argon is used for providing cold energy for a tower top condenser in the methane separation system, so that the cold energy recovery process for separating the nitrogen-containing methane-rich gas is realized.
Further, the methane separation system comprises a methane rectifying tower, a tower bottom reboiler and a tower top dephlegmator; one end of the reboiler is connected with a raw material gas pipeline for conveying the nitrogen-containing methane-rich gas, and the other end of the reboiler is used for conveying the nitrogen-containing methane-rich gas into the methane rectifying tower through a methane rectifying tower feeding pipeline. The raw material containing nitrogen and methane-rich gas is used as a heat source of a reboiler, the raw material transfers heat energy to circulating liquid at the bottom of the tower in the reboiler, and part of the liquid at the bottom of the tower is gasified to form gas phase for separation; part of nitrogen in the ascending gas phase in the tower absorbs argon cold energy in the tower top dephlegmator and condenses into liquid nitrogen, so that reflux liquid in the tower is formed, and high-efficiency separation of methane and nitrogen is realized. And (3) passing through a methane separation tower to obtain a light component which does not contain methane at the top of the tower and comprises nitrogen and lighter hydrogen and carbon monoxide components, and obtaining liquid methane at the bottom of the tower.
Further, the argon circulation refrigerating system comprises a methane throttling expansion valve, a liquid methane-argon heat exchanger, a liquid argon throttling expansion valve, a cold energy heat exchanger, a circulating argon compressor and a first water-cooling heat exchanger, wherein the liquid methane flows into the heat absorption pipeline of the liquid methane-argon heat exchanger from the methane throttling expansion valve to release cold energy to circulating argon, the circulating argon enters the tower top condenser through the liquid argon throttling expansion valve to release cold energy, enters the cold energy heat exchanger through a low-pressure cold argon pipeline to release cold energy again, then enters the circulating argon compressor from a low-pressure reheating argon pipeline to be compressed, further increases the pressure, then enters the first water-cooling heat exchanger to cool and precool, enters the cold energy heat exchanger again through a high-pressure argon pipeline to cool and precool, and then enters the liquid methane-argon heat exchanger to obtain cold energy again to realize an argon circulation refrigerating main loop.
Further, the gas separated in the methane separation system flows out from the top of the methane rectifying tower, enters the cold energy heat exchanger to release cold energy, and then flows into the top gas utilization system from the reheating top gas pipeline. The cold energy heat exchanger at the top of the tower releases cold energy to the refrigerating system, so that the cold energy can be further recovered, and the utilization rate of the cold energy is improved. The gas phase at the top of the tower after reheating is discharged out of the system through a pipeline, and the separation of hydrogen, carbon monoxide and nitrogen (relative to purge gas), hydrogen and nitrogen (relative to dry gas) or hydrogen and helium (relative to oilfield associated gas) can be realized through pressure swing adsorption or membrane separation, so that the utilization rate of the purge gas and the dry gas is improved. The pressure swing adsorption or membrane separation of methane gas compression cooling and overhead gas can be performed by adopting a common technical method in industry.
Further, cold methane gas flowing out of the heat absorption pipeline of the liquid methane-argon heat exchanger enters the cold energy heat exchanger through the cold methane gas pipeline to release cold energy again, and then flows into the methane utilization system from the reheating methane gas pipeline. And the reheated methane gas is discharged out of the system through a pipeline, compressed and cooled according to the pressure requirement of a user, and then is input into a user pipe network.
Further, the argon circulation refrigeration system further comprises an argon circulation refrigeration auxiliary loop, the argon circulation refrigeration auxiliary loop comprises an argon expander, and the argon circulation refrigeration auxiliary loop specifically comprises: and after cooling and precooling, circulating argon gas which is separated from the argon circulation refrigeration main loop directly enters the expander through an expansion end inlet pipeline of the expander to be expanded and cooled, returns to the cold energy heat exchanger through an expansion end outlet pipeline of the expander to release cold energy and reheat, enters the compression end of the expander through a compression end inlet pipeline of the expander to increase pressure, enters a second water-cooling heat exchanger to be cooled through an outlet pipeline of the compression end of the expander to be cooled, enters the first water-cooling heat exchanger to be cooled after the pressure is further increased by the circulating argon gas compressor, and enters the cold energy heat exchanger to be cooled and precooled through a high-pressure argon gas pipeline to form an argon circulation refrigeration auxiliary loop. The system uses argon as a circulating working medium, recovers methane and nitrogen cold energy through a heat pump and a cold energy heat exchanger, supplements cold energy for an argon circulating refrigeration main loop through partial argon expander refrigeration, and transmits the cold energy to a methane separation system after improving the cold energy grade by utilizing an argon Joule-Thomson effect.
Further, the source of the nitrogen-containing methane-rich gas is methanol synthesis purge gas or nitrogen-containing methane gas after ethylene is removed from dry gas of an oil refining device, or methane gas after light hydrocarbon is removed from land and offshore oilfield associated gas, or coal bed gas shale gas after decarburization and purification. In addition to nitrogen and methane, the purge gas also includes hydrogen and carbon monoxide; the dry gas also contains hydrogen, and the dry gas can be used as a raw material to return to the original system after nitrogen is removed by a pressure swing adsorption or membrane separation method; for nitrogen-rich methane raw gas which takes associated gas of land and offshore oil fields as resources, besides nitrogen and methane, hydrogen and helium are also contained, and after nitrogen is removed by a pressure swing adsorption or membrane separation method, the hydrogen and the helium are recovered.
The invention further provides a separation method based on the argon circulation refrigeration nitrogen-containing methane-rich gas separation system, after the nitrogen-containing methane-rich gas is separated in the methane separation system, the separated liquid methane enters the liquid methane-argon heat exchanger, cold energy of the liquid methane is transferred to circulating argon, and the circulating argon is used for providing cold energy for a tower top condenser in the methane separation system, so that the nitrogen-containing methane-rich gas is separated.
Advantageous effects
According to the nitrogen-containing methane-rich separation system based on argon circulation refrigeration, argon is used as a working medium, methane and nitrogen cold energy of the separation system are recovered through a heat pump and a cold energy heat exchanger, part of argon expansion refrigeration is used for supplementing cold energy, then the argon Joule-Thomson effect is utilized for improving the cold energy grade and then is transmitted to the separation system, nitrogen and methane separation is realized through lower refrigeration energy consumption, wherein a gas phase at the top of a methane rectifying tower contains hydrogen, carbon monoxide and nitrogen (relative to purge gas), and hydrogen and nitrogen (relative to dry gas) or hydrogen and helium (relative to onshore or offshore oilfield associated gas), and after being discharged out of the separation system, the nitrogen can be removed through a pressure swing adsorption or membrane separation and other industrial common technical methods, and high-value resources such as hydrogen and helium are recovered.
Drawings
FIG. 1 is a schematic diagram of a nitrogen-containing methane-rich gas separation system based on argon cycle refrigeration in accordance with the present invention;
wherein, the device comprises a 1-tower bottom reboiler, a 1-1-raw gas pipeline, a 2-methane rectifying tower, a 2-1-methane rectifying tower feeding pipeline, a 2-2-tower top gas phase discharging pipeline, a 2-3-tower bottom liquid phase discharging pipeline, a 3-tower top segregator, a 3-1-low pressure cold argon pipeline, a 4-cold energy heat exchanger, a 4-1-reheating tower top gas pipeline, a 4-2-reheating methane gas pipeline, a 4-3-low pressure reheating argon pipeline, a 5-circulating argon compressor, a 6-first water-cooling heat exchanger, a 6-1-high pressure pre-cooling argon pipeline, a 7-liquid methane-argon heat exchanger, a 7-1-high pressure cold argon pipeline, a 7-2-cold methane gas pipeline, an 8-liquid argon throttling expansion valve, an 8-1-high pressure liquid argon pipeline, an 8-2-low pressure liquid argon pipeline, a 9-argon expansion machine, a 9-1-expansion end inlet pipeline, a 9-2-expansion end outlet, a 9-3-expansion machine compression end inlet pipeline, a 9-3-expansion machine inlet pipeline, a 9-4-liquid argon heat exchanger outlet pipeline, a 10-water-cooling heat exchanger and a second throttling heat exchanger.
Detailed Description
The invention is further described below in conjunction with the detailed description. It is to be understood that these examples are illustrative of the present invention and are not intended to limit the scope of the present invention. Further, it is understood that various changes and modifications may be made by those skilled in the art after reading the teachings of the present invention, and such equivalents are intended to fall within the scope of the claims appended hereto.
Example 1
The utility model provides a nitrogen-containing rich methane gas separation system based on argon circulation refrigeration, includes methane separation system and argon circulation refrigeration system, and after nitrogen-containing rich methane gas got into methane separation system, the liquid methane of separation got into in the liquid methane-argon heat exchanger 7 in the argon circulation refrigeration system after flowing out from the bottom of the methane rectifying column, transferred the cold energy of liquid methane to circulation argon, and circulation argon is used for providing cold energy for the top of a tower dephlegmator 3 in the methane separation system, realizes the separation of nitrogen-containing rich methane gas and uses cold energy recovery process.
The methane separation system comprises a methane rectifying tower 2, a reboiler 1 and a tower top dephlegmator 3; one end of the reboiler 1 is connected with a raw material gas pipeline 1-1 for conveying the nitrogen-containing methane-rich gas, and the other end of the reboiler is used for conveying the nitrogen-containing methane-rich gas into the methane rectifying tower 2 through a methane rectifying tower feeding pipeline 2-1. The raw material containing nitrogen and methane-rich gas is used as a heat source of a reboiler 1, the raw material transfers heat energy to the circulating liquid at the bottom of the tower in the reboiler 1, and part of the circulating liquid at the bottom of the tower is gasified to form gas phase for separation; part of nitrogen in the ascending gas phase in the tower absorbs argon cold energy in the tower top dephlegmator 3 and condenses into liquid nitrogen, so that reflux liquid in the tower is formed, and high-efficiency separation of methane and nitrogen is realized. The light components without methane, including nitrogen, lighter hydrogen, carbon monoxide and the like, are obtained at the top of the tower through a gas phase discharge pipeline 2-2 at the top of the tower through a liquid phase discharge pipeline 2-3 at the bottom of the tower through a methane rectifying tower 3.
Further, the argon circulation refrigerating system comprises a methane throttling expansion valve 11, a liquid methane-argon heat exchanger 7, a liquid argon throttling expansion valve 8, a cold energy heat exchanger 4, a circulating argon compressor 5 and a first water-cooling heat exchanger 6. The liquid methane flows into the circulating argon which is released by cold energy from the heat absorption pipeline of the liquid methane-argon heat exchanger 7 through the methane throttling expansion valve 11, the pipeline of the circulating argon before passing through the liquid argon throttling expansion valve 8 is a high-pressure liquid argon pipeline 8-1, and the pipeline after passing through the liquid argon throttling expansion valve 8 is a low-pressure liquid argon pipeline 8-2; after the circulating argon enters the tower top condenser 3 through the liquid argon throttling expansion valve 8 to release cold energy, the circulating argon enters the cold energy heat exchanger 4 through the low-pressure cold argon pipeline 3-1 to release cold energy again, then enters the circulating argon compressor 5 from the low-pressure reheating argon pipeline 4-3 to be compressed, enters the first water cooling heat exchanger 6 to be cooled and precooled, enters the cold energy heat exchanger 4 again through the high-pressure argon pipeline to be cooled and precooled, and then enters the liquid methane-argon heat exchanger 7 through the high-pressure cold argon pipeline 7-1 to obtain cold energy again, so that an argon circulating refrigeration main loop is realized.
Further, the gas separated in the methane separation system flows out from the top of the methane rectifying tower 2, enters the cold energy heat exchanger 4 to release cold energy, and then flows into the top gas utilization system from the reheating top gas pipeline 4-1. The cold energy heat exchanger 4 on the top of the tower releases cold energy to the refrigerating system, so that the cold energy can be further recovered, and the utilization rate of the cold energy is improved. The gas phase at the top of the tower after reheating is discharged out of the system through a pipeline, and the separation of nitrogen and other high-value gases, namely hydrogen carbon monoxide (relative to purge gas), hydrogen (relative to dry gas) or hydrogen and helium (relative to oilfield associated gas) can be realized through pressure swing adsorption or membrane separation, so that the utilization rate of the raw material gas is improved. The pressure swing adsorption or membrane separation of methane gas compression cooling and overhead gas can be performed by adopting a common technical method in industry.
Further, cold methane gas flowing out of the heat absorption pipeline of the liquid methane-argon heat exchanger 7 enters the cold energy heat exchanger 4 through the cold methane gas pipeline 7-2 to release cold energy again, and then flows into the methane utilization system from the reheating methane gas pipeline 4-2. And the reheated methane gas is discharged out of the system through a pipeline, compressed and cooled according to the pressure requirement of a user, and then is input into a user pipe network.
Further, the argon circulation refrigeration system also comprises an argon circulation refrigeration auxiliary loop, wherein the argon circulation refrigeration auxiliary loop comprises an argon expander 9, and specifically: one path of circulating argon gas separated from the argon circulating refrigeration main loop enters the cold energy heat exchanger 4 for cooling and precooling, then directly enters the expander 9 for expansion and cooling through the expander expansion end inlet pipeline 9-1, returns to the cold energy heat exchanger 4 through the expander expansion end outlet pipeline 9-2 for releasing cold energy and reheating, enters the expander compression end through the expander compression end inlet pipeline 9-3 for increasing pressure, enters the second water-cooling heat exchanger 10 for cooling through the expander compression end outlet pipeline 9-4, enters the first water-cooling heat exchanger 6 for cooling after further increasing pressure through the circulating argon gas compressor 5, and enters the cold energy heat exchanger 4 for cooling and precooling through the high-pressure precooled argon gas pipeline 6-1 to form the argon circulating refrigeration auxiliary loop. The system takes argon as a circulating working medium, methane and nitrogen cold energy are recovered through a heat pump and cold energy heat exchanger 4, part of argon is refrigerated through an expander 9 to supplement cold energy for an argon circulating refrigeration main loop, and then the argon Joule-Thomson effect is utilized to improve the cold energy grade and then is transmitted to a methane separation system.
Further, the source of the nitrogen-containing methane-rich gas is the nitrogen-containing methane gas after the ethylene is removed by the methanol synthesis purge gas or the dry gas of the oil refining device, or the methane gas after the light hydrocarbon is removed by the land and offshore oilfield associated gas, or the coal bed gas shale gas after decarburization and purification. In addition to nitrogen and methane, the purge gas also includes hydrogen and carbon monoxide; the dry gas also contains hydrogen, and the dry gas can be used as a raw material to return to the original system after nitrogen is removed by a pressure swing adsorption or membrane separation method; for nitrogen-rich methane raw gas which takes associated gas of land and offshore oil fields as resources, besides nitrogen and methane, hydrogen and helium are also contained, and after nitrogen is removed by a pressure swing adsorption or membrane separation method, the hydrogen and the helium are recovered.
Furthermore, the invention also provides a separation method based on the argon circulation refrigeration nitrogen-containing methane-rich gas separation system, after the nitrogen-containing methane-rich gas is separated in the methane separation system, the separated liquid methane enters the liquid methane-argon heat exchanger 7, cold energy of the liquid methane is transferred to circulating argon, and the circulating argon is used for providing cold energy for the tower top dephlegmator 3 in the methane separation system, so that the nitrogen-containing methane-rich gas is separated.
According to the argon circulation refrigerating system, argon is used as a circulation working medium, methane and nitrogen cold energy of a separating system is recovered through a heat pump and a cold energy heat exchanger, the cold energy is supplemented through partial argon expansion refrigeration, then the cold energy grade is improved through an argon Joule-Thomson effect and then is transmitted to a nitrogen-containing methane-rich gas separating system, high-efficiency separation is realized with lower refrigeration energy consumption, high-price utilization of industrial tail gas resources such as dry gas, purge gas and the like is realized, hydrogen, helium, methane and light hydrocarbon are recovered from associated gas of land and ocean oil fields, and the methane recovery rate can reach more than 99%.
According to the argon circulation refrigerating system, the liquid methane-argon heat exchanger is adopted, the argon is used as a working medium to recycle LNG cold energy through the heat pump, the cold energy grade is improved by utilizing the Joule-Thomson effect of the argon and then is transmitted to a cooled medium, the LNG cold energy utilization rate can be effectively improved, the LNG cold energy utilization rate is improved to be more than 90%, the environment-friendly concept is better realized, and the energy-saving effect is clearly recorded in patent texts of application numbers 2018100218512 or 2018200373138 of the applicant.
While the methods and techniques of the present invention have been described in terms of preferred embodiments, it will be apparent to those skilled in the art from this disclosure that variations and rearrangements of the methods and techniques can be made by those skilled in the art to arrive at a final preparation technique without departing from the spirit and scope of the invention. It is expressly intended that all such similar substitutes and modifications apparent to those skilled in the art are deemed to be included within the spirit, scope and content of the invention.

Claims (3)

1. A nitrogen-containing methane-rich gas separation system based on argon circulation refrigeration is characterized in that: the system comprises a methane separation system and an argon circulation refrigerating system, wherein after nitrogen-containing methane-rich gas enters the methane separation system, separated liquid methane flows out from the bottom of a methane rectifying tower and enters a liquid methane-argon heat exchanger in the argon circulation refrigerating system, cold energy of the liquid methane is transferred to circulating argon, and the circulating argon is used for providing cold energy for a tower top dephlegmator in the methane separation system, so that a cold energy recovery process for separating the nitrogen-containing methane-rich gas is realized;
the methane separation system comprises a methane rectifying tower, a tower bottom reboiler and a tower top dephlegmator; one end of the reboiler is connected with a raw material gas pipeline for conveying the nitrogen-containing methane-rich gas, and the other end of the reboiler is used for conveying the nitrogen-containing methane-rich gas into the methane rectifying tower through a methane rectifying tower feeding pipeline;
the method comprises the steps that argon is adopted as a refrigeration cycle working medium, an argon circulation refrigeration system comprises a methane throttling expansion valve, a liquid methane-argon heat exchanger, a liquid argon throttling expansion valve, a cold energy heat exchanger, a circulating argon compressor and a first water-cooling heat exchanger, cold energy is released to the circulating argon through a heat absorption pipeline of the liquid methane-argon heat exchanger, the circulating argon enters an overhead condenser through the liquid argon throttling expansion valve to release cold energy, then enters the cold energy heat exchanger through a low-pressure cold argon pipeline to release cold energy again, then enters the circulating argon compressor from a low-pressure reheating argon pipeline to be compressed, further increases the pressure, then enters the first water-cooling heat exchanger to cool and precool, enters the cold energy heat exchanger again through a high-pressure precooled argon pipeline to cool and precool, and then enters the liquid methane-argon heat exchanger to obtain cold energy again, and a main circulation refrigeration loop is realized;
the gas separated in the methane separation system flows out from the top of the methane rectifying tower and then enters the cold energy heat exchanger to release cold energy, and then flows into a tower top gas utilization or discharge system from a reheating tower top gas pipeline;
cold methane gas flowing out of a heat absorption pipeline of the liquid methane-argon heat exchanger enters the cold energy heat exchanger through a cold methane gas pipeline to release cold energy again, and then flows into a methane utilization system from a reheating methane gas pipeline;
the argon circulation refrigerating system also comprises an argon circulation refrigerating auxiliary loop, wherein the argon circulation refrigerating auxiliary loop comprises an argon expander, and the argon circulation refrigerating auxiliary loop comprises the following components: and after cooling and precooling, circulating argon gas which is separated from the argon circulation refrigeration main loop directly enters the expander through an expansion end inlet pipeline of the expander, is expanded and cooled in the expander, returns to the cold energy heat exchanger through an expansion end outlet pipeline of the expander to release cold energy and reheat, enters the expander through a compression end inlet pipeline of the expander to increase the pressure, enters a second water-cooling heat exchanger to cool through an outlet pipeline of the compression end of the expander, enters a first water-cooling heat exchanger to cool after further increasing the pressure through a circulating argon gas compressor, and enters the cold energy heat exchanger to cool and precool through a high-pressure precooled argon gas pipeline to form an argon circulation refrigeration auxiliary loop.
2. The nitrogen-containing methane-rich gas separation system based on argon circulation refrigeration of claim 1, wherein: the source of the nitrogen-containing methane-rich gas is nitrogen-containing methane gas after ethylene is removed from methanol synthesis purge gas or oil refining device dry gas, or methane gas after light hydrocarbon is removed from land and offshore oilfield associated gas, or coal bed gas shale gas after decarburization and purification.
3. The separation method based on the argon circulation refrigeration nitrogen-containing methane-rich gas separation system according to any one of claims 1 to 2, characterized by: after the nitrogen-containing methane-rich gas is separated in the methane separation system, the separated liquid methane enters the liquid methane-argon heat exchanger, cold energy of the liquid methane is transferred to circulating argon, and the circulating argon is used for providing cold energy for a tower top condenser in the methane separation system, so that the nitrogen-containing methane-rich gas is separated.
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