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WO2016128111A1 - Method for recovering helium - Google Patents

Method for recovering helium Download PDF

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Publication number
WO2016128111A1
WO2016128111A1 PCT/EP2016/000131 EP2016000131W WO2016128111A1 WO 2016128111 A1 WO2016128111 A1 WO 2016128111A1 EP 2016000131 W EP2016000131 W EP 2016000131W WO 2016128111 A1 WO2016128111 A1 WO 2016128111A1
Authority
WO
WIPO (PCT)
Prior art keywords
nitrogen
fraction
helium
rich fraction
rich
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/EP2016/000131
Other languages
German (de)
French (fr)
Inventor
Heinz Bauer
Martin Gwinner
Andreas Bub
Christoph HERTEL
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Linde GmbH
Original Assignee
Linde GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Linde GmbH filed Critical Linde GmbH
Priority to US15/549,854 priority Critical patent/US20180023888A1/en
Priority to AU2016218602A priority patent/AU2016218602B2/en
Priority to CA2976341A priority patent/CA2976341C/en
Publication of WO2016128111A1 publication Critical patent/WO2016128111A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • F25J3/028—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 noble gases
    • F25J3/029—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 noble gases of helium
    • 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
    • F25J3/0209—Natural gas or substitute natural 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
    • F25J3/0257—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
    • 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
    • F25J2200/02—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
    • F25J2200/40—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
    • F25J2200/70—Refluxing the column with a condensed part of the feed stream, i.e. fractionator top is stripped or self-rectified
    • 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
    • F25J2205/02—Processes or apparatus using other separation and/or other processing means using simple phase separation in a vessel or drum
    • F25J2205/04—Processes or apparatus using other separation and/or other processing means using simple phase separation in a vessel or drum in the feed line, i.e. upstream of the fractionation step
    • 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
    • F25J2205/40—Processes or apparatus using other separation and/or other processing means using hybrid system, i.e. combining cryogenic and non-cryogenic separation techniques
    • 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
    • F25J2205/60—Processes or apparatus using other separation and/or other processing means using adsorption on solid adsorbents, e.g. by temperature-swing adsorption [TSA] at the hot or cold end
    • 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
    • F25J2205/60—Processes or apparatus using other separation and/or other processing means using adsorption on solid adsorbents, e.g. by temperature-swing adsorption [TSA] at the hot or cold end
    • F25J2205/66—Regenerating the adsorption vessel, e.g. kind of reactivation 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
    • F25J2205/00—Processes or apparatus using other separation and/or other processing means
    • F25J2205/82—Processes or apparatus using other separation and/or other processing means using a reactor with combustion or catalytic reaction
    • 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
    • F25J2210/40—Air or oxygen enriched air, i.e. generally less than 30mol% of O2
    • 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
    • F25J2220/00—Processes or apparatus involving steps for the removal of impurities
    • F25J2220/42—Separating low boiling, i.e. more volatile components from nitrogen, e.g. He, H2, Ne
    • 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
    • F25J2230/42—Processes or apparatus involving steps for increasing the pressure of gaseous process streams the fluid being nitrogen
    • 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
    • F25J2240/00—Processes or apparatus involving steps for expanding of process streams
    • F25J2240/02—Expansion of a process fluid in a work-extracting turbine (i.e. isentropic expansion), e.g. of the feed stream
    • F25J2240/12—Expansion of a process fluid in a work-extracting turbine (i.e. isentropic expansion), e.g. of the feed stream the fluid being nitrogen
    • 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
    • F25J2245/42—Processes or apparatus involving steps for recycling of process streams the recycled stream being nitrogen
    • 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
    • F25J2250/00—Details related to the use of reboiler-condensers
    • F25J2250/02—Bath type boiler-condenser using thermo-siphon effect, e.g. with natural or forced circulation or pool boiling, i.e. core-in-kettle heat exchanger
    • 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
    • F25J2270/02—Internal 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
    • F25J2270/04—Internal 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
    • F25J2290/00—Other details not covered by groups F25J2200/00 - F25J2280/00
    • F25J2290/34—Details about subcooling of liquids

Definitions

  • the invention relates to a method for obtaining a helium product fraction from a nitrogen and helium-containing feed fraction, wherein
  • Nitrogen and helium-containing feed fraction warmed, compressed and the partially condensed nitrogen and helium-containing
  • Feed fraction is mixed.
  • helium product fraction includes high purity helium whose
  • Concentration of impurities does not exceed a value of 100 vppm, preferably of 10 vppm.
  • nitrogen and helium-containing feed fraction is to be understood as meaning a fraction which contains 1 to 20 mol% of helium and 80 to 99 mol% of nitrogen. Furthermore, this feed fraction may contain 0.1 to 2 mol% of methane and traces of hydrogen, argon and / or other noble gases.
  • helium is commercially obtained almost exclusively from a mixture of volatile natural gas components, which typically contains, in addition to helium, methane and nitrogen as well as traces of hydrogen, argon and other noble gases. To freeze out unwanted contaminants in the
  • the concentration of these impurities in helium must not exceed a value of 100 vppm, preferably 10 vppm.
  • the actual helium liquefaction upstream helium purification usually consists of a combination of cryogenic - based on partial condensation - and adsorptive process with regeneration by pressure and / or temperature changes. Due to the comparatively high product value, the highest possible helium yield, preferably> 99%, is desirable. For this reason, the helium-rich fraction often goes through the cryogenic step
  • Nitrogen-rich stream which is at elevated pressure and containing helium, is separated by utilizing a pressure gradient into a helium-containing stream of medium pressure and a nitrogen-rich stream of low pressure. This separation takes place in a rectification column which has a reboiler and a condenser.
  • the object of the present invention is to provide a generic method for obtaining a helium product fraction which makes it possible to deliver at least a subset of the nitrogen-rich stream obtained during the separation at the same pressure as the helium-containing stream in order to produce the nitrogen atom. rich stream then, for example, to be able to perform a work-relaxation.
  • Fraction and a second nitrogen-rich fraction is carried out in a separation column to which the 1st nitrogen-rich fraction is fed as reflux,
  • Separation column is fed as stripping gas
  • At least a partial stream of the 2nd nitrogen-rich fraction is evaporated under a pressure of less than 5 bar against the partially to be condensed nitrogen and helium-containing feed fraction
  • a third nitrogen-rich fraction is withdrawn, the amount of stripping gas being adjusted so that the third nitrogen-rich fraction is at least 30% of that in the 1st nitrogen-rich fraction
  • the third nitrogen-rich fraction serves, at least in part, for the cooling of the nitrogen and helium-containing feed fraction which is to be partially condensed.
  • the third nitrogen-rich fraction is at least partially expanded work
  • the separation column is operated at a pressure of 7 to 20 bar, preferably from 10 to 15 bar
  • the third nitrogen-rich fraction at least 50th % of the nitrogen contained in the 1st nitrogen-rich fraction contains, - at least a partial stream of the 2nd nitrogen-rich fraction is evaporated under a pressure of less than 3 bar against the partially to be condensed nitrogen and helium-containing feed fraction, and / or the adsorptive cleaning process is a (V) PSA and / or TSA process.
  • a nitrogen and helium-containing feed fraction which originates for example from a natural gas decomposition process, first a catalytic methane oxidation A and then via line 2 a
  • Drying unit B supplied.
  • the separated in the drying unit B water is withdrawn via line 30.
  • Feed fraction usually a pressure between 10 and 40 bar, preferably between 15 and 25 bar, is fed via line 3 to the heat exchanger E1 and partially condensed in this against yet to be explained process streams. Via line 4, the partially condensed feed fraction becomes a
  • Separator D1 supplied and separated in this in a 1st helium-rich fraction 5 and a first nitrogen-rich fraction 8.
  • the helium-rich fraction 5 is fed after heating in the heat exchanger E1 an adsorptive purification process D. This is designed as (V) PSA and / or TSA process.
  • the helium-rich fraction obtained in it and drawn off via line 6 represents the helium product fraction, its concentration
  • Impurities do not exceed a value of 100 vppm, preferably 100 vppm.
  • this helium product fraction is fed to a liquefaction process, not shown in FIG.
  • the withdrawn from the adsorptive purification process D, helium-containing residual gas is fed via line 7 to a recompressor C, in this compressed to the pressure of the catalytic methane oxidation A feed fraction 1 and this mixed via line 32.
  • nitrogen-rich fraction 8 is expanded in the valve a and fed to the separation column T in the upper region as reflux.
  • the separation column T is preferably operated at a pressure between 7 and 20 bar, in particular between 10 and 15 bar. It is separated into a second helium-rich
  • the second helium-rich fraction 9 is in the heat exchanger E1 against the partially condensed
  • the oxygen contained in the air is used in the catalytic methane oxidation A as an oxidizing agent.
  • a partial stream of the second nitrogen-rich liquid fraction 1 1 is evaporated in the heat exchanger E1 and fed to the separation column T as stripping gas 12.
  • This stripping gas supply effects the separation process taking place in the separation column T and determines the helium content of the second helium-rich fraction 9.
  • At least one substream of the 2nd nitrogen-rich fraction 11 is evaporated under a pressure of less than 5 bar, preferably of less than 3 bar, in the heat exchanger E1 against the feed fraction 3 to be partially condensed.
  • Procedure serves to set the lowest possible temperature in the separator D1.
  • Circulating container D2 supplied. The deducted from this via line 14
  • Liquid fraction is fed under the aforementioned low pressure to the heat exchanger E1, in this at least partially evaporated and fed again to the circulation tank D2.
  • Feed fraction 3 warmed and then the above
  • Drying unit B which is usually an adsorptive
  • Drying process is, fed as a regeneration gas. Via line 16, this laden regeneration gas is withdrawn from the process.
  • the non-circulating tank D2 supplied partial stream 13 of the 2nd nitrogen-rich fraction 1 1 can be supercooled in the heat exchanger E1 and discharged via control valve d and line 17 as supercooled liquid.
  • liquefied nitrogen LIN
  • a partial flow of the liquid fraction 14 withdrawn from the circulation container D2 can be withdrawn in the manner described above via control valve d and line 17.
  • the cold required for the partial condensation of the feed fraction 3 can only by the heating of cold, gaseous decomposition products and the above-described evaporation from the circulation container D2
  • the amount of the stripping gas 12 fed to the separation column T is additionally selected so that a third nitrogen-rich fraction 20 can be withdrawn from the separation column T in the region of its sump, at least 30%, preferably at least 50% of that in FIG Nitrogen-rich fraction 8 contains nitrogen contained.
  • a third nitrogen-rich fraction 20 can be withdrawn from the separation column T in the region of its sump, at least 30%, preferably at least 50% of that in FIG Nitrogen-rich fraction 8 contains nitrogen contained.
  • Procedure can now be obtained in the separation column T, a further nitrogen-rich fraction at elevated pressure.
  • this further or third nitrogen-rich fraction can be compressed to a pressure which is 4 to 20 bar, preferably 5 to 15 bar, above the pressure of the column T.
  • the nitrogen-rich fraction 21 is cooled in the heat exchanger E1 and then expanded in the expansion device X work.
  • the expanded nitrogen-rich fraction 22 is then heated in the heat exchanger E1 against the partially to be condensed feed fraction 3 and the above-described nitrogen-rich fraction 15 admixed.
  • This work-in-progress relaxation X which increases the thermodynamic efficiency of the process, is optional, but allows or increases the amount of supercooled liquid (LIN) withdrawn via line 17.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Mechanical Engineering (AREA)
  • Thermal Sciences (AREA)
  • General Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Separation By Low-Temperature Treatments (AREA)
  • Separation Of Gases By Adsorption (AREA)

Abstract

The invention relates to a method for recovering a helium product fraction (6) from a nitrogen- and helium-containing feed fraction (3). The nitrogen- and helium-containing feed fraction (3) is partially condensed (E1) and separated into a first helium-enriched fraction (5) and a first nitrogen-enriched fraction (8), and the former is cleaned again in an adsorptive manner. According to the invention, the separation is carried out in a separation column (T) which is supplied with the first nitrogen-enriched fraction (8) as a return flow and with a sub-flow of the second nitrogen-enriched fraction as a stripping gas (12). The stripping gas quantity (12) is set such that a third nitrogen-enriched fraction (20) which contains at least 30% of the nitrogen contained in the first nitrogen-enriched fraction (8) can be recovered in the separation column (T).

Description

Beschreibung  description

Verfahren zur Heliumgewinnung Helium recovery process

Die Erfindung betrifft ein Verfahren zum Gewinnen einer Helium-Produktfraktion aus einer Stickstoff- und Helium-enthaltenden Einsatzfraktion, wobei The invention relates to a method for obtaining a helium product fraction from a nitrogen and helium-containing feed fraction, wherein

- die Stickstoff- und Helium-enthaltende Einsatzfraktion partiell kondensiert - The nitrogen and helium-containing feed fraction partially condensed

und in eine 1. Helium-reiche Fraktion und eine 1. Stickstoff-reiche  and into a 1st helium-rich fraction and a 1st nitrogen-rich

Fraktion aufgetrennt wird,  Fraction is separated,

die 1. Helium-reiche Fraktion einem adsorptiven Reinigungsprozess  the 1st helium-rich fraction an adsorptive cleaning process

unterworfen wird und die in ihm gewonnene Helium-reiche Fraktion die Helium- Produktfraktion darstellt,  and the helium-rich fraction recovered in it represents the helium product fraction,

die 1. Stickstoff-reiche Fraktion in eine 2. Helium-reiche Fraktion und eine 2. Stickstoff-reiche Fraktion aufgetrennt wird, und  separating the 1st nitrogen-rich fraction into a 2nd helium-rich fraction and a 2nd nitrogen-rich fraction, and

die 2. Helium-reiche Fraktion gegen die partiell zu kondensierende  the second helium-rich fraction against the partially condensed

Stickstoff- und Helium-enthaltende Einsatzfraktion angewärmt, verdichtet und der partiell zu kondensierenden Stickstoff- und Helium-enthaltenden  Nitrogen and helium-containing feed fraction warmed, compressed and the partially condensed nitrogen and helium-containing

Einsatzfraktion zugemischt wird.  Feed fraction is mixed.

Der Begriff "Helium-Produktfraktion" umfasse hochreines Helium, dessen The term "helium product fraction" includes high purity helium whose

Konzentration an Verunreinigungen einen Wert von 100 vppm, vorzugsweise von 10 vppm nicht überschreitet. Concentration of impurities does not exceed a value of 100 vppm, preferably of 10 vppm.

Unter dem Begriff "Stickstoff- und Helium-enthaltende Einsatzfraktion" sei eine Fraktion zu verstehen, die 1 bis 20 mol-% Helium und 80 bis 99 mol-% Stickstoff enthält. Ferner kann diese Einsatzfraktion 0,1 bis 2 mol-% Methan und Spuren von Wasserstoff, Argon und/oder anderen Edelgase enthalten. The term "nitrogen and helium-containing feed fraction" is to be understood as meaning a fraction which contains 1 to 20 mol% of helium and 80 to 99 mol% of nitrogen. Furthermore, this feed fraction may contain 0.1 to 2 mol% of methane and traces of hydrogen, argon and / or other noble gases.

Gegenwärtig wird Helium kommerziell fast ausschließlich aus einem Gemisch leichtflüchtiger Erdgaskomponenten gewonnen, das typischerweise außer Helium noch Methan und Stickstoff sowie in Spuren Wasserstoff, Argon und andere Edelgase enthält. Um ein Ausfrieren von unerwünschten Verunreinigungen bei der At present, helium is commercially obtained almost exclusively from a mixture of volatile natural gas components, which typically contains, in addition to helium, methane and nitrogen as well as traces of hydrogen, argon and other noble gases. To freeze out unwanted contaminants in the

Heliumverflüssigung zu vermeiden, darf die Konzentration dieser Verunreinigungen in Helium einen Wert von 100 vppm, vorzugsweise von 10 vppm nicht überschreiten. Die der eigentlichen Helium-Verflüssigung vorgeschaltete Heliumreinigung besteht üblicherweise aus einer Kombination von kryogenen - basierend auf partieller Kondensation - und adsorptiven Verfahren mit Regenerierung durch Druck- und/oder Temperaturwechsel. Aufgrund des vergleichsweise hohen Produktwertes ist eine möglichst hohe Heliumausbeute, vorzugsweise > 99 % erstrebenswert. Aus diesem Grund wird die Helium-reiche Fraktion beim kryogenen Schritt oft durch To avoid helium liquefaction, the concentration of these impurities in helium must not exceed a value of 100 vppm, preferably 10 vppm. The actual helium liquefaction upstream helium purification usually consists of a combination of cryogenic - based on partial condensation - and adsorptive process with regeneration by pressure and / or temperature changes. Due to the comparatively high product value, the highest possible helium yield, preferably> 99%, is desirable. For this reason, the helium-rich fraction often goes through the cryogenic step

Druckentlastung und/oder Strippen aus der flüssigen in die gasförmige Phase übergeführt, um für die weitere Verarbeitung verfügbar zu bleiben. Aus dem US-Patent 5,167,125 ist eine Verfahrensführung bekannt, bei der ein Pressure relief and / or stripping from the liquid to the gaseous phase transferred to remain available for further processing. From US Patent 5,167,125 a methodology is known in which a

Stickstoff-reicher Strom, der bei erhöhtem Druck vorliegt und Helium enthält, unter Ausnutzung eines Druckgefälles in einen Helium-haltigen Strom mittleren Druckes und einen Stickstoff-reichen Strom niedrigen Druckes aufgetrennt wird. Diese Auftrennung erfolgt in einer Rektifikationskolonne, die einen Aufkocher und einen Kondensator aufweist.  Nitrogen-rich stream, which is at elevated pressure and containing helium, is separated by utilizing a pressure gradient into a helium-containing stream of medium pressure and a nitrogen-rich stream of low pressure. This separation takes place in a rectification column which has a reboiler and a condenser.

Aufgabe der vorliegenden Erfindung ist es, ein gattungsgemäßes Verfahren zum Gewinnen einer Helium-Produktfraktion anzugeben, das es ermöglicht, zumindest eine Teilmenge des bei der Auftrennung anfallenden Stickstoff-reichen Stroms bei dem gleichen Druck wie den Helium-haltigen Strom abzugeben, um den Stickstoff-reichen Strom anschließend bspw. einer arbeitsleistenden Entspannung zuführen zu können. The object of the present invention is to provide a generic method for obtaining a helium product fraction which makes it possible to deliver at least a subset of the nitrogen-rich stream obtained during the separation at the same pressure as the helium-containing stream in order to produce the nitrogen atom. rich stream then, for example, to be able to perform a work-relaxation.

Zur Lösung dieser Aufgabe wird ein gattungsgemäßes Verfahren zum Gewinnen einer Helium-Produktfraktion vorgeschlagen, das dadurch gekennzeichnet ist, dass To solve this problem, a generic method for obtaining a helium product fraction is proposed, which is characterized in that

- die Auftrennung der 1. Stickstoff-reichen Fraktion in eine 2. Helium-reiche - The separation of the first nitrogen-rich fraction in a second helium-rich

Fraktion und eine 2. Stickstoff-reiche Fraktion in einer Trennkolonne erfolgt, der die 1. Stickstoff-reiche Fraktion als Rücklauf zugeführt wird,  Fraction and a second nitrogen-rich fraction is carried out in a separation column to which the 1st nitrogen-rich fraction is fed as reflux,

ein Teilstrom der 2. Stickstoff-reichen Fraktion verdampft und der  a partial stream of the 2nd nitrogen-rich fraction evaporates and the

Trennkolonne als Strippgas zugeführt wird,  Separation column is fed as stripping gas,

- wenigstens ein Teilstrom der 2. Stickstoff-reichen Fraktion unter einem Druck von weniger als 5 bar gegen die partiell zu kondensierende Stickstoff- und Helium-enthaltende Einsatzfraktion verdampft wird, - At least a partial stream of the 2nd nitrogen-rich fraction is evaporated under a pressure of less than 5 bar against the partially to be condensed nitrogen and helium-containing feed fraction,

aus der Trennkolonne eine 3. Stickstoff-reiche Fraktion abgezogen wird, wobei die Strippgasmenge so eingestellt wird, dass die 3. Stickstoff-reiche Fraktion wenigstens 30 % des in der 1. Stickstoff-reichen Fraktion from the separation column a third nitrogen-rich fraction is withdrawn, the amount of stripping gas being adjusted so that the third nitrogen-rich fraction is at least 30% of that in the 1st nitrogen-rich fraction

enthaltenen Stickstoffs enthält, und  containing nitrogen, and

die 3. Stickstoff-reiche Fraktion zumindest teilweise der Abkühlung der partiell zu kondensierenden Stickstoff- und Helium-enthaltenden Einsatzfraktion dient.  the third nitrogen-rich fraction serves, at least in part, for the cooling of the nitrogen and helium-containing feed fraction which is to be partially condensed.

Weitere vorteilhafte Ausgestaltungen des erfindungsgemäßen Verfahrens zum Further advantageous embodiments of the method according to the invention for

Gewinnen einer Helium-Produktfraktion, die Gegenstände der abhängigen Obtaining a helium product fraction, the objects of the dependent

Patentansprüche darstellen, sind dadurch gekennzeichnet, dass die 3. Stickstoff-reiche Fraktion zumindest teilweise arbeitsleistend entspannt wird, die Trennkolonne bei einem Druck von 7 bis 20 bar, vorzugsweise von 10 bis 15 bar betrieben wird, die 3. Stickstoff-reiche Fraktion wenigstens 50 % des in der 1. Stickstoff-reichen Fraktion enthaltenen Stickstoffs enthält, - wenigstens ein Teilstrom der 2. Stickstoff-reichen Fraktion unter einem Druck von weniger als 3 bar gegen die partiell zu kondensierende Stickstoff- und Helium-enthaltende Einsatzfraktion verdampft wird, und/oder der adsorptive Reinigungsprozess ein (V)PSA- und/oder TSA-Prozess ist. Represent represent claims are characterized in that the third nitrogen-rich fraction is at least partially expanded work, the separation column is operated at a pressure of 7 to 20 bar, preferably from 10 to 15 bar, the third nitrogen-rich fraction at least 50th % of the nitrogen contained in the 1st nitrogen-rich fraction contains, - at least a partial stream of the 2nd nitrogen-rich fraction is evaporated under a pressure of less than 3 bar against the partially to be condensed nitrogen and helium-containing feed fraction, and / or the adsorptive cleaning process is a (V) PSA and / or TSA process.

Das erfindungsgemäße Verfahren zum Gewinnen einer Helium-Produktfraktion sowie weitere vorteilhafte Ausgestaltungen desselben seien anhand des in der Figur 1 dargestellten Ausführungsbeispieles näher erläutert. Über Leitung 1 wird eine Stickstoff- und Helium-enthaltende Einsatzfraktion, die beispielsweise aus einem Erdgas-Zerlegungsprozess stammt, zunächst einer katalytischen Methanoxidation A und anschließend über Leitung 2 einer The inventive method for obtaining a helium product fraction and further advantageous embodiments thereof are explained in more detail with reference to the embodiment shown in the figure 1. Via line 1 is a nitrogen and helium-containing feed fraction, which originates for example from a natural gas decomposition process, first a catalytic methane oxidation A and then via line 2 a

Trocknungseinheit B zugeführt. Das in der Trocknungseinheit B abgetrennte Wasser wird über Leitung 30 abgezogen. Die derart konventionell vorbehandelte Drying unit B supplied. The separated in the drying unit B water is withdrawn via line 30. The thus conventionally pretreated

Einsatzfraktion, die üblicherweise einen Druck zwischen 10 und 40 bar, vorzugsweise zwischen 15 und 25 bar aufweist, wird über Leitung 3 dem Wärmetauscher E1 zugeführt und in diesem gegen noch zu erläuternde Verfahrensströme partiell kondensiert. Über Leitung 4 wird die partiell kondensierte Einsatzfraktion einem Feed fraction, usually a pressure between 10 and 40 bar, preferably between 15 and 25 bar, is fed via line 3 to the heat exchanger E1 and partially condensed in this against yet to be explained process streams. Via line 4, the partially condensed feed fraction becomes a

Abscheider D1 zugeführt und in diesem in eine 1. Helium-reiche Fraktion 5 sowie eine 1. Stickstoff-reiche Fraktion 8 aufgetrennt. Separator D1 supplied and separated in this in a 1st helium-rich fraction 5 and a first nitrogen-rich fraction 8.

Die Helium-reiche Fraktion 5 wird nach Anwärmung im Wärmetauscher E1 einem adsorptiven Reinigungsprozess D zugeführt. Dieser ist als (V)PSA- und/oder TSA- Prozess ausgelegt. Die in ihm gewonnene und über Leitung 6 abgezogene Helium- reiche Fraktion stellt die Helium-Produktfraktion dar, deren Konzentration an The helium-rich fraction 5 is fed after heating in the heat exchanger E1 an adsorptive purification process D. This is designed as (V) PSA and / or TSA process. The helium-rich fraction obtained in it and drawn off via line 6 represents the helium product fraction, its concentration

Verunreinigungen einen Wert von 100 vppm, vorzugsweise von 100 vppm nicht überschreitet. Im Regelfall wird diese Helium-Produktfraktion einem in der Figur 1 nicht dargestellten Verflüssigungsprozess zugeführt. Das aus dem adsorptiven Reinigungsprozess D abgezogene, Helium-enthaltende Restgas wird über Leitung 7 einem Rückverdichter C zugeführt, in diesem auf den Druck der der katalytischen Methanoxidation A zuzuführenden Einsatzfraktion 1 verdichtet und dieser über Leitung 32 zugemischt. Die vorgenannte 1. Stickstoff-reiche Fraktion 8 wird im Ventil a entspannt und der Trennkolonne T in deren oberen Bereich als Rücklauf zugeführt. Die Trennkolonne T wird vorzugsweise bei einem Druck zwischen 7 und 20 bar, insbesondere zwischen 10 und 15 bar betrieben. In ihr erfolgt eine Auftrennung in eine 2. Helium-reiche Impurities do not exceed a value of 100 vppm, preferably 100 vppm. As a rule, this helium product fraction is fed to a liquefaction process, not shown in FIG. The withdrawn from the adsorptive purification process D, helium-containing residual gas is fed via line 7 to a recompressor C, in this compressed to the pressure of the catalytic methane oxidation A feed fraction 1 and this mixed via line 32. The aforementioned 1. nitrogen-rich fraction 8 is expanded in the valve a and fed to the separation column T in the upper region as reflux. The separation column T is preferably operated at a pressure between 7 and 20 bar, in particular between 10 and 15 bar. It is separated into a second helium-rich

Gasfraktion 9 und eine 2. Stickstoff-reiche Flüssigfraktion 1 1. Die 2. Helium-reiche Fraktion 9 wird im Wärmetauscher E1 gegen die partiell zu kondensierende Gas fraction 9 and a second nitrogen-rich liquid fraction 1 1. The second helium-rich fraction 9 is in the heat exchanger E1 against the partially condensed

Einsatzfraktion 3 angewärmt und über das Regelventil b ebenfalls dem erwähnten Rückverdichter C zugeführt. Diesem wird über Leitung 31 zusätzlich Luft zugeführt. Der in der Luft enthaltene Sauerstoff dient in der katalytischen Methanoxidation A als Oxidationsmittel.  Feed fraction 3 warmed and fed via the control valve b also mentioned the reflux compressor C. This is additionally supplied via line 31 air. The oxygen contained in the air is used in the catalytic methane oxidation A as an oxidizing agent.

Ein Teilstrom der 2. Stickstoff-reichen Flüssigfraktion 1 1 wird im Wärmetauscher E1 verdampft und der Trennkolonne T als Strippgas 12 zugeführt. Diese Strippgas- Zuführung bewirkt den in der Trennkolonne T ablaufenden Trennprozess und bestimmt den Helium-Anteil der 2. Helium-reichen Fraktion 9. Wenigstens ein Teilstrom der 2. Stickstoff-reichen Fraktion 1 1 wird unter einem Druck von weniger als 5 bar, vorzugsweise von weniger als 3 bar, im Wärmetauscher E1 gegen die partiell zu kondensierende Einsatzfraktion 3 verdampft. Diese A partial stream of the second nitrogen-rich liquid fraction 1 1 is evaporated in the heat exchanger E1 and fed to the separation column T as stripping gas 12. This stripping gas supply effects the separation process taking place in the separation column T and determines the helium content of the second helium-rich fraction 9. At least one substream of the 2nd nitrogen-rich fraction 11 is evaporated under a pressure of less than 5 bar, preferably of less than 3 bar, in the heat exchanger E1 against the feed fraction 3 to be partially condensed. These

Verfahrensweise dient dazu, eine möglichst niedrige Temperatur im Abscheider D1 einzustellen. Bei dem in der Figur 1 dargestellten Ausführungsbeispiel wird ein Teilstrom der 2. Stickstoff-reichen Fraktion 1 1 über das Regelventil c einem Procedure serves to set the lowest possible temperature in the separator D1. In the embodiment shown in Figure 1, a partial stream of the second nitrogen-rich fraction 1 1 via the control valve c a

Umlaufbehälter D2 zugeführt. Die aus diesem über Leitung 14 abgezogene Circulating container D2 supplied. The deducted from this via line 14

Flüssigfraktion wird unter dem vorgenannten niedrigen Druck dem Wärmetauscher E1 zugeführt, in diesem zumindest teilweise verdampft und erneut dem Umlaufbehälter D2 zugeführt. Liquid fraction is fed under the aforementioned low pressure to the heat exchanger E1, in this at least partially evaporated and fed again to the circulation tank D2.

Aus dem Kopf des Umlaufbehälters D2 wird eine Stickstoff-reiche Gasfraktion 15 abgezogen, im Wärmetauscher E1 gegen die partiell zu kondensierende From the top of the circulation tank D2 a nitrogen-rich gas fraction 15 is withdrawn, in the heat exchanger E1 against the partially condensed

Einsatzfraktion 3 angewärmt und anschließend der vorbeschriebenen Feed fraction 3 warmed and then the above

Trocknungseinheit B, bei der es sich im Regelfall um einen adsorptiven Drying unit B, which is usually an adsorptive

Trocknungsprozess handelt, als Regeneriergas zugeführt. Über Leitung 16 wird dieses beladene Regeneriergas aus dem Prozess abgezogen.  Drying process is, fed as a regeneration gas. Via line 16, this laden regeneration gas is withdrawn from the process.

Der nicht dem Umlaufbehälter D2 zugeführte Teilstrom 13 der 2. Stickstoff-reichen Fraktion 1 1 kann im Wärmetauscher E1 unterkühlt und über Regelventil d und Leitung 17 als unterkühlte Flüssigkeit abgegeben werden. Mittels dieser Ausgestaltung des erfindungsgemäßen Verfahrens kann auf eine gegebenenfalls erforderliche The non-circulating tank D2 supplied partial stream 13 of the 2nd nitrogen-rich fraction 1 1 can be supercooled in the heat exchanger E1 and discharged via control valve d and line 17 as supercooled liquid. By means of this embodiment of the method according to the invention, an optionally required

anderweitige Erzeugung oder Bereitstellung von verflüssigtem Stickstoff (LIN) verzichtet werden. other production or supply of liquefied nitrogen (LIN) are dispensed with.

Alternativ oder ergänzend zu der in der Figur 1 dargestellten Verfahrensführung kann ein Teilstrom der aus dem Umlaufbehälter D2 abgezogenen Flüssigfraktion 14 in vorbeschriebener Weise über Regelventil d und Leitung 17 abgezogen werden. Im Prinzip kann die für die partielle Kondensation der Einsatzfraktion 3 erforderliche Kälte ausschließlich durch die Anwärmung kalter, gasförmiger Zerlegungsprodukte sowie die vorbeschriebene Verdampfung der aus dem Umlaufbehälter D2 As an alternative or in addition to the process control shown in FIG. 1, a partial flow of the liquid fraction 14 withdrawn from the circulation container D2 can be withdrawn in the manner described above via control valve d and line 17. In principle, the cold required for the partial condensation of the feed fraction 3 can only by the heating of cold, gaseous decomposition products and the above-described evaporation from the circulation container D2

abgezogenen Flüssigfraktion 14 bereitgestellt werden. Grundsätzlich gilt: je größer die im Wärmetauscher E1 verdampfte Strippgasmenge 12 ist, umso geringer kann die aus dem Umlaufbehälter D2 entnommene Menge der Flüssigfraktion 14 sein. Allerdings ist darauf zu achten, dass Wärmeumsatz und Temperatur des Stroms 12 zur Abkühlung und Teilkondensation der Einsatzfraktion 3 geeignet sind. Wird der Anteil des Stroms 12 am Wärmeumsatz im Wärmetauscher E1 zu groß, steigt die Temperatur im withdrawn liquid fraction 14 are provided. In principle, the larger the stripping gas quantity 12 vaporized in the heat exchanger E1, the lower the amount of liquid fraction 14 taken from the circulation container D2 can be. However, that is make sure that heat conversion and temperature of the stream 12 for cooling and partial condensation of the feed fraction 3 are suitable. If the proportion of the current 12 in the heat transfer in the heat exchanger E1 too large, the temperature rises in the

Abscheider D1 unerwünscht an. Separator D1 undesirable.

Erfindungsgemäß wird zusätzlich die Menge des der Trennkolonne T zugeführten Strippgases 12 so groß gewählt, dass der Trennkolonne T im Bereich ihres Sumpfes eine 3. Stickstoff-reiche Fraktion 20 abgezogen werden kann, wobei diese wenigstens 30 %, vorzugsweise wenigstens 50 % des in der 1. Stickstoff-reichen Fraktion 8 enthaltenen Stickstoffs enthält. Diese Stickstoff-Anteile werden dadurch erreicht, dass im Sumpf der Trennkolonne T eine größere Strippgasmenge 12 aufgekocht wird, als sie für den eigentlichen Stripprozess in der Trennkolonne T erforderlich wäre. According to the invention, the amount of the stripping gas 12 fed to the separation column T is additionally selected so that a third nitrogen-rich fraction 20 can be withdrawn from the separation column T in the region of its sump, at least 30%, preferably at least 50% of that in FIG Nitrogen-rich fraction 8 contains nitrogen contained. These proportions of nitrogen are achieved in that a larger Strippgasmenge 12 is boiled in the bottom of the separation column T, as they would be required for the actual stripping process in the separation column T.

Im Gegensatz zu der erwähnten, in dem US-Patent 5,167, 125 beschriebenen In contrast to that mentioned, described in U.S. Patent 5,167,125

Verfahrensweise kann nunmehr in der Trennkolonne T eine weitere Stickstoff-reiche Fraktion bei erhöhtem Druck gewonnen werden. Diese weitere bzw. 3. Stickstoff-reiche Fraktion kann nach Anwärmung im Wärmetauscher E1 auf einen Druck verdichtet werden, der um 4 bis 20 bar, vorzugsweise um 5 bis 15 bar über dem Druck der Kolonne T liegt. Nach Abführung der Verdichtungswärme im Wärmetauscher E2 wird die Stickstoff-reiche Fraktion 21 im Wärmetauscher E1 abgekühlt und anschließend in der Expansionsvorrichtung X arbeitsleistend entspannt. Die entspannte Stickstoffreiche Fraktion 22 wird anschließend im Wärmetauscher E1 gegen die partiell zu kondensierende Einsatzfraktion 3 angewärmt und der vorbeschriebenen Stickstoffreichen Fraktion 15 zugemischt. Diese arbeitsleistende Entspannung X, die die thermodynamische Effizienz des Prozesses steigert, ist optional, ermöglicht bzw. erhöht jedoch die Menge der über Leitung 17 abgezogenen unterkühlten Flüssigkeit (LIN). Procedure can now be obtained in the separation column T, a further nitrogen-rich fraction at elevated pressure. After further heating in the heat exchanger E1, this further or third nitrogen-rich fraction can be compressed to a pressure which is 4 to 20 bar, preferably 5 to 15 bar, above the pressure of the column T. After removal of the heat of compression in the heat exchanger E2, the nitrogen-rich fraction 21 is cooled in the heat exchanger E1 and then expanded in the expansion device X work. The expanded nitrogen-rich fraction 22 is then heated in the heat exchanger E1 against the partially to be condensed feed fraction 3 and the above-described nitrogen-rich fraction 15 admixed. This work-in-progress relaxation X, which increases the thermodynamic efficiency of the process, is optional, but allows or increases the amount of supercooled liquid (LIN) withdrawn via line 17.

Claims

Patentansprüche claims 1. Verfahren zum Gewinnen einer Helium-Produktfraktion (6) aus einer Stickstoff- und Helium-enthaltenden Einsatzfraktion (3), wobei A process for recovering a helium product fraction (6) from a nitrogen and helium-containing feed fraction (3), wherein - die Stickstoff- und Helium-enthaltende Einsatzfraktion (3) partiell kondensiert (E1) und in eine 1. Helium-reiche Fraktion (5) und eine 1. Stickstoff-reiche Fraktion (8) aufgetrennt wird,  - the nitrogen and helium-containing feed fraction (3) is partially condensed (E1) and separated into a 1st helium-rich fraction (5) and a 1st nitrogen-rich fraction (8), - die 1. Helium-reiche Fraktion (5) einem adsorptiven Reinigungsprozess (D) unterworfen wird und die in ihm gewonnene Helium-reiche Fraktion die Helium- Produktfraktion (6) darstellt,  - the first helium-rich fraction (5) is subjected to an adsorptive purification process (D) and the helium-rich fraction obtained in it represents the helium product fraction (6), - die 1. Stickstoff-reiche Fraktion (8) in eine 2. Helium-reiche Fraktion (9) und eine 2. Stickstoff-reiche Fraktion (11) aufgetrennt wird, und  the first nitrogen-rich fraction (8) is separated into a second helium-rich fraction (9) and a second nitrogen-rich fraction (11), and - die 2. Helium-reiche Fraktion (9) gegen die partiell zu kondensierende  - the second helium-rich fraction (9) against the partially condensed Stickstoff- und Helium-enthaltende Einsatzfraktion (3) angewärmt (E1), verdichtet (C) und der partiell zu kondensierenden Stickstoff- und Helium- enthaltenden Einsatzfraktion zugemischt wird,  Nitrogen and helium-containing feed fraction (3) warmed (E1), compressed (C) and mixed with the nitrogen and helium-containing feed fraction to be partially condensed, dadurch gekennzeichnet, dass  characterized in that - die Auftrennung der 1. Stickstoff-reichen Fraktion (8) in eine 2. Helium-reiche Fraktion (9) und eine 2. Stickstoff-reiche Fraktion (11) in einer Trennkolonne (T) erfolgt, der die 1. Stickstoff-reiche Fraktion (8) als Rücklauf zugeführt wird, - The separation of the first nitrogen-rich fraction (8) in a second helium-rich fraction (9) and a second nitrogen-rich fraction (11) in a separation column (T), which is the 1st nitrogen-rich Fraction (8) is fed as reflux, - ein Teilstrom der 2. Stickstoff-reichen Fraktion verdampft (E1) und der - A partial stream of the 2nd nitrogen-rich fraction evaporates (E1) and the Trennkolonne (T) als Strippgas zugeführt wird (12),  Separation column (T) is supplied as stripping gas (12), - wenigstens ein Teilstrom (11) der 2. Stickstoff-reichen Fraktion unter einem Druck von weniger als 5 bar gegen die partiell zu kondensierende Stickstoff- und Helium-enthaltende Einsatzfraktion (3) verdampft wird (E1),  - At least a partial stream (11) of the second nitrogen-rich fraction under a pressure of less than 5 bar is evaporated against the partially to be condensed nitrogen and helium-containing feed fraction (3) (E1), - aus der Trennkolonne (T) eine 3. Stickstoff-reiche Fraktion (20) abgezogen wird,  - a third nitrogen-rich fraction (20) is withdrawn from the separation column (T), - wobei die Strippgasmenge (12) so eingestellt wird, dass die 3. Stickstoff-reiche Fraktion (20) wenigstens 30 % des in der 1. Stickstoff-reichen Fraktion (8) enthaltenen Stickstoffs enthält, und  wherein the amount of stripping gas (12) is adjusted so that the third nitrogen-rich fraction (20) contains at least 30% of the nitrogen contained in the 1st nitrogen-rich fraction (8), and - die 3. Stickstoff-reiche Fraktion (20) zumindest teilweise der Abkühlung (E1) der partiell zu kondensierenden Stickstoff- und Helium-enthaltenden Einsatzfraktion (3) dient. - The third nitrogen-rich fraction (20) at least partially the cooling (E1) of the partially condensing nitrogen and helium-containing feed fraction (3). 2. Verfahren nach Anspruch 1 , dadurch gekennzeichnet, dass die 3. Stickstoff-reiche Fraktion (20) zumindest teilweise arbeitsleistend entspannt wird (X). 2. The method according to claim 1, characterized in that the third nitrogen-rich fraction (20) is at least partially decompressed work (X). 3. Verfahren nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass die 3. The method according to claim 1 or 2, characterized in that the Trennkolonne (T) bei einem Druck von 7 bis 20 bar, vorzugsweise von 10 bis 15 bar betrieben wird.  Separation column (T) is operated at a pressure of 7 to 20 bar, preferably from 10 to 15 bar. 4. Verfahren nach einem der Ansprüche 1 bis 3, dadurch gekennzeichnet, dass die 3. 4. The method according to any one of claims 1 to 3, characterized in that the 3. Stickstoff-reiche Fraktion (20) wenigstens 50 % des in der 1. Stickstoff-reichen Fraktion (8) enthaltenen Stickstoffs enthält.  Nitrogen-rich fraction (20) contains at least 50% of the nitrogen contained in the 1st nitrogen-rich fraction (8). 5. Verfahren nach einem der Ansprüche 1 bis 4, dadurch gekennzeichnet, dass 5. The method according to any one of claims 1 to 4, characterized in that wenigstens ein Teilstrom (1 1) der 2. Stickstoff-reichen Fraktion unter einem Druck von weniger als 3 bar gegen die partiell zu kondensierende Stickstoff- und Helium- enthaltende Einsatzfraktion (3) verdampft wird (E1 ).  at least a partial stream (1 1) of the second nitrogen-rich fraction is vaporized under a pressure of less than 3 bar against the nitrogen and helium-containing feed fraction (3) to be partially condensed (E1). 6. Verfahren nach einem der Ansprüche 1 bis 5, dadurch gekennzeichnet, dass der adsorptive Reinigungsprozess (D) ein (V)PSA- und/oder TSA-Prozess ist. 6. The method according to any one of claims 1 to 5, characterized in that the adsorptive cleaning process (D) is a (V) PSA and / or TSA process.
PCT/EP2016/000131 2015-02-10 2016-01-26 Method for recovering helium Ceased WO2016128111A1 (en)

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US15/549,854 US20180023888A1 (en) 2015-02-10 2016-01-26 Method for recovering helium
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