CA2976341C - Method for recovering helium - Google Patents

Method for recovering helium Download PDF

Info

Publication number
CA2976341C
CA2976341C CA2976341A CA2976341A CA2976341C CA 2976341 C CA2976341 C CA 2976341C CA 2976341 A CA2976341 A CA 2976341A CA 2976341 A CA2976341 A CA 2976341A CA 2976341 C CA2976341 C CA 2976341C
Authority
CA
Canada
Prior art keywords
nitrogen
fraction
helium
enriched fraction
enriched
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.)
Active
Application number
CA2976341A
Other languages
French (fr)
Other versions
CA2976341A1 (en
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
Publication of CA2976341A1 publication Critical patent/CA2976341A1/en
Application granted granted Critical
Publication of CA2976341C publication Critical patent/CA2976341C/en
Active legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02Processes 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
    • F25J3/0204Processes 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
    • F25J3/0209Natural gas or substitute natural gas
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02Processes 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
    • F25J3/0228Processes 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
    • F25J3/0257Processes 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/02Processes 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
    • F25J3/0228Processes 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
    • F25J3/028Processes 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
    • F25J3/029Processes 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00Processes or apparatus using separation by rectification
    • F25J2200/02Processes or apparatus using separation by rectification in a single pressure main column system
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00Processes or apparatus using separation by rectification
    • F25J2200/40Features relating to the provision of boil-up in the bottom of a column
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00Processes or apparatus using separation by rectification
    • F25J2200/70Refluxing the column with a condensed part of the feed stream, i.e. fractionator top is stripped or self-rectified
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00Processes or apparatus using other separation and/or other processing means
    • F25J2205/02Processes or apparatus using other separation and/or other processing means using simple phase separation in a vessel or drum
    • F25J2205/04Processes 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00Processes or apparatus using other separation and/or other processing means
    • F25J2205/40Processes or apparatus using other separation and/or other processing means using hybrid system, i.e. combining cryogenic and non-cryogenic separation techniques
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00Processes or apparatus using other separation and/or other processing means
    • F25J2205/60Processes 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00Processes or apparatus using other separation and/or other processing means
    • F25J2205/60Processes 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
    • F25J2205/66Regenerating the adsorption vessel, e.g. kind of reactivation gas
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00Processes or apparatus using other separation and/or other processing means
    • F25J2205/82Processes or apparatus using other separation and/or other processing means using a reactor with combustion or catalytic reaction
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2210/00Processes characterised by the type or other details of the feed stream
    • F25J2210/40Air or oxygen enriched air, i.e. generally less than 30mol% of O2
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2215/00Processes characterised by the type or other details of the product stream
    • F25J2215/04Recovery of liquid products
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2220/00Processes or apparatus involving steps for the removal of impurities
    • F25J2220/42Separating low boiling, i.e. more volatile components from nitrogen, e.g. He, H2, Ne
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2230/00Processes or apparatus involving steps for increasing the pressure of gaseous process streams
    • F25J2230/42Processes or apparatus involving steps for increasing the pressure of gaseous process streams the fluid being nitrogen
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2240/00Processes or apparatus involving steps for expanding of process streams
    • F25J2240/02Expansion of a process fluid in a work-extracting turbine (i.e. isentropic expansion), e.g. of the feed stream
    • F25J2240/12Expansion of a process fluid in a work-extracting turbine (i.e. isentropic expansion), e.g. of the feed stream the fluid being nitrogen
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2245/00Processes or apparatus involving steps for recycling of process streams
    • F25J2245/42Processes or apparatus involving steps for recycling of process streams the recycled stream being nitrogen
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2250/00Details related to the use of reboiler-condensers
    • F25J2250/02Bath type boiler-condenser using thermo-siphon effect, e.g. with natural or forced circulation or pool boiling, i.e. core-in-kettle heat exchanger
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00Refrigeration techniques used
    • F25J2270/02Internal refrigeration with liquid vaporising loop
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00Refrigeration techniques used
    • F25J2270/04Internal refrigeration with work-producing gas expansion loop
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2290/00Other details not covered by groups F25J2200/00 - F25J2280/00
    • F25J2290/34Details about subcooling of liquids

Landscapes

  • 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

Specification Method for recovering helium The invention relates to a method for recovering a helium product fraction from a nitrogen- and helium-containing feed fraction, wherein - the nitrogen- and helium-containing feed fraction is partially condensed and separated into a first helium-enriched fraction and a first nitrogen-enriched fraction, - the first helium-enriched fraction is subjected to an adsorptive cleaning process and the helium-enriched fraction recovered therefrom represents the helium product fraction, - the first nitrogen-enriched fraction is separated into a second helium-enriched fraction and a second nitrogen-enriched fraction, and - the second helium-enriched fraction is preheated against the nitrogen- and helium-containing feed fraction to be partially condensed, condensed and admixed to the nitrogen- and helium-containing feed fraction to be partially condensed.
.. The term "helium product fraction" be comprised of highly purified helium, the concentration and contamination of which do not exceed a value of 100 vppm, preferably of 10 vppm.
The term "nitrogen- and helium-containing feed fraction" be understood as a fraction, which contains 1 to 20 mol-% helium and 80 to 99 mol-% nitrogen. Further, this feed fraction can contain 0,1 to 2 mol-% methane and traces of hydrogen, argon and/or other noble gases.
Currently, helium is obtained almost exclusively from a mixture of volatile natural gas components, which typically contains methane and nitrogen as well as traces of hydrogen, argon and other noble gases besides helium. To avoid separation by freezing of undesired decontamination during helium liquification, the concentration of this decontamination in helium cannot exceed a value of 100 vppm, preferably of 10 vppm.
The helium purification prior to the actual helium liquefaction generally consists of a combination of cryogenic ¨ based on partial condensation ¨ and adsorptive methods with regeneration through pressure and/or temperature changes. Based on the comparatively high product value, a helium yield as high as possible, preferably > 99 %, is desirable. In consequence, the helium-enriched fraction is often transferred from the liquid into the gaseous phase by pressure release and/or stripping from the liquid to the gaseous phase during the cryogenic step to remain available for further processing.

A method implication is known from US patent 5,167,125, wherein a nitrogen-enriched flow, which has elevated pressure and contains helium, is separated by using a pressure drop in a helium-containing flow of average pressure and a nitrogen-enriched flow of lower pressure.
Such separation is implemented in a rectification column, which has a reboiler and a condenser.
Figure 1 illustrates a method for recovering a helium product fraction in accordance with the present invention.
It is the object of the present invention to specify a generic method for recovering a helium product fraction, which facilitates generation of at least a partial quantity of the nitrogen-enriched flow accruing during separation at the same pressure as the helium-containing flow, to be able to subsequently supply the nitrogen-enriched flow to a work-performing expansion.
For the solution of said object, a generic method for recovering a helium product fraction is suggested, which is characterized in that - the separation of the first nitrogen-enriched fraction into a second helium-enriched fraction and a second nitrogen-enriched fraction is implemented in a separation column, to which the first nitrogen-enriched fraction is supplied as return flow, - a sub-flow of the second nitrogen-enriched fraction evaporates and the separation column is supplied as stripping gas, - at least a sub-flow of the second nitrogen-enriched fraction is evaporated against the nitrogen- and helium-containing feed fraction to be partially condensed under a pressure of less than 5 bar, - a third nitrogen-enriched fraction is removed from the separation column, - wherein the stripping gas quantity is set such that the third nitrogen-enriched fraction contains at least 30 % of the nitrogen contained in the first nitrogen-enriched fraction, and - the third nitrogen-enriched fraction serves at least partially to cool the nitrogen- and helium-containing feed fraction to be partially condensed.
Further advantageous embodiments of the method according to the invention for recovering a helium product fraction, which represent subject matters of the dependent claims are characterized in that the third nitrogen-enriched fraction is at least partially work-performing expanded (X),
2 Date Regue/Date Received 2022-06-29 the separation column is operated with a pressure of 7 to 20 bar, preferably of 10 to 15 bar, the third nitrogen-enriched fraction contains at least 50 % of the nitrogen contained in the first nitrogen-enriched fraction, at least a sub-flow of the second nitrogen-enriched fraction is evaporated against the nitrogen- and helium-containing feed fraction to be partially condensed under a pressure of less than 3 bar, and/or the adsorptive cleaning process is a (V)PSA and/or TSA process.
The method according to the invention for recovering a helium product fraction as well as further advantageous embodiments thereof are explained in further detail by means of the embodiment example represented in Figure 1.
Via line 1, a nitrogen- and helium-containing feed fraction, which originates, for example, from a separation process of natural gas, is first supplied to catalytic methane oxidation A and subsequently via line 2 to a drying unit B. The water separated in the drying unit B is removed via line 30. The feed fraction conventionally pretreated in such way, which typically has a pressure of between 10 and 40 bar, preferably between15 and 25 bar, is supplied to the heat exchanger El via line 3 and partially condensed therein against method flows yet to be explained. Via line 4, the partially condensed feed fraction is supplied to a separator D1 and separated therein into a first helium-enriched fraction 5 as well as a first nitrogen-enriched fraction 8.
The helium-enriched fraction 5 is supplied to an adsorptive cleaning process D
after preheating in the heat exchanger El. Such process is designed as (V)PSA and/or TSA
process. The helium-enriched fraction recovered therein and removed via line 6, represents the helium product fraction, the concentration of decontamination of which does not exceed a value of 100 vppm, preferably of 100 vppm. As a rule, this helium product fraction is supplied to a liquefaction process not illustrated in Figure 1.
The helium-containing residue gas removed from the adsorptive cleaning process D is supplied to a return compressor C via line 7, is compressed therein to the pressure of the feed fraction 1 to be supplied to the catalytic methane oxidation A and admixed thereto via line 32.
3 Date Regue/Date Received 2022-06-29 The above mentioned first nitrogen-enriched fraction 8 is expanded in valve a and supplied to the separation column T in its upper section as return flow. The separation column T is preferably operated at a pressure between 7 and 20 bar, in particular between 10 and 15 bar. A
separation into a second helium-enriched gas fraction 9 and a second nitrogen-enriched liquid fraction 11 is implemented therein. The second helium-enriched fraction 9 is preheated in heat exchanger El against the feed fraction 3 to be partially condensed, and supplied to the mentioned return compressor C via control valve b, as well. Additional air is supplied thereto via line 31. The oxygen contained in the air serves as oxidation means for the catalytic methane oxidation A.
A sub-flow of the second nitrogen-enriched liquid fraction 11 is evaporated in heat exchanger El and supplied to the separation column T as stripping gas 12. Such stripping gas supply causes the separation process taking place in separation column T and determines the helium content of the second helium-enriched fraction 9.
At least a sub-flow of the second nitrogen-enriched fraction 11 is evaporated in heat exchanger El against the feed fraction to be partially condensed 3 under a pressure of less than 5 bar, preferably of less than 3 bar. This method serves to set a temperature as low as possible in separator DI. In the embodiment example illustrated in Figure 1, a sub-flow of the second nitrogen-enriched fraction 11 is supplied to a circulation container D2 via control valve c. The liquid fraction removed therefrom via line 14 is supplied to heat exchanger El under the above mentioned low pressure, at least partially evaporated therein, and resupplied to the circulation container D2.
A nitrogen-enriched gas fraction 15 is removed from the top of circulation container D2, preheated in heat exchanger El against the feed fraction to be partially condensed 3, and subsequently resupplied as regeneration gas to the above mentioned drying unit B, which is an adsorptive drying process, as a rule. This loaded regeneration gas is removed from the process via line 16.
The sub-flow 13 of the second nitrogen-enriched fraction 11, which is not supplied to the circulation container D2, can be supercooled in heat exchanger El and can be generated as supercooled liquid via control valve d and line 17. By means of this configuration of the method according to the invention, an otherwise required generation or provision of liquefied nitrogen (LIN), as the case may be, can be refrained from.
4 Date Regue/Date Received 2022-06-29 Alternative or supplemental to the method implementation illustrated in Figure 1, a sub-flow of liquid fraction 14 removed from the circulation container D2 can be removed in the above described manner via control valve d and line 17.
The coldness required for the partial condensation of the feed fraction 3 can principally be provided by preheating cold, gaseous decomposition products as well as the above described evaporation of liquid fraction 14, which was removed from the circulation container D2.
Generally, the following is true: the larger the stripping gas quantity 12 evaporated in heat exchanger El, the lower can be the quantity of liquid fraction 14 removed from the circulation container D2. It must, however, be ensured that heat exchange and temperature of flow 12 are suitable for cooling and partially condensing feed fraction 3. If the content of flow 12 in the heat turnover in heat exchanger El becomes too large, the temperature in separator Dl increases undesirably.
The quantity of the stripping gas 12 supplied to separation column T is selected according to the invention to such amount that a third nitrogen-enriched fraction 20 can be removed from separation column Tin the section of its bottom, wherein such fraction contains at least 30 %, preferably at least 50 % of the nitrogen contained in the first nitrogen-enriched fraction 8.
These nitrogen contents are achieved in that a larger stripping gas quantity 12 is boiled up in the bottom of separation column T than would be required for the actual stripping process in separation column T.
Opposed to the method mentioned and described in US patent 5,167,125, a further nitrogen-enriched fraction can be recovered in separation column T under increased pressure. This further or third nitrogen-enriched fraction can be condensed to a pressure after preheating in heat exchanger El, which is above the pressure of column T by 4 to 20 bar, preferably by 5 to 15 bar. After removing the condensation heat in heat exchanger E2, the nitrogen-enriched fraction 21 is cooled in heat exchanger El and subsequently work-performing expanded in expansion device X. The expanded nitrogen-enriched fraction 22 is subsequently preheated against the feed fraction to be partially condensed 3 in heat exchanger El and admixed to the above described nitrogen-enriched fraction 15. Such work-performing expansion X, which increases thermo-dynamic efficiency of the process, is optional, facilitates or increases the quantity of the cooled liquid (UN) removed via line 17, however.
Date Regue/Date Received 2022-06-29

Claims

Patent Claims 1. A method for recovering a helium product fraction from a nitrogen-and helium-containing feed fraction, wherein - the nitrogen- and helium-containing feed fraction is partially condensed and separated into a first helium-enriched fraction and a first nitrogen-enriched fraction, the first helium-enriched fraction is subjected to an adsorptive cleaning process and the helium-enriched fraction recovered therefrom represents the helium product fraction, the first nitrogen-enriched fraction is separated into a second helium-enriched fraction and a second nitrogen-enriched fraction, and the second helium-enriched fraction is preheated against the nitrogen- and helium-containing feed fraction to be partially condensed, condensed and admixed to the nitrogen- and helium-containing feed fraction to be partially condensed, wherein the separation of the first nitrogen-enriched fraction into the second helium-enriched fraction and the second nitrogen-enriched fraction is implemented in a separation column, to which the first nitrogen-enriched fraction is supplied as return flow, - a first sub-flow of the second nitrogen-enriched fraction evaporates and the separation column is supplied as stripping gas, at least a second sub-flow of the second nitrogen-enriched fraction is evaporated against the nitrogen- and helium-containing feed fraction to be partially condensed under a pressure of less than 5 bar, - a third nitrogen-enriched fraction is removed from the separation column, wherein the stripping gas quantity is set such that the third nitrogen-enriched fraction contains at least 30 % of the nitrogen contained in the first nitrogen-enriched fraction, and the third nitrogen-enriched fraction serves at least partially to cool the nitrogen- and helium-containing feed fraction to be partially condensed.
2. The method according to claim 1, wherein the third nitrogen-enriched fraction is at least partially work-performing expanded.

Date Recue/Date Received 2022-06-29 3. The method according to claim 1 or 2, wherein the separation column is operated under a pressure of 7 to 20 bar.
4. The method according to claim 1 or 2, wherein the separation column is operated under a pressure of 10 to 15 bar.5. The method according to any one of claims 1 to 4, wherein the third nitrogen-enriched fraction contains at least 50 % of the nitrogen contained in the first nitrogen-enriched fraction.
6. The method according to any one of claims 1 to 5, wherein at least the second sub-flow of the second nitrogen-enriched fraction is evaporated against the nitrogen- and helium-containing feed fraction to be partially condensed under a pressure of less than 3 bar.
7. The method according to any one of claims 1 to 6, wherein the adsorptive cleaning process is a (V)PSA and/or TSA process.

Date Recue/Date Received 2022-06-29
CA2976341A 2015-02-10 2016-01-26 Method for recovering helium Active CA2976341C (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE102015001664.4 2015-02-10
DE102015001664.4A DE102015001664A1 (en) 2015-02-10 2015-02-10 Helium recovery process
PCT/EP2016/000131 WO2016128111A1 (en) 2015-02-10 2016-01-26 Method for recovering helium

Publications (2)

Publication Number Publication Date
CA2976341A1 CA2976341A1 (en) 2016-08-18
CA2976341C true CA2976341C (en) 2023-07-11

Family

ID=55273198

Family Applications (1)

Application Number Title Priority Date Filing Date
CA2976341A Active CA2976341C (en) 2015-02-10 2016-01-26 Method for recovering helium

Country Status (6)

Country Link
US (1) US20180023888A1 (en)
AU (1) AU2016218602B2 (en)
CA (1) CA2976341C (en)
DE (1) DE102015001664A1 (en)
RU (1) RU2689252C2 (en)
WO (1) WO2016128111A1 (en)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR3096900B1 (en) * 2019-06-06 2021-10-01 Air Liquide Helium purification process and unit

Family Cites Families (15)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3205669A (en) * 1960-08-15 1965-09-14 Phillips Petroleum Co Recovery of natural gas liquids, helium concentrate, and pure nitrogen
SU1645796A1 (en) * 1989-01-26 1991-04-30 Всесоюзный научно-исследовательский институт природных газов Process of simultaneous production of heliun ethan and heavier hydrocarbons
US5167125A (en) 1991-04-08 1992-12-01 Air Products And Chemicals, Inc. Recovery of dissolved light gases from a liquid stream
US5257505A (en) * 1991-04-09 1993-11-02 Butts Rayburn C High efficiency nitrogen rejection unit
DE4210637A1 (en) * 1992-03-31 1993-10-07 Linde Ag Process for the production of high-purity hydrogen and high-purity carbon monoxide
US5771714A (en) * 1997-08-01 1998-06-30 Praxair Technology, Inc. Cryogenic rectification system for producing higher purity helium
DE10007440A1 (en) * 2000-02-18 2001-08-23 Linde Ag Recovering a helium pure fraction from a stream containing at least methane, nitrogen and helium comprises using two-stage purifying process
DE10106484A1 (en) * 2001-02-13 2002-08-14 Linde Ag Simultaneous recovery of helium and nitrogen pure fractions from process stream containing methane, nitrogen and helium, involves partially condensing process stream, and further processing
FR2881417B1 (en) * 2005-02-01 2007-04-27 Air Liquide PROCESS FOR THE PRODUCTION OF LOW-EMITTING SYNTHESIS GAS OF CARBON DIOXIDE
DE102005010054A1 (en) * 2005-03-04 2006-09-07 Linde Ag Process for simultaneously recovering a helium and a nitrogen pure fraction
DE102008007925A1 (en) * 2008-02-07 2009-08-13 Linde Aktiengesellschaft Separating helium, comprises condensing helium-containing fraction, separating into e.g. helium-enriched gas fraction, condensing the gas fraction, evaporating liquid fraction, separating into e.g. helium-rich gas fraction and heating
DE102011010634A1 (en) * 2011-02-08 2012-08-09 Linde Aktiengesellschaft A method of separating trace components from a fraction containing at least nitrogen and helium
DE102012008446A1 (en) * 2012-04-26 2013-10-31 Linde Aktiengesellschaft Method for obtaining pure helium-fraction from helium-containing, methane- and nitrogen-rich feed fraction, involves condensing feed fraction at ten bar pressure, which is separated into helium-depleted fraction and helium-rich fraction
DE102013007208A1 (en) * 2013-04-25 2014-10-30 Linde Aktiengesellschaft Process for recovering a methane-rich liquid fraction
DE102013012656A1 (en) * 2013-07-30 2015-02-05 Linde Aktiengesellschaft A method of separating unwanted components from a helium stream

Also Published As

Publication number Publication date
WO2016128111A1 (en) 2016-08-18
DE102015001664A1 (en) 2016-08-11
RU2015124169A3 (en) 2018-10-29
RU2015124169A (en) 2017-01-10
US20180023888A1 (en) 2018-01-25
CA2976341A1 (en) 2016-08-18
RU2689252C2 (en) 2019-05-24
AU2016218602A1 (en) 2017-08-31
AU2016218602B2 (en) 2021-04-08

Similar Documents

Publication Publication Date Title
CA2893197C (en) Argon production method and apparatus
EP0593703B1 (en) Ultra-high purity nitrogen and oxygen generator and process
JPH0140271B2 (en)
TWI687633B (en) Oxygen production system and oxygen production method
JP2008013406A (en) Method for recovering ammonia, method for reutilizing ammonia, ammonia recovery system and ammonia reutilization system
US4872893A (en) Process for the production of high pressure nitrogen
JPH06207775A (en) Low-temperature air separating method for manufacturing nitrogen having no carbon monoxide
JP2007064617A (en) Method of manufacturing krypton and/or xenon by cryogenic air separation
US20140208798A1 (en) Apparatus and Integrated Process for Separating a Mixture of Carbon Dioxide and at Least One Other Gas and for Separating Air by Cryogenic Distillation
FR2975478A1 (en) Method for liquefying gas stream rich in carbon dioxide, involves heating part of liquid flow in heat exchanger, and sending recycled molecules of refrigerant to be cooled in exchanger during partial or total failure of compressor
CA2976341C (en) Method for recovering helium
US20140165648A1 (en) Purification of inert gases to remove trace impurities
JP2009299930A (en) Air separating method and device used for the same
FR2971044A1 (en) Method for separating gas containing carbon dioxide to produce carbon dioxide enriched liquid flow in agro-food industry, involves sending part of liquid flow to exchanger, where part of flow is vaporized before being sent to lower part
JP2721591B2 (en) Ultra high purity nitrogen production equipment
US20210310733A1 (en) Method for recycling argon
JP4960277B2 (en) Method for producing ultra-high purity oxygen
CN112577262A (en) High-purity oxygen production equipment
JP5005894B2 (en) Nitrogen generation method and apparatus used therefor
JP6091847B2 (en) Gas supply equipment and gas supply method using the same
US3073093A (en) Process and apparatus for purifying gases
US5787730A (en) Thermal swing helium purifier and process
JP4430351B2 (en) Fluorine compound gas separation and purification equipment
JP2006349322A (en) Method of manufacturing argon by low-temperature air separator
US20080134716A1 (en) Method for Separating Trace Components from a Nitrogen-Rich Stream

Legal Events

Date Code Title Description
EEER Examination request

Effective date: 20201203

EEER Examination request

Effective date: 20201203

EEER Examination request

Effective date: 20201203

EEER Examination request

Effective date: 20201203

EEER Examination request

Effective date: 20201203

EEER Examination request

Effective date: 20201203