EP2567159B1 - Gas liquefaction system and method - Google Patents

Gas liquefaction system and method Download PDF

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Publication number
EP2567159B1
EP2567159B1 EP11720246.5A EP11720246A EP2567159B1 EP 2567159 B1 EP2567159 B1 EP 2567159B1 EP 11720246 A EP11720246 A EP 11720246A EP 2567159 B1 EP2567159 B1 EP 2567159B1
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EP
European Patent Office
Prior art keywords
gas
pressure
liquefaction
interior tank
coldhead
Prior art date
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EP11720246.5A
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German (de)
English (en)
French (fr)
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EP2567159A2 (en
Inventor
Conrado Rillo MILLÁN
Leticia Tocado MARTÍNEZ
Richard C. Reineman
Richard J. Warburton
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Consejo Superior de Investigaciones Cientificas CSIC
Universidad de Zaragoza
GWR Instruments Inc
Original Assignee
Consejo Superior de Investigaciones Cientificas CSIC
Universidad de Zaragoza
GWR Instruments Inc
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Classifications

    • 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
    • F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
    • F25J1/0002—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the fluid to be liquefied
    • F25J1/0005—Light or noble gases
    • F25J1/0007—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
    • F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
    • F25J1/02—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process
    • F25J1/0225—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process using other external refrigeration means not provided before, e.g. heat driven absorption chillers
    • 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
    • F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
    • F25J1/02—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process
    • F25J1/0243—Start-up or control of the process; Details of the apparatus used; Details of the refrigerant compression system used
    • F25J1/0257—Construction and layout of liquefaction equipments, e.g. valves, machines
    • F25J1/0258—Construction and layout of liquefaction equipments, e.g. valves, machines vertical layout of the equipments within in the cold box
    • 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
    • F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
    • F25J1/02—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process
    • F25J1/0243—Start-up or control of the process; Details of the apparatus used; Details of the refrigerant compression system used
    • F25J1/0257—Construction and layout of liquefaction equipments, e.g. valves, machines
    • F25J1/0275—Construction and layout of liquefaction equipments, e.g. valves, machines adapted for special use of the liquefaction unit, e.g. portable or transportable devices
    • F25J1/0276—Laboratory or other miniature devices
    • 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
    • F25J2230/30—Compression of the feed stream
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/90—External refrigeration, e.g. conventional closed-loop mechanical refrigeration unit using Freon or NH3, unspecified external refrigeration
    • F25J2270/908—External refrigeration, e.g. conventional closed-loop mechanical refrigeration unit using Freon or NH3, unspecified external refrigeration by regenerative chillers, i.e. oscillating or dynamic systems, e.g. Stirling refrigerator, thermoelectric ("Peltier") or magnetic refrigeration
    • 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
    • F25J2290/60—Details about pipelines, i.e. network, for feed or product distribution
    • 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
    • F25J2290/62—Details of storing a fluid in a tank

Definitions

  • This invention relates generally to systems and methods for liquefaction of gases, and more particularly to such systems and methods adapted for improved liquefaction and performance efficiency.
  • a gas liquefaction system according to the preamble of claim 1 is known from US 2009/293505 .
  • Helium is a scarce element on earth and its numerous scientific and industrial applications continue to drive a growing demand.
  • common uses of gas-phase helium include welding, lifting (balloons), and semiconductor and fiber optic manufacturing.
  • common uses include refrigeration of certain medical and scientific equipment, purging fuel tanks (NASA), and basic research in solid-state physics, magnetism, and a wide variety of other research topics.
  • NASH purging fuel tanks
  • liquid helium is used as the refrigerant in many applications in which it is necessary to reach temperatures below -200° C.
  • Such applications are frequently related to the use of superconductors, and particularly in low-temperature physics research equipment which operates in evacuated and insulated containers or vacuum flasks called Dewars or cryostats.
  • cryostats contain a mixture of both the gas and liquid phases and, upon evaporation, the gaseous phase is often released to the atmosphere. Therefore it is often necessary to purchase additional helium from an external source to continue the operation of the equipment in the cryostat.
  • liquid helium One of liquid helium's most important applications is to refrigerate the high magnetic field superconducting coils used in magnetic resonance imaging (MRI) equipment, which provides an important diagnostic technique by non-invasively creating images of the internal body for diagnosing a wide variety of medical conditions in human beings.
  • MRI magnetic resonance imaging
  • the largest users of liquid helium are large international scientific facilities or installations, such as the Large Hadron Collider at the CERN international laboratory.
  • Laboratories such as CERN recover, purify, and re-liquefy the recovered gas through their own large scale (Class L) industrial liquefaction plants, which typically produce more than 100 liters/h and require input power of more than 100 kW.
  • Class L large scale
  • Class M medium liquefaction plants are available that produce about 15 liters/hour.
  • These large and medium liquefaction plants achieve a performance, R, of about 1 liter hour/kW (24 liters/day/kW) when the gas is pre-cooled with liquid nitrogen, and about 0.5 liters/hour/kW (12 liters/day/kW) without pre-cooling.
  • small-scale refrigerators are now commercially available which are capable of achieving sufficiently low temperatures to liquefy a variety of gases and, in particular, to liquefy helium at cryogenic temperatures below 4.2 Kelvin.
  • these small-scale refrigerators are normally referred to as closed-cycle cryocoolers.
  • cryocoolers have three components: (1) a coldhead (a portion of which is called the "cold finger” and typically has one or two cooling stages), where the coldest end of the cold finger achieves very low temperatures by means of the cyclical compression and expansion of helium gas; (2) a helium compressor which provides high pressure helium gas to and accepts lower pressure helium gas from the coldhead; and (3) the high and low pressure connecting hoses which connect the coldhead to the helium compressor.
  • Each of the one or more cooling stages of the cold finger has a different diameter to accommodate variations in the properties of the helium fluid at various temperatures.
  • Each stage of the cold finger comprises an internal regenerator and an internal expansion volume where the refrigeration occurs at the coldest end of each stage.
  • cryocooler coldhead operates in the neck of a double-walled container, often called a Dewar, which contains only the gas to be liquefied and is thermally insulated to minimize the flow of heat from the outside to the inside of the container. After the gas condenses, the resulting liquid is stored inside the inner tank of the Dewar.
  • GB 2 457 054 as well as the above cited US 2009/293505 are both designed as recondensing systems in low temperature device cryostats with the purpose to keep the system at the low design temperature required for operating e. g. superconducting devices such as a SQUID in US 2009/293505 or a superconducting magnet in GB 2 457 054 .
  • superconducting devices such as a SQUID in US 2009/293505 or a superconducting magnet in GB 2 457 054 .
  • These systems are therefore not designed for a maximum liquefaction rate but rather for optimized cooling of the system.
  • an optimized liquefaction rate may rather not be obtained at the typical lower temperatures provided for a safe operation of said superconducting devices as considered by the above documents.
  • a liquefaction system In order to obtain a liquefaction system with optimized liquefaction rate, there is provided a liquefaction system according to claim 1. It is a purpose of embodiments of this invention to provide a gas liquefaction system, and methods for liquefaction of gas therein, based on a cryocooler, that is adapted to utilize the thermodynamic properties of gaseous elements to extract increased cooling power from the cryocooler by operating at elevated pressures, and hence elevated liquefaction temperatures, wherein the increased cooling power of the cryocooler is utilized to improve the liquefaction rate and performance of the system.
  • the gas liquefaction system is adapted with a means for controlling pressure within a liquefaction region of the system such that an elevated pressure provides operation at increased liquefaction temperature as described above.
  • an elevated pressure provides operation at increased liquefaction temperature as described above.
  • an internal liquefaction pressure can be maintained at an elevated threshold.
  • the increased cooling power of the coldhead is utilized.
  • the liquefaction region is herein defined as a volume within the Dewar including a first cooling region adjacent to a first stage of a cryocooler where gas entering the system is initially cooled, and a second condensation region adjacent to a second or subsequent stage of the cryocooler where the cooled gas is further condensed into a liquid- phase.
  • the liquefaction region includes the neck portion of the Dewar and extends to the storage portion where liquefied cryogen is stored.
  • the means for controlling-pressure-can include a unitary pressure control module being adapted to regulate an input gas flow for entering the liquefaction region such that pressure within the liquefaction region is precisely maintained during a liquefaction process.
  • a series of pressure control components selected from solenoid valves, a mass flow meter, pressure regulators, and other pressure control devices may be individually disposed at several locations of the system such that a collective grouping of the performance of small-scale liquefiers, and such improvements would be of particular benefit in the art.
  • the gas liquefaction system is adapted with a means for controlling pressure within a liquefaction region of the system such that an elevated pressure provides operation at increased liquefaction temperature as described above.
  • an elevated pressure provides operation at increased liquefaction temperature as described above.
  • an internal liquefaction pressure can be maintained at an elevated threshold.
  • the increased cooling power of the coldhead is utilized.
  • the liquefaction region is herein defined as a volume within the Dewar including a first cooling region adjacent to a first stage of a cryocooler where gas entering the system is initially cooled, and a second condensation region adjacent to a second or subsequent stage of the cryocooler where the cooled gas is further condensed into a liquid-phase.
  • the liquefaction region includes the neck portion of the Dewar and extends to the storage portion where liquefied cryogen is stored.
  • the means for controlling pressure can include a unitary pressure control module being adapted to regulate an input gas flow for entering the liquefaction region such that pressure within the liquefaction region is precisely maintained during a liquefaction process.
  • a series of pressure control components selected from solenoid valves, a mass flow meter, pressure regulators, and other pressure control devices may be individually disposed at several locations of the system such that a collective grouping of the individualized components is adapted to provide control of an input gas entering into the liquefaction region of the system.
  • the liquefied gas element is helium.
  • the helium gas is then liquefied at pressures close to 2.27 bar and at about 5.19 K to maximize the power available from the closed-cycle cryocooler.
  • the system is capable of liquefying a mass of 19 kg of helium from 105,000 liters of helium gas under standard conditions into a container of 150 liter volume.
  • a gas liquefaction system for liquefying gas comprising:
  • a gas intake module configured to provide gas to the system from a gas source
  • thermally isolated container whose upper part is comprised of at least one neck portion, and further comprises at least one interior tank configured to hold gas and the resulting liquid from gas that has already been liquefied;
  • cryocooler coldhead located at the top of the thermally isolated container, with its cold portion at least partially extending within the neck portion and routed toward the interior tank of the container;
  • a gas compressor configured for providing compressed gas to the cryocooler coldhead by means of confections for the operation of the cryocooler
  • At least one gas pressure control mechanism configured to control the gas intake pressure flowing from the gas intake module and to adjust such pressure to the required gas pressure inside the system
  • control devices configured to control the performance of the system and the cryocooler coldhead by means of the gas pressure control mechanisms.
  • the system according to embodiments of the invention is adapted to maintain precise control over the vapor pressure inside the container, and thus is adapted to maintain precise control of the temperature and hence the power of the cryocooler where condensation is produced. Consequently, the system allows control of the operating point and power of the cryocooler, as determined by the temperatures of its one or more stages, and thereby the amount of heat that can be extracted from the gas, both for its pre-cooling from room temperature to the point of operation, and for its condensation and liquefaction.
  • Another aspect of the invention provides a gas liquefaction method that makes use of the gas liquefaction system disclosed in the present application which comprises the following steps:
  • the gas liquefaction system described in the detailed Description below achieves much higher efficiencies than existing cryocooler-based liquefiers by performing the gas liquefaction at a higher pressure and therefore a higher temperature, where the cryocooler has much greater cooling power to perform the liquefaction and the cryogen being liquefied has a much lower heat of condensation.
  • the liquefaction efficiency of the system is further enhanced and stabilized by precisely controlling the flow rate of the room temperature gas entering the liquefaction region, and thereby precisely controlling the pressure of the condensing gas in the liquefaction region of the system.
  • a liquefaction system also referred to herein as a cryostat, includes an isolated storage container or Dewar comprising a storage portion and a neck portion extending therefrom and connected to an outer vessel which is at ambient temperature.
  • the Dewar is insulated by a shell with the volume within the shell external of the storage portion being substantially evacuated of air.
  • the neck portion is adapted to at least partially receive a cryocooler coldhead.
  • the coldhead may comprise one or more stages, each having a distinct cross section.
  • the neck portion of the isolated container may be optionally adapted to geometrically conform to one or more stages of the coldhead cryocooler in a stepwise manner.
  • the isolated container further comprises a transfer port extending from the storage portion to an upper surface of the Dewar.
  • a control mechanism is further provided for controlling gas flow and, thereby, pressure within a liquefaction region of the Dewar.
  • the control mechanism generally includes: a pressure sensor for detecting pressure within the liquefaction region of the cryostat; a pressure regulator or other means for regulating pressure of gas entering the liquefaction region of the Dewar; a mass flow meter; and one or more valves for regulating input gas flow entering the liquefaction region.
  • the control mechanism is further connected to a computer for dynamically modulating input gas flow, and hence, pressure within the liquefaction region of the cryostat for yielding optimum efficiency.
  • cryostat may comprise one or more storage portions and one or more neck portions extending therefrom within the isolated container.
  • the refrigeration coldhead of the gas liquefaction system is routed toward the interior tank of the container and comprises at least one stage defining a refrigeration stage.
  • the cryocooler coldhead comprises a cylinder that routes toward the interior tank of the container consisting of a first stage and a second stage, both parallel-oriented to the neck of the container, and that collectively define two refrigeration stages.
  • cryocooler coldhead routed toward the interior tank of the container comprises three or more stages collectively defining three or more refrigeration stages.
  • the coldhead comprising one or more stages of the refrigeration system operates in the neck of a thermally isolated container or Dewar.
  • the first stage is the warmest and operates in the neck further from the liquefaction region than the other stages that operate in the neck closer to the liquefaction region.
  • the gas enters at the warm end of the neck and is pre-cooled by the walls of the first stage of the coldhead, by the coldest end of the first stage, further precooled by the walls of the colder stages, and is then condensed at the coldest end of the coldest stage of the coldhead.
  • the condensation occurs at the coldest end of the first stage.
  • the liquid falls to the bottom of the tank, or storage portion, located in the interior of the isolated container.
  • the cooling power that each stage of a closed-cycle cryocooler generates is determined mainly by its temperature, but also depends to second order on the temperature of the previous stages. This information is generally supplied by the cryocooler manufacturer as a two dimensional load map that plots the dependence of the power of the first and second stages versus the temperatures of the first and second stages. Of importance to this invention is that the cooling power available at each stage generally increases with temperature.
  • the coldhead In addition to generating cooling power at the first and subsequent stages, the coldhead also generates cooling power along its entire length, in particular along the surface of the cylindrical cold finger between room temperature and the coldest end of the first stage, and along the length of the cylindrical cold finger between the first and subsequent stages. It is an object of this invention to optimize the heat exchange between the gas and the various cooling stages, as well as between the gas and the walls of the cylindrical cold finger between the various cooling stages of the cryocooler coldhead. This is achieved by using the high thermal conductivity properties of the gas without the need for mechanical heat exchangers or condensers of any kind that attach to the coldhead, or any radiation screens in the neck, which have generally been considered as essential in previous state-of-the-art systems.
  • a multi-stage coldhead is constructed with the upper or first stage having a larger diameter than the lower stages of the coldhead.
  • the stages of the cryocooler coldhead are manufactured in a step pattern where the two or more stages have different cross sections.
  • the neck portion of the isolated container can be adapted in various embodiments for receiving the one or more stages of the cryocooler coldhead.
  • the neck portion of the isolated container can include an inner surface adapted to closely match the surface of the one or more stages of the cryocooler coldhead, such that the neck portion comprises a first inner diameter at the first stage and a second inner diameter at the second stage, wherein the first inner diameter is distinct from the second inner diameter.
  • the narrowed volume reduces the heat load down the neck, while the stepped neck improves the exchange process between the gas and the cryocooler, favoring natural convection in the stepped area, at least during the initial cooldown.
  • the neck portion can be adapted with a uniform inner diameter extending along a length of the neck portion adjacent to the one or more stages of the cryocooler coldhead.
  • the exchange process is still efficient for initial cooldown and liquefaction.
  • the present invention can make use of straight or stepped necks inside the container.
  • the gas pressure control mechanism comprises one or more of the following elements:
  • a system of pipes or tubing, valves (manually or electronically controlled), and control mechanisms enables the manipulation of both the pressure and mass flow rate of the gas as it enters the Dewar.
  • the intake gas pressure may differ from the pressure of gas present within the Dewar, or the pressure in the Dewar may need to be adjusted to achieve optimal performance.
  • the system integrates the aforementioned gas-pressure control mechanisms by means of, for instance, a solenoid valve and a pressure control mechanism. This process regulates the intake pressure as deemed necessary to control the flow of gas from the gas-intake mechanisms to the Dewar.
  • the system of this invention achieves its precision pressure control through the use of control-mechanisms that regulate the cooling power of the cryocooler's coldhead by adjusting the valves and the mass flow of the gas.
  • control mechanisms receive the necessary data from the system to calculate the level of liquid inside the container, which is needed to perform the necessary adjustments.
  • the liquefying processes can be performed under varying pressure ranges starting at slightly above atmospheric pressures and reaching near-critical gas pressure values. All functions and procedures are controllable remotely or in situ, using programmable devices. such as personal computers or an FPGA (Field Programmable Gate Array), with specific control software (such as LabView-based applications), or connected to digital storage hardware in which such software is stored and remotely accessed.
  • FPGA Field Programmable Gate Array
  • the liquefaction system comprises a transfer port and valve located at the top of the isolated container that allows the extraction of the liquid, resulting from liquefied gas present in the storage portion within the interior tank.
  • the gas liquefaction method comprises the determination of the level of liquefied gas inside the storage portion of the interior tank from the total mass of the gas contained in the interior tank and the gas and liquid densities determined by measurement of the pressure or temperature at thermodynamic equilibrium.
  • the gas level can be calculated based upon an algorithm involving the mass flow rate, the integrated mass flow rate, the total volume of the inner tank of the container, and the densities of the gas and liquid as determined by the pressure and temperature inside the container.
  • the gas liquefaction method includes a cleaning mode comprising the steps of:
  • the gas liquefaction method includes a stand-by mode, in which the volume of liquefied gas is indefinitely conserved in equilibrium with the vapor, initiated by the control devices, triggering of the intake valve by means of the gas pressure control mechanisms to close the gas intake into the system and obtaining the necessary reduced power by performing start/stop cycles of the coldhead or through the speed control of the coldhead of the cryocooler.
  • the start/stop cycles of the cryocooler coldhead produce temperature cycles in the coldhead that permit the fusion and subsequent precipitation of impurities acquired at the stepped cylinder of the aforementioned coldhead.
  • the gas liquefaction method enables direct liquefaction of recovered gas at or slightly above atmospheric pressure, the method comprising:
  • the temperature of gaseous and liquid helium is solely defined by the equilibrium vapor-pressure curve.
  • the temperature of helium increases with pressure along the vapor-pressure curve.
  • both pressure and temperature increase from the triple point of helium (at an absolute pressure of 0.051 bar and a temperature of 2.17 K) to the critical point of helium, which occurs at the critical pressure, P c , of 2.27 bar absolute and critical temperature, T c , of 5.19 K.
  • the lowest temperature reached by closed cycle cryocoolers is about 3 K for which the vapor pressure of helium is about 0.5 bar.
  • a practical range over which the capabilities of closed-cycle cryocooler systems and the helium vapor-pressure curve overlap is from about 0.5 bar at 3 K to 2.27 bar at 5.19 K. Accordingly, the refrigeration system can also perform at the intermediate point at atmospheric pressure and at a temperature of 4.23 K.
  • the gas pressure control mechanisms, the gas intake module, and the control devices are governed by means of a software program in at least one digital data storage means.
  • the digital data storage means is connected to a programmable device in charge of executing the software program.
  • a method for liquefaction of gas in conjunction with the described systems.
  • the method comprises:
  • the method may further comprise the step of processing data on a computer for dynamic control of the cryostat, wherein the data includes at least one of: the measured vapor pressure; and a rate of the input gas flow.
  • cryogens may be utilized in a similar manner including, without limitation: nitrogen, oxygen, hydrogen, neon, and other gases.
  • the components of the control mechanism can be individually located near other system components and adapted to effectuate a similar liquefaction process.
  • the pressure regulator can be attached to the gas storage source or otherwise positioned anywhere between the storage source and liquefaction region of the cryostat system.
  • the source can be fitted with a compressor for supplying an input gas at a desired pressure.
  • Such a system would not necessarily require a pressure regulator within the pressure control mechanism.
  • the pressure control mechanism is intended to include a collection of components in direct attachment or otherwise collectively provided within the system for dynamically controlling input gas flow, and thus pressure within the liquefaction region of the cryostat.
  • Fig.1 illustrates a general phase diagram of helium 4.
  • the range of operation for general closed cycle cryocooler coldheads is between about 3.0 K and about 5.2 K and between about 0.25 bar and about 2.27 bar.
  • Z 1 represents a point at which helium gas is liquefied at atmosphere, and the liquefaction temperature is about 4.2 K, as is the current state of the art for small scale liquefiers.
  • Z 2 represents a point on the liquefaction curve at which helium gas is liquefied just below the critical point where the liquid and gas are in equilibrium.
  • the pressure at Z 2 is near the critical pressure Pc (here about 2.2 bar), and the liquefaction temperature at Z 2 is about 5.2 K. It is at this point (Z 2 ) where the present liquefaction system is intended to operate and is preferably operated during a typical helium gas liquefaction process.
  • the optimal liquefaction pressure is slightly below the critical pressure, that is, 2.1 bar for the case of helium, a pressure for which rates can reach and surpass 65 liters/day at 2.1 bar (260 g/h), equivalent to 50 liters/day at 1 bar, with efficiencies equal to or even greater than 7 liters/day/kW.
  • Fig. 2 represents a load map, which defines the characteristics of a typical cryocooler coldhead 18 (see Fig. 3 ) operating at 50 Hz and using 7.5 kW of power.
  • the load map defines the unique relationship between a set of paired points (T 1 , T 2 ) and (P 1 , P 2 ), where T 1 is the temperature of the coldest end of the first stage, T 2 is the temperature of the coldest end of the second stage, P 1 is the power of first stage 10, and P 2 is the power of second stage 11.
  • the measured point (0 W, 0 W) maps to the point (3 K, 24 K), which indicates that the lowest temperatures achieved with no load applied to either of the two stages of this cryocooler are about 3 K on the second stage and 24 K on the first stage.
  • the measured point (5 W, 40 W) maps to the point (6.2 K, 45 K) and shows that if 5 W of power is applied to the second stage and 40W of power is applied to the first stage, then the second stage will operate at about 6.2 K and the first stage at about 45 K.
  • the measured load map points are connected by lines to interpolate intermediate points.
  • An efficient helium gas liquefaction cycle is also shown on the load map as the continuous line cycle connecting points (a), (b), and (c).
  • the points are determined by the temperature (or pressure) of the helium and are plotted versus the temperature T 2 of the second stage.
  • Point (a) is at a temperature (T 2 ) of about 4.3 K, which corresponds to a pressure of about 1.08 bar, which is slightly above atmospheric pressure at 1.0 bar.
  • the liquefaction rate is about 20 liters/day.
  • Point (b) is close to the critical point and is at a temperature T 2 of 5.1 K, which corresponds to a pressure of 2.1 bar.
  • Point (b) is where the maximum liquefaction efficiency occurs and normally the system is maintained at point (b) until the volume of the interior tank is completely filled with liquid helium. At point (b), the liquefaction rate is about 65 liters/day (260 g/hr), which is equivalent to 50 liters/day at 1.0 bar.
  • the trajectory shown joining point (a) to point (b) is one the most efficient paths to follow between these two points while maintaining quasi-equilibrium conditions.
  • Point (c) is at about 4.2 K (T 2 ) at atmospheric pressure, the pressure that the system is normally returned to before transferring liquid out of the Dewar and into scientific or medical equipment.
  • the trajectory shown joining point (b) and point (c) is one of the most efficient trajectories taken between these two points. Not only is the pressure being decreased in the interior tank, but since the density of liquid increases between these two points, the volume of the liquid contracts and therefore liquefaction must continue along this trajectory to keep the interior tank filled with liquid when it reaches point (c).
  • the gas liquefaction system can also operate over a much wider range than the trajectory defined by points (a), (b), and (c).
  • An example of the total working area of the liquefier is depicted as an area enclosed by dashed lines in Fig. 2 .
  • the lower left region of this working area includes the liquefaction of helium gas for pressures less than 1 atmosphere, where T 2 , the temperature of the coldest end of the second stage, is under 4.2K and the liquefaction rates in turn are about 17 liters/day. This region is appropriate for MRI equipment and other equipment that must operate under these conditions.
  • T 2 the temperature of the coldest end of the second stage
  • the liquefaction rates in turn are about 17 liters/day.
  • This region is appropriate for MRI equipment and other equipment that must operate under these conditions.
  • the liquefier can operate above the critical point, where it fills the interior tank only with dense helium gas.
  • Other efficient trajectories include, for example, the case where
  • Fig. 3 illustrates a schematic of the general gas liquefaction system 1 according to various embodiments of the invention.
  • the system is supplied primarily with gas through gas intake module 2, preferably with recovered gas, of 99% purity or higher in the case of helium, although it can operate with lower purity grades if necessary.
  • the system of Fig. 3 illustrates two helium gas sources 25, a first source is directly connected to the gas intake module, and a second source further comprises buffer storage tank 24 for operation with sensitive MRI and other equipment.
  • the gas is liquefied in interior tank 9 of thermally isolated vacuum flask or container 8, such as a Dewar or a thermos container.
  • the liquefaction process comprises controlling the gas pressure in the interior tank, while the gas is cooled and condensed by one or more cryocooler coldheads 18 comprised of closed-cycle cryocoolers of one or more stages, placed in one or more necks 20 of the interior tank of the isolated container.
  • cryocooler coldhead 18 has two cold stages defined by a step pattern, with the cylindrical diameter of first stage 10 being larger than the diameter of second stage 11.
  • the high thermal conductivity of the gas and the convection currents generated by thermal gradients in the direction of the gravity force provides extremely efficient heat exchange between the two stages of the coldhead and the gas, and eliminates the need for mechanical heat exchangers, condensers, and radiation screens.
  • Convection currents are of importance only during the first cool down, since after the bottom of interior tank 9 becomes cooled, helium is stratified in temperature and the gradient is always opposite to the gravity force.
  • Temperature sensors are used to measure the vapor temperature T S1 at the lower end of first stage 10, the vapor temperature T S2 at the lower end of second stage 11, and the vapor or liquid temperature T S3 at the bottom of interior tank 9. After condensing, the liquid descends into and fills the storage portion of the interior tank. The liquid is transferred out of the interior tank, either manually or automatically, via transfer valve or port 6 when needed.
  • Means of connection 17 on the coldhead are used to connect to refrigeration compressor 22, via which compressed gas is supplied to and returned from coldhead 18 via compressor hoses 21 and electrical power via compressor power cable 22A.
  • Gas pressure control mechanism 19 maintains control over the input flow of the gas to control the pressure inside interior tank 9.
  • the gas pressure control mechanism measures the pressure of the interior tank using pressure sensor 7 and controls the flow rate of the gas going to the container using input valve 3 (preferably a solenoid valve), pressure regulator 4, and various flow-control input valves, preferably electronic solenoid valves or manual valves 12, 13, 14, 15, 16.
  • Gas mass flow meter 5 measures the instantaneous flow rate, which is modulated by gas pressure regulator 4 as it controls the pressure.
  • the integrated gas flow, pressure, and temperature are used to calculate the total amount of gas as well as the level of liquid accumulated within the interior tank of isolated container 9.
  • Gas pressure control mechanism 19 can halt the gas input if the pressure of the helium supply is insufficient, and can switch the system into stand-by mode to maintain the mass of the liquefied gas.
  • the mass flow of the gas going to the isolated container, and consequently the liquefaction rate, will increase as the power available for condensation on last stage 11 of coldhead 18 of the cryocooler increases. Since helium is stratified with the same temperature profile as the coldhead, thermal exchange between the gas and the coldhead is optimal.
  • Computer control device 23 comprising at least a computer equipped with programmed software/hardware and a monitor, controls the performance of the system by means of gas pressure control mechanism 19, refrigeration coldhead 18, cryocooler compressor 22, temperature sensors, and optional level indicators inside the interior tank.
  • the liquefaction process comprises introducing into interior tank 9 the mass of gas equivalent to 100% of its volume and maintaining it as close as possible to atmospheric pressure or to the pressure of the chosen application for the liquid in the shortest possible time.
  • the maximum power must be extracted from the gas by the coldhead of the cryocooler 18 during the entire process. This is to say, the trajectory that the process describes on the cryocooler coldhead load map is ideally the most efficient one.
  • gas liquefaction system 1 is configured for the recovery of helium in MRI machines.
  • the gas recovery system may include an additional manual safety valve that is located between the MRI machine and small buffer storage tank 24, preferably metallic, which is placed immediately before the entry of gases.
  • the function of such a buffer storage tank or external container is to establish a small gas reserve in which the pressure can be adjusted to perform at or near atmospheric pressures, always within the specific range of the MRI machines.
  • vertical access port 6 can be located on one of the sides of the top part of the Dewar for transferring the liquid helium from the liquefier to the scientific or medical MRI equipment. This can either be configured to insert a simple transfer tube, or it may be configured with a cryogenic valve.
  • the condensation process of the cold vapor accumulating as liquid in interior tank 9 corresponds to an isobaric process during which any disturbance in pressure yields a diminished liquefaction rate.
  • gas liquefaction system 1 it is therefore necessary to perform precise pressure control of interior tank 9 using electronic control of the diverse gas pressure control mechanism 19, and maintain the control throughout the entire process.
  • the standby mode can also be used to clean the surfaces of the coldhead and to restore efficiency.
  • the temperatures of the first stage and the second stage are set high enough to produce fusion and sublimation of any impurities, the system undergoes a process of regeneration, or cleaning, without loss of gas.
  • the liquefaction rate increases again to values characteristic of liquefying high purity gas.
  • the same purge or regeneration effect is reproduced, due to the temperature increase (over 100 K) of both the first stage and the second stage of the refrigeration coldhead.
  • Figs. 4 and 5 further illustrate a system for liquefaction of cryogen according to various embodiments of the invention.
  • System 101 includes vacuum isolated container 102 having storage portion or tank 103 and neck portion 104 extending from the storage portion, a coldhead cryocooler 105 at least partially received within the neck portion, and liquefaction region 106 defined by a volume of space generally disposed between the storage portion and neck portion adjacent to the coldhead as is further depicted by the dashed area of Fig. 5 .
  • the coldhead includes N coldhead stages represented as first stage 107, second stage 108, third stage 109, and Nth stage 110.
  • the neck portion is a straight neck. However as noted by dashed lines in Fig.
  • the neck can optionally be adapted to geometrically conform to the surface of the coldhead stages.
  • Cooling gas convection paths 111 are further depicted in Fig. 4 .
  • the system is adapted for improved liquefaction of cryogen by controlling pressure within the liquefaction region of the cryostat.
  • Pressure control mechanism 114 includes electronic pressure controller 112 and mass flow meter 113 for controlling input gas flowing into the cryostat such that pressure within the liquefaction region is optimized for improved liquefaction.
  • Extraction port 115 provides access to the liquefied cryogen.
  • a method for improved liquefaction of cryogen such as helium, includes:

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Mechanical Engineering (AREA)
  • Thermal Sciences (AREA)
  • General Engineering & Computer Science (AREA)
  • Health & Medical Sciences (AREA)
  • Clinical Laboratory Science (AREA)
  • Filling Or Discharging Of Gas Storage Vessels (AREA)
  • Separation By Low-Temperature Treatments (AREA)
EP11720246.5A 2010-05-03 2011-05-02 Gas liquefaction system and method Active EP2567159B1 (en)

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ES201030658 2010-05-03
PCT/US2011/034842 WO2011139989A2 (en) 2010-05-03 2011-05-02 Gas liquefaction system and method

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JP2013144099A (ja) * 2011-12-12 2013-07-25 Toshiba Corp 磁気共鳴イメージング装置
CN102997614A (zh) * 2012-12-04 2013-03-27 安徽万瑞冷电科技有限公司 小型氦液化装置
US10060655B2 (en) * 2014-08-11 2018-08-28 Raytheon Company Temperature control of multi-stage cryocooler with load shifting capabilities
US10788244B2 (en) * 2016-02-01 2020-09-29 Medtronic Cryocath Lp Recovery system for N20
JP7071255B2 (ja) * 2016-03-30 2022-05-18 住友重機械工業株式会社 超伝導マグネット装置及び極低温冷凍機システム
CA2969978C (en) * 2016-06-24 2019-07-02 Universidad De Zaragoza System and method for improving the liquefaction rate in cryocooler- based cryogen gas liquefiers
JP6123041B1 (ja) * 2017-01-04 2017-04-26 株式会社日立製作所 磁気共鳴イメージング装置、クライオシステムの制御装置、および、クライオシステムの制御方法
EP3569951A1 (en) 2018-05-17 2019-11-20 Universidad De Zaragoza Cryocooler suitable for gas liquefaction applications, gas liquefaction system and method comprising the same
CN110195822B (zh) * 2019-06-21 2021-04-02 江苏准信化学工程有限公司 一种自动控制氯气液化效率的装置及方法
CN112600067A (zh) * 2020-12-04 2021-04-02 江苏大学 用于变功率低温激光器高效散热的开式液氮喷雾冷却系统
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WO2022248255A1 (de) 2021-05-27 2022-12-01 Bruker Switzerland Ag Vorrichtung zur reinigung und verflüssigung von helium und zugehöriges verfahren
DE102021205423B4 (de) 2021-05-27 2023-09-21 Bruker Switzerland Ag Vorrichtung zur Reinigung und Verflüssigung von Helium und zugehöriges Verfahren

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CN102971593B (zh) 2015-12-16
ES2617357T3 (es) 2017-06-16
JP5891221B2 (ja) 2016-03-22
CN102971593A (zh) 2013-03-13
WO2011139989A2 (en) 2011-11-10
JP2013531773A (ja) 2013-08-08
WO2011139989A3 (en) 2012-01-05

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