CN103776238A - Method and equipment for separating methane from synthesis gas - Google Patents

Method and equipment for separating methane from synthesis gas Download PDF

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Publication number
CN103776238A
CN103776238A CN201310757056.7A CN201310757056A CN103776238A CN 103776238 A CN103776238 A CN 103776238A CN 201310757056 A CN201310757056 A CN 201310757056A CN 103776238 A CN103776238 A CN 103776238A
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cold
heat exchanger
producing medium
expander
methane
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Chinese (zh)
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H·施密特
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Linde GmbH
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Linde GmbH
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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
    • F25J3/0204—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
    • F25J3/0223—H2/CO mixtures, i.e. synthesis gas; Water gas or shifted synthesis 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
    • 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
    • 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
    • F25J3/0271—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 H2/CO mixtures, i.e. of synthesis 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
    • F25J2200/00—Processes or apparatus using separation by rectification
    • F25J2200/40—Features relating to the provision of boil-up in the bottom of a 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
    • F25J2200/72—Refluxing the column with at least a part of the totally 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
    • F25J2200/00—Processes or apparatus using separation by rectification
    • F25J2200/78—Refluxing the column with a liquid stream originating from an upstream or downstream fractionator 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
    • F25J2205/00—Processes or apparatus using other separation and/or other processing means
    • F25J2205/30—Processes or apparatus using other separation and/or other processing means using a washing, e.g. "scrubbing" or bubble column for purification purposes
    • 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
    • F25J2215/00—Processes characterised by the type or other details of the product stream
    • F25J2215/02—Mixing or blending of fluids to yield a certain product
    • 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
    • F25J2215/00—Processes characterised by the type or other details of the product stream
    • F25J2215/04—Recovery of liquid products
    • 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
    • F25J2230/00—Processes or apparatus involving steps for increasing the pressure of gaseous process streams
    • F25J2230/08—Cold compressor, i.e. suction of the gas at cryogenic temperature and generally without afterstage-cooler
    • 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
    • F25J2245/00—Processes or apparatus involving steps for recycling of process streams
    • F25J2245/02—Recycle of a stream in general, e.g. a by-pass stream
    • 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
    • F25J2270/14—External refrigeration with work-producing gas expansion loop
    • F25J2270/16—External refrigeration with work-producing gas expansion loop with mutliple gas expansion loops of the same refrigerant
    • 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
    • F25J2270/42—Quasi-closed internal or closed external nitrogen refrigeration cycle
    • 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
    • F25J2290/00—Other details not covered by groups F25J2200/00 - F25J2280/00
    • F25J2290/34—Details about subcooling of liquids

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Mechanical Engineering (AREA)
  • Thermal Sciences (AREA)
  • General Engineering & Computer Science (AREA)
  • Separation By Low-Temperature Treatments (AREA)

Abstract

The invention proposes a method for separating methane (LNG) from a methane-containing synthesis gas (SYN) in low temperature separation equipment (10). The low temperature separation equipment includes a refrigerant circuit having at least one expander (X1) and at least one separating column (S2) having a condenser (E5), and A portion of compressed and cooled refrigerant from the refrigerant circuit is supplied to the at least one expander (X1) and the condenser (E5) respectively. A primary portion of the refrigerant which is cooled to an intermediate temperature (TI) from a starting temperature (TA) is supplied to the at least one expander (X1). A secondary portion of the refrigerant which is firstly cooled to an intermediate temperature (TI) from a starting temperature (TA) and then cooled to a lower final temperature (TE) is supplied to the condenser (E5). The invention also relates to equipment (10, 11, 12) used for implementing the method according to the invention.

Description

Isolate the method and apparatus of methane from synthesis gas
Technical field
The present invention relates to synthesis gas from containing methane and isolate method and the corresponding equipment of methane.
Background technology
The synthesis gas of preparing from coal, oil or natural gas by known method conventionally also contains content and is generally the methane of 3 to 30 volume % and other components of less amount after removing sour gas except containing desired component hydrogen and carbon monoxide.For example nitrogen, oxygen, argon, carbon dioxide and the ethane that is less than separately 1 volume %.Because do not wish to have especially methane in synthesis gas, so be conventionally isolated out.
Can in cryogenic separation, isolate methane from the synthesis gas that contains methane.This equipment can utilize refrigerating circuit operation, and in refrigerating circuit, cold-producing medium compresses the in the situation that for example in multistage mode and in centre, cooling and later stage being cooling.So it is cooling that compressed cold-producing medium can carry out in one or more heat exchangers.Subsequently, compressed and cooling cold-producing medium is to produce the mode of refrigeration
Figure BSA0000100514000000011
decompression.
For example US2009/0205367A1 discloses synthesis gas from containing methane and has isolated the method and system of methane.
Especially the in the situation that of needing liquid refrigerant or corresponding two-phase mixture in corresponding equipment, known method is proved to be inefficiency, and this is because the generation of this type of mixture and/or processing are compressed, cooling, reducing pressure and/or carrying is accompanied by sizable cost conventionally.
Therefore, the object of the invention is to set forth the possibility of more effectively isolating methane from the synthesis gas that contains methane.
Summary of the invention
Under this background, method and the corresponding equipment of methane is isolated in the present invention's suggestion from the synthesis gas that contains methane, and it has the feature of independent claims.Preferred embodiment is the theme of each dependent claims and following description.
In this application, the material in equipment or method and for example synthesis gas of mixture of substances and cold-producing medium are called to " stream " and " fraction ".Stream guides in the pipeline for this reason arranging usually used as fluid.Fraction typically refers to the starting mixt by the isolated part of starting mixt.Fraction can form corresponding stream in the time correspondingly guiding.Stream for example can return for starting mixt is provided, and can isolate fraction by this starting mixt.
Stream or fraction can " be rich in " or " content is low " one or more components, wherein separately based on weight basis or volume reference, " be rich in " and represent that content is greater than 75%, 80%, 85%, 90%, 95%, 99%, 99.5% or 99.9%, " content is low " represents to be less than 25%, 20%, 15%, 10%, 5%, 1%, 0.5% or 0.1%.
Advantage of the present invention
The inventive example is as can be for isolating the method for methane from the synthesis gas that contains methane, fraction at the bottom of the tower that wherein goes out to be rich in methane and contain carbon monoxide from synthesis gas cryogenic separation in the first knockout tower, and in second knockout tower with condenser from fraction desorb carbon monoxide at the bottom of tower.The application's applicant has developed the cryogenic separation that can be used for this, and it is the theme of parallel patent application.This environment division ground shows, and is at length explained in affiliated accompanying drawing declaratives in Fig. 1.
Can be first by the cooling synthesis gas that contains methane of heat exchange in this type of cryogenic separation.Fraction at the bottom of the tower that goes out to be rich in methane and contain carbon monoxide from the cooling synthesis gas cryogenic separation that contains methane in the first knockout tower.At the bottom of the tower that this is rich in to methane and contains carbon monoxide, fraction is delivered in the second knockout tower, makes carbon monoxide substantially from fraction desorb (stripping goes out) at the bottom of tower in the second knockout tower.The overhead streams that particularly obtains the methane fraction that carbon dioxide content is low and be rich in carbon monoxide at this.The latter can be used as to reflux and returns in the first knockout tower.
Described cryogenic separation comprises the refrigerant circulation with for example nitrogen of cold-producing medium.In this refrigerant circulation, cold-producing medium is compressed to paramount final pressure from low initial pressure in the situation that for example cooling and later stage being cooling in multistage mode and in centre.Then compressed cold-producing medium is cooled to lower medium temperature at the first heat exchanger for the cooling synthesis gas that contains methane also by initial temperature.
At same the second heat exchanger for the cooling synthesis gas that contains methane, the Part I of the cold-producing medium that is cooled to medium temperature is directly continued to be cooled to lower final temperature.Unlike this, the Part II of the cold-producing medium that is cooled to medium temperature is not cooled to final temperature, but is delivered to tower bottom reboiler and the side evaporimeter of the second knockout tower.Cold-producing medium is also cooling to a certain extent at this.Again this two parts cold-producing medium is converged subsequently.Obtain thus cold-producing medium stream, its temperature is made up of this two-part contribution.
Then, cold-producing medium stream to produce the decompression of doing work of the mode of refrigeration, and is sent in the condenser of the second knockout tower in expander.Condenser is for example designed to overhead condenser.Cold-producing medium when decompression partly condensation go out.In the application's category, the pressure producing due to decompression is called to feed pressure (Einspeisedruck).
The condenser of the second knockout tower, for cooling fluid of being discharged in tower top side by the second knockout tower, by making compressed and cooling cold-producing medium stream be decompressed to feed pressure and be sent in condenser, also makes described condenser cooling, thereby makes cold-producing medium stream cooling.Make thus the liquefaction at least in part of cold-producing medium stream.Another stock-traders' know-how compression and cooling cold-producing medium stream are used for making expander work.In expander, the mode that makes cold-producing medium flow the to produce refrigeration decompression of doing work.
The cold-producing medium that partly condensation goes out can heat and evaporation completely after condenser is discharged.Then there is again its initial pressure and initial temperature thereof, and can again be compressed to as previously mentioned final pressure.Therefore refrigerant circulation seals.
For cooler condenser, need to be decompressed to the specific liquid part of the cold-producing medium of feed pressure, have submerged heat exchanger because carry out cooling condenser for the tower top fraction to from the second knockout tower, this heat exchanger must be covered by liquid in the course of the work.But be present in the validity variation of the described liquid part of the cold-producing medium in the exit of expander used.In addition, in described method, also limit the available initial pressure of maximum of cold-producing medium, this is because particularly due to the pressure loss in the pipeline that causes leading to condenser that increases of liquid part in the cold-producing medium that is decompressed to feed pressure.Therefore, need many circulating energies, so that cold-producing medium is compressed to its final pressure separately.Required compressor is correspondingly expensive.
Generally speaking, also relate to the method for isolating methane in cryogenic separation from the synthesis gas that contains methane, described cryogenic separation comprises the knockout tower that has the refrigerant circulation of at least one expander and at least one and have condenser, wherein the cold-producing medium of compressed and cooling part is supplied to described at least one expander and condenser from refrigerant circulation.
According to the present invention, the cold-producing medium that is cooled to the Part I of medium temperature by initial temperature is supplied to expander, and is supplied to condenser by being cooled to by initial temperature the cold-producing medium that then medium temperature continue the Part II that is cooled to lower final temperature first equally.At this, preferably described Part I and Part II are cooled to medium temperature as common cold-producing medium stream.
Therefore, different from aforementioned device, condenser used needs the specific liquid part of the cold-producing medium of sending into, and it is not via expander supply, but for example via the pressure-reducing valve supply arranging for this reason.Be different from equally the working method of aforementioned device, expander is to utilize not to be cooled in advance final temperature the therefore cold-producing medium work of hotter part.
As previously mentioned, for the cold-producing medium of Part II is supplied in condenser, more preferably use pressure-reducing valve, utilize pressure-reducing valve to make the cold-producing medium of Part II be decompressed to feed pressure, and liquefaction at least in part thus.Different from expander, pressure-reducing valve can also be without any problems for providing the cold-producing medium stream of partial liquefaction.Unlike this, the expander of other existence can utilize gaseous flow work completely.Improve thus validity.
More preferably use at least one first heat exchanger so that the cold-producing medium of the first and second parts is cooled to medium temperature from initial temperature, and use the second heat exchanger so that the cold-producing medium of Part II is continued to be cooled to final temperature from medium temperature.It is preferably heat-exchangers of the plate type, and it can be cooling or heating a plurality of fluids, thereby can reduce cost of equipment, and can reduce thermal losses.In the time that the first and second parts are cooled to medium temperature, can as described belowly add other heat exchanger at this.
Before in the synthesis gas that contains methane is sent into the first knockout tower, more preferably also in the first heat exchanger, carry out coolingly, then in the second heat exchanger, carry out cooling.Refrigeration requirement and the heat demand of the second knockout tower are provided by same refrigerating circuit thus, and provide the cooling synthesis gas that contains methane required cold.Preferably by the decompression cold in described expander and optionally discharging in one or more other expanders for the cooling synthesis gas that contains methane.Synthesis gas by containing methane can be guided through equally to heat exchanger by the synthesis gas product of isolating methane acquisition in the adverse current of the synthesis gas with respect to containing methane.
Particularly advantageously, in described method, use at least one other heat exchanger, in wherein the fluid of discharging at definite feeding At The Height of at least one knockout tower being heated.At this, other heat exchanger for example can be designed to so-called tower bottom reboiler, in described tower bottom reboiler, can the fluid of being discharged in tower bottom side by the second knockout tower be heated and optionally be evaporated.In addition other heat exchanger designs can also be become, to the form of so-called side evaporimeter.In wherein can the fluid of for example discharging at the bottom of knockout tower tower being heated and optionally be evaporated.By using corresponding heat exchanger to improve the separative efficiency in the second knockout tower.
More preferably can be at least one in other heat exchanger at least a portion of the cold-producing medium to the first and second parts cooling in the first heat exchanger continue cooling.In other words, use the cold-producing medium in refrigerant circulation at this, for example, in tower bottom reboiler, the fluid of discharging at least one definite feeding At The Height of the second knockout tower is heated.Can reduce thus its temperature, and the cold discharging when the fluid of discharging at least one definite feeding At The Height of the second knockout tower is heated is effectively utilized.
Alternatively or extraly, at least one in other heat exchanger, can also proceed the synthesis gas that contains methane cooling in the first heat exchanger coolingly, the fluid of discharging from the second knockout tower be heated thus simultaneously.Reduce thus the required energy of the cooling synthesis gas that contains methane.
In these class methods, it can be also favourable in the second heat exchanger, at least a portion of fraction at the bottom of the isolated tower that contains carbon monoxide in the first knockout tower being heated.Other the heat exchanger (tower bottom reboiler and/or side evaporimeter) that can dispense thus otherwise need.
In a corresponding method, more preferably make Part I cold-producing medium in expander with acting and/or provide the mode of refrigeration to reduce pressure, send into subsequently the cold junction of the second heat exchanger.As previously mentioned, can effectively utilize thus the decompression cold producing in expander.Because expander only utilizes gas work, so it is with higher validity work.
Particularly advantageously, in the second heat exchanger, a part for fraction at the bottom of the isolated tower that is rich in methane and contain carbon monoxide in the first knockout tower is heated, and send in the second knockout tower at definite entry level place.Can dispense thus the side evaporimeter of common needs.The function of side evaporimeter realizes by the second heat exchanger, and this has reduced cost of equipment and has reduced thermal losses.
More preferably by first or the refrigerant compression to 50 of Part II to 100 bar, the especially pressure of 60 to 90 bar, and/or decompression to 8 to 20 bar, the especially feed pressure of 10 to 15 bar (PC), and/or be cooled to the medium temperature (TI) of-120 to-170 ℃, especially-130 to-160 ℃, and/or be cooled to the final temperature (TE) of-140 to-180 ℃, especially-150 to-170 ℃.
In a corresponding method, more preferably use cold-producing medium 80% as Part I, and/or use cold-producing medium 20% as Part II.Described various piece for example can regulate according to the refrigeration requirement in condenser and/or the second heat exchanger.
More preferably use main compressor and at least one later stage compressor that cold-producing medium is compressed to final pressure from initial pressure.As previously mentioned the Part I cold-producing medium that is cooled to medium temperature by initial temperature is supplied to expander, expander is connected with later stage compressor.If a later stage compressor is only set, coupled in the case; Be provided with more than one later stage compressor in the situation that unlike this, (being the last later stage compressor in tandem compressor unit) is connected with the later stage compressor that final pressure is provided.Expander is mechanically connected with this later stage compressor, and drives this later stage compressor.Its permission is worked especially effectively, especially depends on the amount of methane to be separated and depends on thus required cold, only needs an expander or second expander, so it is mechanically connected with other later stage compressor.
Equipment according to the present invention is isolated the method for methane from the synthesis gas that contains methane described in being designed to implement, and has corresponding device.It has benefited from above-mentioned advantage in the same manner, therefore can be with reference to these advantages.
Basic thought of the present invention is generally, the cold-producing medium stream reducing pressure is directly supplied to the condenser of the second knockout tower in pressure-reducing valve.Be not via expander, but directly provide cold via the discharge currents of choke valve to condenser.
Another basic thought of the present invention is, by cold-producing medium diverting flow, wherein the first gaseous state tributary is supplied to expander in expander upstream, and cooling the second gaseous state tributary, in choke valve, reduce pressure, and send into as low pressure refrigerant in the condenser of the second knockout tower.
According to the present invention particularly advantageously, expander is worked as follows, makes the discharge currents of expander be gaseous state.Make thus expander there is high validity.Expander preferably can work as follows, and outlet is roughly within the scope of the dew point in cold-producing medium.In addition, can also this mode improve the swabbing pressure of the compressor of refrigerant circulation, this has improved the validity of described process equally.
Further set forth the present invention according to accompanying drawing below, these accompanying drawings are depicted as other preferred embodiments of the present invention.
Accompanying drawing explanation
Figure 1 shows that the schematic diagram of being isolated the equipment of methane according to prior art by the synthesis gas that contains methane.
Figure 2 shows that the schematic diagram of being isolated the equipment of methane according to one embodiment of the invention by the synthesis gas that contains methane.
Figure 3 shows that the schematic diagram of being isolated the equipment of methane according to one embodiment of the invention by the synthesis gas that contains methane.
Figure 4 shows that the schematic diagram of being isolated the equipment of methane according to one embodiment of the invention by the synthesis gas that contains methane.
In figure, identical Reference numeral represents the element of identical or mutual correspondence.Unless be otherwise noted separately, the statement about pressure, temperature, composition etc. related in Fig. 1 relates to the embodiment of the present invention shown in Fig. 2 to 4 too.
The specific embodiment
Figure 1 shows that the non-equipment of being isolated methane by the synthesis gas that contains methane of the present invention.On this Whole Equipment, represent with Reference numeral 100.
Equipment 100 has the first knockout tower S1 and the second knockout tower S2.The first knockout tower S1 and the second knockout tower S2 work under different pressure.Pressure differential is for example 5 to 30 bar, especially 10 to 20 bar.Can be by the pressure limit of the second knockout tower S2 at 25 to 30 bar, to guarantee that pressure differential between gas phase and liquid phase is for 240kg/m at least 3, especially at least 270kg/m 3.
The synthesis gas SYN that contains methane is cooled in the first heat exchanger E1 to the temperature of for example-60 to-110 ℃, especially-80 to-95 ℃, and in the second heat exchanger E2, be cooled to the temperature of for example-120 to-170 ℃, especially-130 to-160 ℃, be then supplied to the first knockout tower S1 at definite entry level place.In the first knockout tower S1, can utilize via the circulation of being rich in carbon monoxide of pump L1 pumping and wash out methane from the synthesis gas SYN that contains methane.Fraction at the bottom of the tower that obtains in this way the tower top fraction that methane content is low and be rich in methane and contain carbon monoxide.
Isolate fraction at the bottom of the tower that contains carbon monoxide in the bottom of the first knockout tower S1.Discharge the low tower top fraction of methane content from the tower top of the first knockout tower S1, in heat exchanger E2 and E1, heat, and discharge as the synthesis gas product P RO that is for example 0.01 to 1.00 volume %, especially 0.1 to 0.5 volume % by dilution to methane residual content.
Via valve V3 by the tower that is rich in methane and contains carbon monoxide from the first knockout tower S1 at the bottom of fraction be decompressed to the pressure of the second knockout tower S2, send into wherein at definite entry level place again.The second knockout tower S2 works as so-called carbon monoxide stripper.Be provided with the third and fourth heat exchanger E3 and E4 for this reason, they are worked as tower bottom reboiler (the 3rd heat exchanger E3) on the one hand, work as side evaporimeter (the 4th heat exchanger E4) on the other hand, and utilize cold-producing medium to heat.In addition, the second knockout tower S2 also has condenser E5, and it is for example designed to overhead condenser, and therein can be by the steam-condensation rising in the second knockout tower S2 out.
Can at the bottom of the tower of the second knockout tower S2, obtain thus the low methane fraction of carbon dioxide (carbon monoxide) content, its carbonomonoxide concentration is for example 0.01 to 1.00 volume %, especially 0.1 to 0.5 volume %.For example can be guided through heat exchanger E2.Optionally, its form using methane product LNG can be discharged as boiling liquid or subcooled liquid or the gas under pressure arbitrarily.For example, by the scope selection pressure of 1 to 100 bar.Methane product LNG can be divided into equally to multiple parallel product streams with different discharge states, for example liquid state, boiling, the cold and/or gaseous state of mistake.
The gaseous overhead fraction of the second knockout tower S2 is again compressed to the pressure of the first knockout tower S1 in recycle compressor (R ü ckverdichter) C4, and is sneaked into the incoming flow SYN that leads to the first knockout tower S1.
Discharge from the uppermost column plate of the second knockout tower S2 the liquid overhead streams that is rich in carbon monoxide, in described pump L1, be pumped to the pressure of the first knockout tower S1, and deliver to the first knockout tower S1 as the backflow of being rich in carbon monoxide.Its in the first knockout tower S1 for washing out methane.
The refrigerant circulation of preferred sealing is set with cooling or heating the second knockout tower S2, for making the 3rd heat exchanger E3, the 4th heat exchanger E4 and condenser E5 work.
It comprises preferred multistage main compressor C1 and the first and second later stage compressors (supercharger Booster) C2 and the C3 with intercooler E6, E7 and E8, and it has later stage cooler E9.In main compressor C1 and later stage compressor C2 and C3, drying nitrogen pure for example technology of gaseous refrigerant can be compressed to for example 50 to 100 bar, especially the final pressure PE of 60 to 90 bar from the initial pressure PA of for example 5 to 20 bar, especially 8 to 15 bar via corresponding intermediate pressure.According in this related definition, initial pressure PA is positioned at the suction side of main compressor C1, and final pressure PE is positioned at later stage compressor C3 on the pressure side, shows in the drawings with dotted line frame.
Can drive the first later stage compressor C2 and the second later stage compressor C3 by the expander X2 and the X1 that utilize equally cold-producing medium work separately.Cold-producing medium in expander X2 and X1 separately with acting and provide the mode of refrigeration to reduce pressure, wherein by the cold discharging separately for making the first and second heat exchanger E1 and E2 work, and by the mechanical output discharging for making the first and second later stage compressor C2 and C3 work.Also expander X1 and X2 are called to " heat " and " cold " expander X2 and X1 according to the optional temperature of the cold-producing medium of decompression therein below, the expander X2 of wherein said heat belongs to the first later stage compressor C2, and the first expander belongs to the second later stage compressor C3.
If should discharge and be rich in the product of methane and need thus less cold with gaseous state, can dispense hot expander X2 and dispense thus the first later stage compressor C2.If incoming flow E contains the methane that is less than 10 volume %, is especially less than 7 volume %, this is especially applicable.With this understanding, even without the cold of expander X2 that carrys out self-heating, also can meet economically the refrigeration requirement in the first heat exchanger E1.
If there is hot expander X2, the cold-producing medium that can make " heat " part is therein to provide the mode of refrigeration and acting reduce pressure for example 5 to 20 bar, the especially pressure of 8 to 15 bar.Then the cold-producing medium stream through decompression can be continued to heating in the first heat exchanger E1, then again be supplied to main compressor C1.
If there is not hot expander X2, make whole cold-producing mediums, be the part not reducing pressure in hot expander X2 in other cases, in the first heat exchanger E1, be first cooled to the temperature of for example-60 to-110 ℃, especially-80 to-95 ℃ from initial temperature TA.
Then from the first heat exchanger E1 distribute major part for example 40 to 90%, 75 to 85% cold-producing medium especially, be supplied to the third and fourth heat exchanger E3 and E4, and at the bottom of this uses it for the tower from the fluid of the second knockout tower S2, boil again or side evaporation.At this, this part is further cooled to the temperature of for example-90 to-130 ℃, especially-105 to-120 ℃.
Unlike this, in the first heat exchanger E1, then the smaller portions of the cold-producing medium from the first heat exchanger E1 for example 5 to 25% are further cooled to the lower final temperature TE of for example-120 to-170 ℃, especially-130 to-160 ℃ in the second heat exchanger E2 after cooling.
Subsequently this two-part cold-producing medium is converged again, jointly in cold expander X1, reduce pressure.At this, this part cold-producing medium guiding process valve V2 of final temperature TE will be cooled to.
By decompression in expander X1 wherein there is a part for example 1 to 30 % by weight, the especially liquid refrigerant of 5 to 25 % by weight in partly liquefaction after decompression with cold-producing medium.Amount and temperature that cold-producing medium enters this part cold-producing medium that inlet temperature in cold expander X1 for example can be by being cooled to final temperature TE are regulated, thereby after decompression, obtain desired liquid part in cold expander X1.In the application's category, post-decompression pressure is called to " feed pressure (Einspeisedruck) ".
The cold-producing medium of partial liquefaction is supplied to condenser E5 under thus obtained feed pressure PC.In condenser E5, make the liquid part evaporation of at least a portion.Subsequently can be by the cold-producing medium for example now with 0 to 20%, especially 0 to 10% liquid part on the one hand via thering is the liquid line of valve V4 and discharging discretely from the top of condenser E5 via gas piping on the other hand, if desired evaporation completely in heat exchanger E2 and E1, and optionally overheated, be again supplied to subsequently main compressor C1.
Need certain refrigerant liquid polymorphic segment fully cooling to carry out in condenser E5.Therefore cold-producing medium must exist with two-phase form in the exit of cold expander X1.As described in, this can make the validity variation of cold expander X1.In addition, shown in arrangement in, can be limited by cold-producing medium evaporating pressure required in E5 as the maximum pressure of initial pressure PA.
Figure 2 shows that the schematic diagram of being isolated the equipment of methane according to one embodiment of the invention by the synthesis gas that contains methane, represent with Reference numeral 10 on the whole.Equipment 10 has the basic module of aforementioned device 100.
From wherein different to the equipment 100 of the condenser E5 feed of the second knockout tower S2 via cold expander X1, pressure-reducing valve V1 is set in equipment 10 for this reason.Different from the working method of equipment 100, in equipment 10 cold expander X1 utilize before without over-heat-exchanger E2 therefore hotter part of refrigerant work.
As described in reference device 100 before, all first cold-producing mediums or the part that do not reduce pressure in the optional hot expander X2 existing carry out cooling in the first heat exchanger E1.
Can distribute subsequently for example 50 to 97% cold-producing medium of a part, and be guided through as previously mentioned the third and fourth heat exchanger E3 and E4.This as described in carry out cooling accordingly.After again converging with the not directed remainder through the third and fourth heat exchanger E3 and E4, cold-producing medium has medium temperature TI, and this medium temperature is on the one hand by the cooling procedure in the first heat exchanger E1 and produced by the further cooling procedure of the part in heat exchanger E3 and E4 on the other hand.As described in, cold-producing medium is cooled in the first heat exchanger E1 to the temperature of for example-60 to-120 ℃, especially-90 to-110 ℃.The part correspondingly distributing is further cooled to the temperature of for example-80 to-130 ℃, especially-100 to-120 ℃ in the third and fourth heat exchanger E3 and E4.Therefore medium temperature TI is between these temperature, and still in all cases all higher than final temperature TE, this final temperature reaches in the second heat exchanger, for example-140 to-180 ℃, especially-150 to-170 ℃.
Now the cold-producing medium with medium temperature TI is repartitioned and become the first and second parts.For example 60 to 95% cold-producing medium of Part I is supplied to cold expander X1.Because the medium temperature TI of cold-producing medium that is supplied to cold expander X1 is higher than the final temperature TE adopting in equipment 100, in cold expander X1, do not liquefy.Therefore cold expander X1 can work more effectively.
Unlike this, Part II is that remainder is directly cooled to from described medium temperature TI the final temperature TE repeatedly addressing subsequently, as described in be for example-140 to-180 ℃, especially-150 to-170 ℃.This Part II cold-producing medium is decompressed to feed pressure PC via pressure-reducing valve V1, and sends in condenser E5.Make thus cold-producing medium liquefy partially or completely.
In other words, meet the demand of condenser C5 liquid towards cold-producing medium by pressure-reducing valve V1 and the cold-producing medium with final temperature TE.Unlike this, the cold-producing medium with higher temperature T I is supplied to cold expander X1, thereby cold-producing medium does not liquefy in expander X1.But the refrigeration work consumption discharging and working power still can be used for making the second heat exchanger E2 and later stage compressor C3 work.
Cold-producing medium can evaporate at least in part again in condenser E5, discharges subsequently, and converge with the Part I cold-producing medium reducing pressure in cold expander X1 by liquid line and the gas piping with valve V4 from the top of condenser E5 in the mode separating.Guide subsequently cold-producing medium through over-heat-exchanger E2 and E1, again send in main compressor C1 in suction side subsequently.
Except having improved the validity of cold expander X1, the initial pressure PA that can adopt in equipment 10 is apparently higher than equipment 100, and this has reduced required circulating energy.The method that can implement in equipment 10 has been improved efficiency on the whole significantly.The minimizing degree of the required shaft power of main compressor C1 especially can reach approximately 10% to 20% scope.
In addition, the gaseous overhead fraction of the second knockout tower S2 again can also be compressed in recycle compressor C4 to the pressure of the first knockout tower S1, in E2 and E1, after heating, sneak in the product P RO that methane content is low.Can also directly sneak in the overhead product of knockout tower S1.
Figure 3 shows that the schematic diagram of being isolated the equipment of methane according to one embodiment of the invention by the synthesis gas that contains methane, represent with Reference numeral 11 on the whole.Equipment 11, except having as many as the 4th heat exchanger E4, also has the basic module of aforementioned device 100.
Do not use the 4th heat exchanger E4 that is designed to side evaporimeter, but by part fraction guiding process pressure-reducing valve V5 at the bottom of the isolated tower that is rich in methane and contain carbon monoxide in the tower bottom side of the first knockout tower S1, and heat in the second heat exchanger E2.Subsequently fraction at the bottom of this part tower reducing pressure via pressure-reducing valve V5 and heat in the second heat exchanger E2 is sent in the second knockout tower S2 at definite entry level place, thereby heated at this.The function that thus can less cost of equipment realizes the 4th heat exchanger E4, this has saved cost.
Therefore the cooling procedure by the first heat exchanger E1 and the further cooling procedure of appropriate section is produced the medium temperature TI of cold-producing medium in the 3rd heat exchanger E3 in equipment 11.
Figure 4 shows that the schematic diagram of being isolated another equipment of methane according to one embodiment of the invention by the synthesis gas that contains methane, represent with Reference numeral 12 on the whole.Equipment 12 has the basic module of aforementioned device 11.
But in equipment 12, be not by the cold-producing medium from refrigerant circulation, but at least one tributary of the synthesis gas SYN that contains methane cooling in the first heat exchanger E1 is supplied to the 3rd heat exchanger as tower bottom reboiler work.So this its directed first through the first heat exchanger E1, then through the 3rd heat exchanger E3, then through the second heat exchanger E2.Therefore equipment 12 can be worked more effectively.
Therefore in equipment 12, substantially only produce the medium temperature TI of cold-producing medium by the cooling procedure in the first heat exchanger E1.
The favourable embodiment that another of described method do not illustrate in the drawings relates to heat exchanger E1 and/or E2.This can also be advantageously on the one hand for methane LNG, the synthesis gas SYN that contains methane and/or product stream PRO and the heat exchanger of each self-separation is set for cold-producing medium stream on the other hand.This can reduce costs.This is especially applicable to heat exchanger E1, but can be also favourable for heat exchanger E2.Shown heat exchanger E1 and/or E2 can also realize with the form of two or more construction units separately.
Although with reference between the first knockout tower S1 and the second knockout tower S2, adopt comparable pressure differential size device description the present invention, can also use it in the method and apparatus with less pressure differential.Therefore operational outfit correspondingly, contain therein the synthesis gas SYN of methane between the entrance and exit of the whole process of inlet and outlet, be defined as respectively the entrance and exit of inlet and outlet the first heat exchanger E1 at this, only bear pressure differential, especially for example, pressure drop in the scope of 1 to 3 bar, 1.5 to 2.5 bar.

Claims (13)

1. in cryogenic separation (10), isolate the method for methane (LNG) from the synthesis gas (SYN) that contains methane, described cryogenic separation comprises the knockout tower (S2) that has the refrigerant circulation of at least one expander (X1) and at least one and have condenser (E5), wherein supply separately the cold-producing medium from the compressed and cooling part of refrigerant circulation at least one expander (X1) and condenser (E5), it is characterized in that, the Part I cold-producing medium that is cooled to medium temperature (TI) from initial temperature (TA) is supplied to at least one expander (X1), and be supplied to condenser (E5) by being cooled to from initial temperature (TA) the Part II cold-producing medium that medium temperature (TI) is then further cooled to lower final temperature (TE) first equally.
2. according to the method for claim 1, wherein for Part II cold-producing medium being supplied in condenser (E5), use pressure-reducing valve (V1) that Part II cold-producing medium is decompressed to feed pressure (PC), and make thus it liquefy at least in part.
3. according to the method for claim 1 or 2, wherein use at least one first heat exchanger (E1) that the first and second part cold-producing mediums are cooled to medium temperature (TI) from initial temperature (TA), and use the second heat exchanger (E2) that Part II cold-producing medium is further cooled to final temperature (TI) from medium temperature (TI).
4. according to the method for claim 3, wherein in cryogenic separation (10) by the synthesis gas that contains methane (SYN) equally at least at the first heat exchanger and then carry out cooling in the second heat exchanger (E1, E2).
5. according to the method for claim 3 or 4, wherein use at least one other heat exchanger (E3, E4), the fluid of therein the feeding At The Height definite being discharged by least one knockout tower (S2) heats.
6. according to the method for claim 5, wherein in other heat exchanger (E3, E4), carry out further cooling at least a portion of the first and second part cold-producing mediums cooling in the first heat exchanger (E1) at least one.
7. according to the method for claim 5 or 6, wherein in other heat exchanger (E3, E4), carry out further cooling to the synthesis gas that contains methane (SYN) cooling in the first heat exchanger (E1) at least one.
8. according to the method for one of claim 3 to 7, wherein Part I cold-producing medium, to do work and/or to provide the mode of refrigeration to reduce pressure in expander (X1), is then sent into the cold junction of the second heat exchanger (E2).
9. according to the method for one of claim 3 to 8, wherein use at least two knockout tower (S1, S2), fraction at the bottom of the tower that goes out to be rich in methane and contain carbon monoxide from synthesis gas (SYN) cryogenic separation in the first knockout tower (S1), and in second knockout tower (S2) with condenser (E5), make carbon monoxide from fraction desorb at least in part at the bottom of tower, in the second heat exchanger (E2), at least a portion of fraction at the bottom of the isolated tower that is rich in methane and contain carbon monoxide in the first knockout tower (S1) is heated, and it is sent in the second knockout tower (S2) at definite entry level place.
10. according to the method for one of claim 3 to 9, wherein by first and/or Part II refrigerant compression to 50 to 100 bar, the especially pressure of 60 to 90 bar, and/or decompression to 8 to 20 bar, the especially feed pressure of 10 to 15 bar (PC), and/or be cooled to the medium temperature (TI) of-120 to-170 ℃, especially-130 to-160 ℃, and/or be cooled to the final temperature (TE) of-140 to-180 ℃, especially-150 to-170 ℃.
11. according to the method for one of claim 2 to 10, wherein uses 80% cold-producing medium as described Part I, and/or uses 20% cold-producing medium as described Part II.
12. according to the method for one of aforementioned claim, wherein use main compressor (C1) and at least two later stage compressor (C2, C3) compressed refrigerant, expander (X1) mechanically with described at least two later stage compressor (C2, one of C3) be connected, and it is driven.
13. isolate the equipment (10 of the method for methane (LNG) according to one of aforementioned claim from the synthesis gas (SYN) that contains methane for implementing, 11, 12), it is designed to cryogenic separation (10), it comprises that at least one expander (X1) and at least one have the knockout tower (S2) of condenser (E5), wherein the design of at least one expander (X1) and condenser (E5) makes to supply separately the cold-producing medium from the compressed and cooling part of refrigerant circulation to it, setting device, its design makes to be cooled to from initial temperature (TA) at least one expander (X1) supply the Part I cold-producing medium of medium temperature (TI), and be cooled to medium temperature (TI) and be then further cooled to first equally the Part II cold-producing medium of lower final temperature (TE) from initial temperature (TA) to condenser (E5) supply.
CN201310757056.7A 2012-10-18 2013-10-17 Method and equipment for separating methane from synthesis gas Pending CN103776238A (en)

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