WO2013126060A1 - Récupération de 3he à partir d'hélium naturel par distillation - Google Patents

Récupération de 3he à partir d'hélium naturel par distillation Download PDF

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Publication number
WO2013126060A1
WO2013126060A1 PCT/US2012/026293 US2012026293W WO2013126060A1 WO 2013126060 A1 WO2013126060 A1 WO 2013126060A1 US 2012026293 W US2012026293 W US 2012026293W WO 2013126060 A1 WO2013126060 A1 WO 2013126060A1
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WO
WIPO (PCT)
Prior art keywords
stream
helium
distillation column
overhead
conduit
Prior art date
Application number
PCT/US2012/026293
Other languages
English (en)
Inventor
Jianguo Xu
David Ross GRAHAM
Vipul S. PAREKH
Original Assignee
Air Products And Chemicals, Inc.
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Filing date
Publication date
Application filed by Air Products And Chemicals, Inc. filed Critical Air Products And Chemicals, Inc.
Priority to PCT/US2012/026293 priority Critical patent/WO2013126060A1/fr
Publication of WO2013126060A1 publication Critical patent/WO2013126060A1/fr

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D59/00—Separation of different isotopes of the same chemical element
    • B01D59/02—Separation by phase transition
    • B01D59/04—Separation by phase transition by distillation
    • 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
    • F25J3/08—Separating gaseous impurities from gases or gaseous mixtures or from liquefied gases or liquefied gaseous mixtures
    • 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
    • F25J2200/50—Processes or apparatus using separation by rectification using multiple (re-)boiler-condensers at different heights of the column
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2200/00—Processes or apparatus using separation by rectification
    • F25J2200/76—Refluxing the column with condensed overhead gas being cycled in a quasi-closed loop refrigeration cycle
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • 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
    • F25J2215/00—Processes characterised by the type or other details of the product stream
    • F25J2215/30—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
    • F25J2220/00—Processes or apparatus involving steps for the removal of impurities
    • F25J2220/90—Separating isotopes of a component, e.g. H2, 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
    • 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
    • F25J2270/12—External refrigeration with liquid vaporising loop
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/30—Quasi-closed internal or closed external helium refrigeration cycle

Definitions

  • He-3 helium-3
  • He-3 and helium-4 are naturally-occurring isotopes of helium. He-3 is currently used in a variety of applications, including neutron detection instruments, cryogenics, medical imaging, and nuclear fusion research.
  • the He-3 concentration in naturally-occurring helium (hereinafter, “helium”) is very small - typically on the order of 0.1-1.Oppm by volume, with the remainder comprising He-4.
  • the disclosed embodiments satisfy the need in the art by providing a distillation process that enables the more efficient recovery of He-3 from helium, and enables the withdrawal of a He-3-enriched overhead stream within a much shorter time than the systems of the prior art.
  • a method for recovering He-3 from helium comprising:
  • Aspect 2 The method of any of Aspects 1 and 3 through 14, wherein step (b) comprises withdrawing and recovering an overhead stream comprising He-3-enriched helium from the top section, wherein the first diameter is at least four times larger than the second diameter.
  • Aspect 3 The method of any of Aspects 1 , 2, and 4 through 14, wherein step (d) comprises condensing at least a first portion of a vapor stream in the distillation column by heat exchange with a first stream comprising helium or He-3 depleted helium as the first stream passes through an intermediate condenser located at a third location within the main section of the distillation column at which a concentration of He-3 within the distillation column is no more than 99.0%.
  • Aspect 4 The method of any of Aspects 1 through 3 and 5 through 14, further comprising the step of:
  • Aspect 5 The method of any of Aspects 1 through 4 and 6 through 14, further comprising the step of:
  • Aspect 6 The method of any of Aspects 1 through 5 and 7 through 14, further comprising the steps of:
  • Aspect 7 The method of any of Aspects 1 through 6 and 8 through 14, further comprising the step of: (i) reboiling a portion of a liquid stream in the distillation column by heat exchange with a second helium stream.
  • Aspect 8 The method of any of Aspects 1 through 7 and 9 through 14, further comprising the steps of:
  • step (k) returning a first portion of the overhead stream condensed in step (j) to the top section of the distillation column as reflux;
  • step (I) storing a second portion of the overhead stream condensed in step (j) in a product storage vessel.
  • Aspect 9 The method of any of Aspects 8 and 10 through 14, further comprising the steps of:
  • Aspect 10 The method of any of Aspects 9 and 1 1 through 14, further comprising the step of:
  • step (o) prior to performing step (m), increasing a pressure of the overhead vapor stream
  • step (p) increasing a second pressure of the first combined stream before performing step (n).
  • Aspect 1 1 The method of any of Aspects 9, 10, and 12 through 14, further comprising the step of:
  • step (q) after performing step (n) on the at least a first portion of the combined stream, dividing the at least a first portion of the combined stream into the first stream and the overhead vaporizing stream, wherein the first stream comprises a major fraction of the first portion of the combined stream and the overhead vaporizing stream comprises a minor fraction of the first portion of the combined stream.
  • Aspect 12 The method of any of Aspects 1 1 , 13, and 14, further comprising the steps of:
  • Aspect 13 The method of any of Aspects 9 through 12 and 14, further comprising the step of:
  • Aspect 14 The method of any of Aspects 9 through 13, further comprising the step of:
  • a method for recovering He-3 from helium comprising:
  • step (g) after performing step (f) on the first helium stream, condensing at least a first portion of a vapor stream in the distillation column by heat exchange with the first helium stream as the first helium stream passes through an intermediate condenser located at a third location that is above the first location and is within the main section of the distillation column;
  • Aspect 16 An apparatus for recovering He-3 from helium, the apparatus comprising: a distillation column having a main section and a top section, the main section being located below the top section and the main section having a first diameter that is greater than a second diameter of the top section;
  • a feed conduit for introducing a feed stream comprising helium into the distillation column at a first location, the feed conduit being in fluid flow communication with a supply of helium;
  • a bottom conduit for withdrawing a bottom stream comprising He-3-depleted helium from a bottom of the main section of the distillation column;
  • an intermediate condenser located in the main section at a third location that is located above the first location and having an upstream side that is in fluid flow communication with an intermediate conduit that supplies a first stream to the upstream side of the intermediate condenser.
  • Aspect 17 The apparatus of any of Aspects 16 and 18 through 20, wherein the first diameter is at least four times larger than the second diameter.
  • Aspect 18 The apparatus of any of Aspects 16, 17, and 19, further comprising a first heat exchanger located in a bottom portion of the main section, wherein the intermediate conduit is in flow communication with a downstream side of the first heat exchanger.
  • Aspect 19 The apparatus of any of Aspects 16 through 18 and 20, further comprising a chamber conduit and a top condenser, the chamber conduit being in flow communication with the intermediate conduit and with a chamber located above the top section of the distillation column, the top condenser being located with the chamber, the overhead conduit being in fluid flow communication with an upstream side of the top condenser.
  • Aspect 20 The apparatus of any of Aspects 16 through 19, wherein the intermediate conduit is in fluid flow communication with the chamber and supplies a second stream to the chamber.
  • Figure 1 is a flow diagram of an exemplary embodiment of the invention
  • Figure 2 is a flow diagram of a second exemplary embodiment of the invention.
  • Figure 3 is a flow diagram of a third exemplary embodiment of the invention, which shows the second exemplary embodiment incorporated into an exemplary liquefied helium plant.
  • flow communication and “fluid flow communication” are intended to mean that the elements described are connected (either directly or indirectly) in a manner that enables fluids to flow between the elements, including connections that may contain valves, gates, or other devices that may selectively restrict fluid flow.
  • conduit is intended to mean any pipe, tube, passageway or the like, through which a fluid may be conveyed.
  • An intermediate device such as a pump, compressor or vessel may be present between a first device in fluid flow communication with a second device, unless explicitly stated otherwise.
  • downstream and upstream refer to the intended flow direction of the process fluid transferred. If the intended flow direction of the process fluid is from the first device to the second device, the second device is in downstream fluid flow communication of the first device.
  • cryogen or “cryogenic fluid” is intended to mean a liquid, gas, or mixed-phase fluid having a temperature less than -70 degrees C.
  • cryogens include liquid nitrogen (LIN), liquid oxygen (LOX), liquid argon (LAR), liquid helium, liquid carbon dioxide and pressurized, mixed phase cryogens (e.g., a mixture of LIN and gaseous nitrogen).
  • cryogenic temperature is intended to mean a temperature below -70 degrees C.
  • helium refers to naturally occurring helium, which is a mixture of He-3 and He-4, with the content of He-3 typically in the range of 0.1 - 1.0 ppm by volume.
  • He-3 enriched helium is intended to mean helium having a concentration of He-3 that is higher than the helium used as a feed stream for the process or apparatus in question.
  • He-3 depleted helium is intended to mean helium having a concentration of He-3 that is lower than the helium used as the feed stream for the process or apparatus in question.
  • stage is well-known in the art and, as used herein, is intended to have its ordinary meaning.
  • stage is intended to mean theoretical stage. For the purposes of the specification and claims of this application, theoretical stages should be understood to increase from top to bottom, with the uppermost stage being stage 1. In other words, for the purposes of this application, an element that is located at the 30 th theoretical stage of a column is below an element that is located at the 20 th theoretical stage.
  • the system 10 comprises a distillation column 12 having packing 18, 20 positioned at several locations along the height H1 of the column.
  • the column 12 is preferably relatively small.
  • the construction of column 12 is preferably in accordance with conventional distillation columns used in cryogenic distillation processes.
  • the inner wall of the column 12 is preferably made of stainless steel or aluminum and is surrounded by a vacuum jacket.
  • the column 12 has a generally cylindrical main section 48 and a top section 46, which is significantly smaller in diameter than the main section 48.
  • the preferred overall height H1 of the column 12, as well as the individual heights H2 and H3 of the main section 48 and top section 46, respectively, will also depend upon the operational parameters of the system 10.
  • the column 12 is preferably operated in a temperature range of 2.3K - 4.3K.
  • the operating pressure of the column is preferably in the range of 5 - 15 psia (35 - 103 kPa) and, more preferably, in the range of 6- 10 psia (41 - 60 kPa).
  • the primary lower limitations on temperature and pressure are the avoidance of operating under conditions that would result in He-4 transitioning to a superfluid state, which occurs at 2.17K at 14.7 psia (101.4 kPa).
  • the primary upper constraint on operating pressure is the critical pressure of He-3, which is 16.5 psia (1 13.8 kPa). With the parameters set forth in this paragraph, the preferred operating temperature and pressure for the column will vary, depending on the configuration and other operating conditions of the plant in which the system 10 is implemented.
  • a helium feed stream is introduced into the main section 48 of the column 12 via a feed conduit 14.
  • the helium could be supplied from any suitable source.
  • the source could be storage vessel 15.
  • the feed stream is liquid helium (hereinafter "LHe").
  • LHe liquid helium
  • mixed phase vapor/liquid helium or helium vapor could be supplied to the feed stream.
  • the preferred location of the feed conduit 14 will depend upon the operating conditions of the column 12.
  • the feed stream would preferably be introduced via the feed conduit 14 at a location corresponding to a range of between the 20 th and 50 th theoretical stages and, more preferably, at a location corresponding to the 25 th theoretical stage.
  • This feed conduit 14 is connected to a suitable source of LHe and the LHe is supplied at a pressure that is higher than or equal to the operating pressure of the distillation column 12.
  • the feed conduit 14 could be connected to a source of two-phase helium or helium vapor.
  • the concentration of He-3 in the feed stream will depend upon the helium source, but will typically be in the range of 0.1 - 1 .0 ppm by volume.
  • a vaporous He- 3-enriched (hereinafter "VHe-3”) overhead stream exits the distillation column 12 at the top of the column via an overhead conduit 16 and is preferably compressed and then condensed.
  • a portion of the condensed (liquid) He-3-enriched stream is recycled via conduit 36 (as described below), and the remaining portion is stored using any suitable means.
  • the condensed He-3-enriched stream could be pumped into a storage tank (not shown).
  • a bottom stream comprising a He-3 liquid, exits the column 12 at the bottom via a bottom conduit 34 and is also collected and stored using any suitable means, such as a liquid storage tank (not shown).
  • a pump (not shown) could optionally be used to increase the pressure of the He-3 depleted liquid that is fed to the storage tank.
  • VHe vapor helium stream
  • a LHe stream exits the downstream side of the heat exchanger 24 via an intermediate conduit 26 and is then reduced in pressure through a valve or another flow restriction device 28, and vaporized in an intermediate condenser 30 to provide refrigeration for condensation of at least some of the fluid in the distillation column 12 that is in vapor phase at the location of the intermediate condenser 30 (referred to in the claims as a vapor stream).
  • a VHe stream exits the downstream side of the intermediate condenser 30 via a conduit 32 at a relatively low pressure, where it is heated to close to ambient temperature, compressed to a higher pressure (using any suitable means, represented schematically as box 23), and recirculated through the heat exchanger 24 via conduit 22.
  • the VHe stream could be cold compressed instead of being heated to ambient temperature prior to compression.
  • the intermediate condenser 30 is located in the main section 48 of the column
  • the intermediate condenser 30 is positioned within the column 12 at or below a stage at which the concentration of He-3 is no more than 99.0% and, more preferably, no more than 1.0%.
  • the portion of the vaporous He-3-enriched overhead stream that is recycled is compressed and supplied to a heat exchanger 38 located near the bottom of the column 12 by the conduit 36, where it is condensed.
  • the He-3-enriched stream may be heated to ambient temperature before compression and may also be cooled after compression to a cryogenic temperature by any suitable means prior to entering the heat exchanger 38.
  • Box 25 schematically represents suitable means for heating, compressing, and cooling the He-3- enriched stream.
  • the condensed VHe-3 stream is then fed by a conduit 40 as reflux into the column 12 in the top section 46, near the top of the column 12.
  • a valve 42 is preferably located on the conduit 40, in order to reduce the pressure of the condensed VHe-3 stream before it is reintroduced into the column 12.
  • Applicants have discovered that providing a top section 46 having a diameter that is significantly smaller than that of the main section 48 and providing the intermediate condenser 30 at a location between zero and 30 stages above the LHe feed stream (conduit 14), at the conditions used for simulation, provides acceptable separation performance, while enabling the void volume and overall surface area of the column 12 to be significantly less than a system 10 in which these features are not provided. Due to the fact that the system 10 is operated at very low cryogenic temperatures, keeping the surface area of the column 12 to a minimum is a very important aspect of operational efficiency because surface area is proportional to heat loss. In addition, as noted above, keeping the overall volume of the column and the volume of the top section 46 small is even more important for this process due to the extremely small amount of He-3 in the feed stream.
  • the diameter D1 of the main section 48 is preferably between 4 and 20 (more preferably about 10) times the diameter D2 of the top section 46. In the event that the diameter D1 of the main section 48 is ten times the diameter D2 of the top section 46, the flow area in the top section 46 is about 1 % of that in the main section 48.
  • Packing material 18, 20 is preferably located within both the top section 46 and the main section 48 of the column 12.
  • any heat exchangers 24, 38 that perform a reboiling function are preferably located beneath all of the packing material 18, 20 located in the column 12.
  • no packing material is positioned in the main section between the intermediate condenser 30 and the shoulder 52, which defines the transition between the main section 48 and the top section 46.
  • the preferred arrangement of packing material described in this paragraph applies to all three systems 10, 1 10, 210 described herein.
  • the column 12 may also include a distributor, liquid collectors and other components known in the art (not shown).
  • the condensed LHe stream in the intermediate conduit 126 is split into two streams, which flow through conduit 127 and a chamber conduit 129.
  • the stream passing through conduit 127 is reduced in pressure and fed into the intermediate condenser 130, where the stream is vaporized.
  • the stream flowing through the conduit 127 provides condensation duty for vapor rising in the column 1 12, thereby greatly reducing the amount of vapor that rises above the intermediate condenser 130.
  • the other stream (referred to herein as the overhead vaporizing stream), which flows through the chamber conduit 129, is vaporized in a chamber 161 (often referred to in the art as a "can") located above the top of the column 1 12.
  • a He-3- enriched vapor steam (also referred to herein as an overhead He-3-enriched stream) flows through the overhead conduit 1 16 into the upstream side of a condenser 154, where it is condensed through heat exchange with the helium that flows into the chamber 161 from the chamber conduit 129. This heat exchange results in vaporization of the helium, which is withdrawn from the top of the chamber 161 as an overhead vapor stream via a conduit 157.
  • He-3 enriched liquid exits the downstream side of the condenser 154 and is separated into a reflux stream, which is returned to the top of the column 1 12 via conduit 159, and a product stream, which flows into conduit 156 and is pumped (using a pump 158) into a storage vessel 160.
  • the stream being fed to the intermediate condenser 130 via conduit 127 preferably represents a major fraction of the LHe stream from the intermediate conduit 126, and the stream being fed to the chamber 161 via the chamber conduit 129 preferably represents a minor fraction of the LHe stream from the intermediate conduit 126. This eliminates the need for a VHe-3 stream to be used for additional reboiling duty and reflux, as needed in the first exemplary system 10.
  • the helium vapor withdrawn from the chamber 161 in the overhead vapor stream via conduit 157 and helium vapor withdrawn from the downstream side of the intermediate condenser 130 via conduit 132 are preferably recycled via conduit 139 for use in reboiling (via heat exchanger 124) and/or as part of the feed stream. In either case, it is necessary to perform work on the helium vapor, for example by compressing, warming and/or cooling the vapor, by any suitable means (represented schematically by box 123) prior to being recycled.
  • the portion of the helium vapor from conduits 139 and 132 that is used for reboiling is transported to the heat exchanger 124 via conduit 122.
  • the portion of the helium vapor from conduits 139 and 132 that is used in the feed stream is transported via conduit 133 and is cooled and liquefied by any suitable means (represented schematically by box 1 15) prior to being reintroduced to the feed conduit 1 14.
  • the feed stream could alternatively be a two phase (vapor/liquid) stream or a vapor stream.
  • Make-up helium will need to be added to the system 1 10 in order to balance the fluids being withdrawn via conduits 134 and 156. Any suitable source of helium could be used and the make-up helium could be added at any suitable location.
  • the makeup helium is shown as being added via conduit 137 at box 123, which schematically represents that apparatus in which work is performed on helium vapor from conduits 139 and 132.
  • make-up helium could be added at box 1 15, which schematically represents the apparatus used to liquefy helium prior to being introduced into the feed conduit 1 14.
  • packing material 1 19 is located between the feed conduit 1 14 and the intermediate condenser 130.
  • FIG. 3 a third exemplary system 210 is shown. In this system
  • the system 210 represents an example of the incorporation of the He-3 separation process into a helium liquefaction plant.
  • LHe from a storage vessel 262 is fed into the column 212 via the feed conduit 214.
  • a valve 217 is preferably provided on the feed conduit 214 in order to enable adjustment of flow rates and, if necessary, to reduce the pressure of the LHe feed stream before being introduced into the column 212.
  • He stream flowing through the chamber conduit 229 into the chamber 261 is withdrawn from the chamber 261 by conduit 257 and is heated to a temperature that is preferably close to ambient temperature by being passed through a heat exchanger 272, and then through three compression stages 274, 276, 278.
  • Each of the stages 274, 276, 278 schematically shown in Figure 3 could represent one or more physical stages.
  • intercoolers (not shown) could optionally be provided between physical stages.
  • a conduit 288 returns the helium to a liquefier 266, where it is liquefied, sent to the storage vessel 262, and then recycled through the feed conduit 214.
  • a portion of the partially compressed helium is drawn from conduit 286 (extending between the second and third stages 276, 278) by conduit 280 and is cooled by the heat exchanger 272.
  • the VHe stream exiting the heat exchanger 272 then flows into conduit 222, where it provides a reboiling function by being passed through a heat exchanger 224 located at or near the bottom of the column 212.
  • a portion of the LHe feed stream is diverted from the feed conduit 214 via conduit 221 , which is then combined with the condensed LHe stream in the intermediate conduit 226.
  • the helium stream in intermediate conduit 226 is then split into two streams. One of the streams is fed to, and vaporized in, the intermediate condenser 230 via conduit 227 and the other stream is fed to, and vaporized in, the chamber 261 via the chamber conduit 229.
  • the stream being fed to the intermediate condenser 230 by conduit 227 preferably represents a major fraction of the LHe stream from intermediate conduit 226, and the stream being fed to the chamber 261 by the chamber conduit 229 preferably represents a minor fraction of the LHe stream flowing through intermediate conduit 226.
  • the vaporized He stream exiting the downstream side of the intermediate condenser 230 via conduit 232 passes through the heat exchanger 272.
  • at least a portion of the helium stream exiting the last compression stage 278 may be diverted via conduit 289 to be cooled via the heat exchanger 272, before being delivered to the liquefier 266 via a conduit 290.
  • the overall effect of the heat exchanger 272 is to cool the portion of the recycled VHe stream which is drawn off between the second and third stages 276 via conduit 280 and the portion of the VHe stream flowing through conduit 289, to heat the overhead vapor stream in conduit 257 to a temperature close to ambient temperature prior to the first compression stage 274, and to heat the VHe stream in conduit 232 to a temperature close to ambient temperature prior to being combined with the VHe stream in conduit 284 at a location in the compression process where the pressures in the conduit 284 and conduit 232 are roughly equal. In this exemplary embodiment, this occurs between the first and second compression stages 274, 276.
  • a pump could optionally be used to boost the pressure of the LHe-4 stream before it is fed into the storage vessel 235.
  • the LHe feed stream is fed into the column 12 via conduit 14 from a source of
  • LHe having about 0.1 ppm He-3 at a flow rate of 1 kmol/s, at a pressure that is roughly equal to pressure in the column 12, and at a temperature below the dew point of the fluid in the LHe feed stream.
  • a LHe-4 stream is withdrawn from the bottom of the column 12 via the bottom conduit 34 at a temperature of about 3.26K.
  • a VHe stream is fed into the heat exchanger 24 via conduit 22 at a flow rate of approximately 1 kmol/s, a pressure that allows it to condense at a temperature somewhat higher than 3.26 K (e.g., 0.1 K higher), and a temperature of close to its dew point.
  • VHe-3 stream via overhead conduit 16 at a flow rate of at least 9.93 x 10 "8 kmol/s, at a pressure of 5 psia (34 kPa) and temperature of 2.33K.
  • the portion of the VHe-3 stream that is diverted via conduit 36 for reboiling has a flow rate of 0.01 kmol/s.
  • Example 2 This example is based on the exemplary system 1 10 shown in Figure 2 and described above. The total number of theoretical stages is 55. The intermediate condenser 130 is located at the 20th stage.
  • the LHe feed stream is fed into the column 1 12 via the feed conduit 1 14 from a source of LHe having about 0.2 ppm He-3 at a flow rate of 1 kmol/s, a pressure that is above the pressure in the column 1 12 and a temperature close to its dew point.
  • the LHe-4 stream is withdrawn from the bottom of the column 12 via conduit 134 at a temperature of 3.26K.
  • the VHe stream is fed into the heat exchanger 124 via conduit 122 at a flow rate of 1 kmol/s, a pressure of 6 psia (41 kPa), and at a temperature near its dew point.
  • the LHe stream is fed into the intermediate condenser 130 via conduit 127 at a pressure of 4 pisa (28 kPA).
  • the LHe stream is fed into the chamber 161 by a chamber conduit 129 as reflux at a flow rate of 0.0059 kmol/s and a pressure of 0.85 psia (586 Pa).
  • a stream of LHe-3 at a purity of 99.3% is withdrawn from the condenser 154 via conduit 156 at a flow rate of 0.0000002 kmol/s, a pressure of 5 psia, and temperature of 2.33K.
  • a stream of VHe is withdrawn from the top of the chamber 161 via conduit 157 at a flow rate of 0.0059 kmol/s, a pressure of 0.85 psia (586 Pa), and a temperature of 2.23K.
  • the duty of the intermediate condenser 130 is -90.000 kW/h.
  • the duty of the heat exchanger 124 used for reboiling is 88.621 kW/h.
  • the duty of the condenser 154 is - 0.452 kW/h.
  • This example is also based on the exemplary system 1 10 shown in Figure 2 and described above.
  • the total number of theoretical stages is 75.
  • the intermediate condenser 130 is located at the 20th stage.
  • the LHe feed stream is fed into the column 1 12 via the feed conduit 1 14 from a source of LHe having about 0.1 ppm He-3 at a flow rate of 1 kmol/s, a pressure that is above the pressure in the column 1 12 and a temperature close to its dew point.
  • the LHe-4 stream is withdrawn from the bottom of the column 12 via conduit 134 at a temperature of 3.53K.
  • the VHe stream is fed into the heat exchanger 124 via conduit 122 at a flow rate of 1 kmol/s, a pressure of 14.7psia (101 kPa), and at a temperature near its dew point.
  • the LHe stream is fed into the intermediate condenser 130 via conduit 127 at a pressure of 4 psia (28 kPa).
  • the LHe stream is fed into the chamber 161 via the chamber conduit 129 as reflux at a flow rate of 0.02 kmol/s and a pressure of 1 .22psia (8.41 kPa).
  • a stream of LHe-3 at a purity of 99.9% is withdrawn from the condenser 154 via conduit 156 at a flow rate of 0.0000001 kmol/s, a pressure of 7 psia (48 kPa), and a temperature of 2.57K.
  • a stream of VHe is withdrawn from the top of the chamber 161 via conduit 157 at a flow rate of 0.02 kmol/s, a pressure of 1 .22 psia (8.41 kPa), and a temperature of 2.40K.
  • the duty of the intermediate condenser 130 is -120.000 kW/h.
  • the duty of the heat exchanger 124 used for reboiling is 122.519 kW/h.
  • the duty of the condenser 154 is - 0.851 kW/h.

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

Abstract

La présente invention concerne un système et un procédé de récupération d'hélium 3 à partir d'hélium. Une colonne de distillation présentant une section supérieure dont le diamètre est plus petit que celui d'une section principale est décrite. La colonne inclut également un condenseur intermédiaire situé dans la section principale et au-dessus d'un flux d'alimentation d'hélium. Le reflux dans la colonne peut être fourni par de l'hélium 3 liquide provenant d'une conduite ou d'un condenseur de tête. Dans un cycle préféré, la colonne de distillation est exploitée à une pression sous-atmosphérique et à une température s'étendant entre 2,3 K et 4,3 K.
PCT/US2012/026293 2012-02-23 2012-02-23 Récupération de 3he à partir d'hélium naturel par distillation WO2013126060A1 (fr)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
RU2830470C1 (ru) * 2024-05-31 2024-11-19 Публичное акционерное общество "Газпром" Способ получения изотопа гелия-3 из природного гелия и устройство для его осуществления

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4525186A (en) * 1972-11-17 1985-06-25 Leo Garwin Method for producing isotopically enriched helium-4 and use of same as nuclear reactor coolant

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4525186A (en) * 1972-11-17 1985-06-25 Leo Garwin Method for producing isotopically enriched helium-4 and use of same as nuclear reactor coolant

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
KHIMISCHESKOE I NEFTYANOE MACHINOSTROENIE, February 1995 (1995-02-01), pages 38 - 39
KUZ'MENKO; LEBEDEV, CHEMICAL AND PETROLEUM ENGINEERING, vol. 31, no. 1-2, 1995

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
RU2830470C1 (ru) * 2024-05-31 2024-11-19 Публичное акционерное общество "Газпром" Способ получения изотопа гелия-3 из природного гелия и устройство для его осуществления

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