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WO2012123690A2 - Method and apparatus for the liquefaction of co2 - Google Patents

Method and apparatus for the liquefaction of co2 Download PDF

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Publication number
WO2012123690A2
WO2012123690A2 PCT/FR2012/050562 FR2012050562W WO2012123690A2 WO 2012123690 A2 WO2012123690 A2 WO 2012123690A2 FR 2012050562 W FR2012050562 W FR 2012050562W WO 2012123690 A2 WO2012123690 A2 WO 2012123690A2
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WO
WIPO (PCT)
Prior art keywords
liquid
pressure
gas
fraction
cycle
Prior art date
Application number
PCT/FR2012/050562
Other languages
French (fr)
Other versions
WO2012123690A3 (en
Inventor
Olivier De Cayeux
Arthur Darde
Hervé Le Bihan
Xavier Traversac
Original Assignee
L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude
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 L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude filed Critical L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude
Priority to CA2828179A priority Critical patent/CA2828179C/en
Priority to CN201280013148.8A priority patent/CN103797321A/en
Priority to EP12714804.7A priority patent/EP2791602A2/en
Priority to US14/003,531 priority patent/US20130340472A1/en
Publication of WO2012123690A2 publication Critical patent/WO2012123690A2/en
Publication of WO2012123690A3 publication Critical patent/WO2012123690A3/en

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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • 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
    • F25J1/0027—Oxides of carbon, e.g. CO2
    • 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
    • F25J1/003—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production
    • F25J1/0032—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production using the feed stream itself or separated fractions from it, i.e. "internal refrigeration"
    • F25J1/004—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production using the feed stream itself or separated fractions from it, i.e. "internal refrigeration" by flash gas recovery
    • 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
    • F25J1/003—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production
    • F25J1/0032—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production using the feed stream itself or separated fractions from it, i.e. "internal refrigeration"
    • F25J1/0042—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production using the feed stream itself or separated fractions from it, i.e. "internal refrigeration" by liquid expansion with extraction of work
    • 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
    • F25J1/003—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production
    • F25J1/0032—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production using the feed stream itself or separated fractions from it, i.e. "internal refrigeration"
    • F25J1/0045—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the kind of cold generation within the liquefaction unit for compensating heat leaks and liquid production using the feed stream itself or separated fractions from it, i.e. "internal refrigeration" by vaporising a liquid return 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
    • 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
    • F25J1/0201—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 only internal refrigeration means, i.e. without external refrigeration
    • F25J1/0202—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 only internal refrigeration means, i.e. without external refrigeration in a quasi-closed internal refrigeration 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
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/06—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation
    • F25J3/0605—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation characterised by the feed stream
    • F25J3/0625—H2/CO mixtures, i.e. synthesis gas; Water gas or shifted synthesis gas
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/06—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation
    • F25J3/063—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation characterised by the separated product stream
    • F25J3/067—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation characterised by the separated product stream separation of carbon dioxide
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2210/00—Processes characterised by the type or other details of the feed stream
    • F25J2210/02—Multiple feed streams, e.g. originating from different sources
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2210/00—Processes characterised by the type or other details of the feed stream
    • F25J2210/70—Flue or combustion exhaust gas
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2220/00—Processes or apparatus involving steps for the removal of impurities
    • F25J2220/80—Separating impurities from carbon dioxide, e.g. H2O or water-soluble contaminants
    • F25J2220/82—Separating low boiling, i.e. more volatile components, e.g. He, H2, CO, Air gases, CH4
    • 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
    • F25J2230/00—Processes or apparatus involving steps for increasing the pressure of gaseous process streams
    • F25J2230/42—Processes or apparatus involving steps for increasing the pressure of gaseous process streams the fluid being nitrogen
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2235/00—Processes or apparatus involving steps for increasing the pressure or for conveying of liquid process streams
    • F25J2235/80—Processes or apparatus involving steps for increasing the pressure or for conveying of liquid process streams the fluid being carbon dioxide
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2240/00—Processes or apparatus involving steps for expanding of process streams
    • F25J2240/30—Dynamic liquid or hydraulic expansion with extraction of work, e.g. single phase or two-phase turbine
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2245/00—Processes or apparatus involving steps for recycling of process streams
    • F25J2245/02—Recycle of a stream in general, e.g. a by-pass stream
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2260/00—Coupling of processes or apparatus to other units; Integrated schemes
    • F25J2260/80—Integration in an installation using carbon dioxide, e.g. for EOR, sequestration, refrigeration etc.
    • 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
    • F25J2270/80—Quasi-closed internal or closed external carbon dioxide refrigeration cycle
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2

Definitions

  • the present invention relates to a method and apparatus for liquefying CO 2 .
  • An industrial route envisaged for the transport of CO2 is that of transport by boats, requiring the liquefaction of CO2, for example from different sources: coal-fired power plants, iron and steel units, SMR, gasification processes, etc.
  • This liquefaction may be preceded by one or more treatments of the fumes (or synthesis gas) by physical and / or chemical separation methods.
  • US-A-4699642 discloses a method for liquefying a CO2-rich gas according to the preamble of claim 1.
  • the cycle liquid vaporizes at a pressure substantially equal to that of the gas to be liquefied.
  • the invention provides optimized schemes for the liquefaction of CO2 and optionally the conditioning of CO2 for pipeline transport from one or more sources, minimizing CO2 losses as well as the specific energy related to purification and liquefaction CO2.
  • the impure CO2 from one or more sources is compressed via the cycle compressor to the desired pressure to condense the CO2 at ambient temperature (or against an intermediate cold fluid).
  • Part of this CO2 can be directly compressed at a pressure sufficient for the transport of CO2 by pipeline, another part of the CO2 can be used in the cold box.
  • the liquid CO2 sent into the cold box potentially has two uses: one part can be purified for the production of liquid CO2, the other ensures the refrigeration balance by expansion of the liquid CO2.
  • the unit may also include the following technological bricks:
  • This arrangement thus allows a reliable use of the liquefier even if one of the sources of CO2 is lost.
  • the gas from this source is preferably chosen for the production of liquid CO2.
  • the cycle liquid vaporizes at two different pressures, each lower than the first pressure.
  • the liquid derived from the cycle liquid is derived by separation in a phase separator to produce a gaseous fraction and a liquid fraction, the liquid fraction constituting the liquid derived from the cycle liquid.
  • the vaporized cycle liquid in the exchanger has the same composition as the liquid or supercritical flow cooled in the exchanger
  • the fraction of the liquid or supercritical flow is not cooled in the heat exchanger and serves as a product.
  • a second feed gas is purified in the separation means or at least one of the separation means, without being compressed with the first feed gas.
  • At least a fraction of the cycle gas is vaporised at a lower pressure than the first pressure and compressed to the first pressure before being mixed with the first feed gas.
  • the auxiliary fraction and / or the second feed gas is / are purified to form the liquid product or one of the liquid products by separation in at least one phase separator and / or at least one distillation column.
  • the feed gas mixed with the cycle gas at the second pressure is cooled upstream of the heat exchanger to provide the liquid or supercritical flow and the liquid or supercritical flow is then fed to the heat exchanger.
  • the feed gas at the second pressure is cooled upstream of the heat exchanger to form a single liquid or supercritical flow and no gas flow.
  • an apparatus for liquefying a gas containing at least 60 mol%. of CO2 to produce at least one liquid product comprising a heat exchanger, a compression means comprising at least two stages in series including a first stage and a second stage downstream of the first stage, a conduit for supplying a feed gas at the inlet of the second stage of the compression means to be compressed from a first pressure to a second pressure, means for cooling the gas at the second pressure to form a liquid or supercritical flow, optionally a pipe to bring a part of the liquid or supercritical flow to serve as a product without passing through the heat exchanger, a pipe for causing at least a portion of the liquid or supercritical flow to cool in the exchanger to form a cycle liquid at the second pressure, at the least a pipe to send at least a fraction of the liquid to vaporize in the exchanger, in the case where several fractions vaporize there mo yen
  • At least one said pipe for sending a gas formed by vaporization to the compression means is connected to a point of the compression means upstream of the inlet of the first feed gas in the compression means.
  • the apparatus comprises a cold box containing the exchanger and means for expanding a liquid to be vaporized in the exchanger, and means for treating the auxiliary fraction of the cycle liquid, constituted by at least one phase separator and / or at least one distillation column.
  • the apparatus comprises a pipe for sending a second feed gas to the processing means without having been compressed in the compression means.
  • the condu ite to send a second feed gas to the treatment means is connected to the exchanger.
  • the exchanger is constituted by a single exchange body
  • the apparatus does not include means for enriching the CO2 cycle liquid before dividing it.
  • the apparatus comprises a plate brazed aluminum heat exchanger E1, a pump 42, a four-stage compressor C1, C2, C3, C4 and a series of phase separators P1, P2, P3.
  • phase separators, the heat exchanger and the expansion valves are in a cold box.
  • a mixture of gases from three different sources is liquefied to form a supercritical CO2 flow and purified to form a pure liquid flow of CO2.
  • the gas 1 containing at least 60 mol%. of CO2, or even at least 90 mol%. of CO2 or possibly at least 95 mol%. of CO2 and at least one other gas, which may be for example nitrogen, methane, carbon monoxide is to be liquefied.
  • the gas contains 99% of CO2, and 1% of nitrogen.
  • the gas 1 at a first pressure is mixed with the gases 1A, 1B and the mixture formed is sent to the third stage C3 of a four-stage compressor.
  • the gas is cooled by the cooler R3, compressed in the fourth stage C4 to a second pressure above the critical pressure, for example 83 bar abs and then cooled in the exchangers E3, E4 to form a supercritical fluid.
  • a portion 40 of the fluid is not sent to the heat exchanger E1 but is pressurized by the pump 42 to a pressure of 1 50 bar to form a product, for example to be sent in a pipe.
  • the remainder of the fluid or the fluid at the outlet pressure of stage C4 is cooled to about -50 ° C in exchanger E1 to form a cycle liquid, since it is no longer supercritical.
  • the liquid is divided into possibly five fractions.
  • a fraction at very high pressure 4 is expanded in the valve 6, vaporized in the exchanger E1 and sent to the third stage C4 of the compressor.
  • a high pressure fraction 5 is expanded in the valve 15, vaporized in the exchanger E1 and sent to the third stage C3 of the compressor.
  • a medium-pressure fraction 7 is expanded in a vaporized valve in the exchanger E1 and sent to the inlet of the second stage C2 of the compressor.
  • a low-pressure fraction is expanded in a valve 43 at 6.9 bar a and sent to a phase separator 35.
  • This low-pressure fraction will be at 5.6 bar abs, if the nitrogen concentration is reduced to about 100 ppm, the factor limiting the pressure drop is the temperature: it must be avoided that this fluid is too cold (for example -54.5 ° C) to prevent it from approaching the temperature at which the CO 2 will freeze .
  • Only the vaporization of a flow rate in the exchanger is required, for example the vaporization of the low-pressure fraction. This being the case, multi-pressure vaporization improves exchange and reduces energy consumption.
  • the formed liquid 39 and the formed gas 37 are vaporized and heated in the exchanger E1, mixed and sent to the inlet of the first stage C1 of the compressor.
  • the remainder of the liquid 13 is expanded in a valve 19 (or a liquid turbine), without passing through the exchanger E1, and sent to a phase separator P1.
  • a phase separator In the phase separator, it forms a liquid 23 and a gas 21.
  • the liquid 23 is heated in the exchanger and then sent to the third phase separator P3.
  • the liquid of this separator is the carbon dioxide-rich product of the apparatus at -50 ° C and 7 bar abs.
  • the gases of the separators P1 and P3 are mixed, cooled in the exchanger E1, compressed by a compressor C5, for example at 20 bar, cooled in a cooler 31 and then partially condensed in the exchanger E1 and sent to the second phase separator P2.
  • the gas 33 of this separator contains 39% of carbon dioxide and 61% of nitrogen and is heated in the exchanger E1.
  • the liquid is reheated in the exchanger as flow 36 and then mixed with fraction 13 sent to separator P1.
  • the process does not necessarily include the treatment of the fraction 13 or the gaseous phases of pots P1 and P3 and therefore that these gaseous fractions can simply be returned to the compressor after reheating in the exchanger E1.
  • the liquid 20 and / or the liquids 22 or 25 constitute (s) one of the liquid products of the process. It is also possible to treat the fraction 13 by distillation to produce a liquid product rich in carbon dioxide or to treat it simply to remove a gaseous part.
  • the cooled liquid flow rate in the exchanger E1 is divided into four parts 4, 5, 7 and 41 which are then reheated in the exchanger E1 to be sent to the compressor C1, C2, C3, C4, in addition to the flow rates for liquid production.
  • liquid from the P3 phase separator may be the only one or one of the products.
  • At least one of the phase separator P1, P3 can be replaced by a distillation column.

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

Abstract

In a method for the liquefaction of a gas containing at least 60 mol % of CO2, in order to produce at least one liquid product, a first feed gas is compressed from a first pressure to a second pressure and cooled so as to form a liquid or supercritical flow, at least part of the liquid or supercritical flow is cooled in a heat exchanger (E1) in order to form a cyclic liquid at the second pressure, the cyclic liquid is divided into at least two fractions, including an auxiliary fraction, at least one fraction being vaporised in the exchanger by means of heat exchange with the liquid or supercritical flow part, and where there are at least two fractions, each one is vaporised at a different pressure, and the at least one gas formed is then compressed and mixed with the first feed gas, the auxiliary fraction (13) either forming the liquid product or one of the liquid products, or being treated by separation at a sub-ambient temperature in at least one separating means (P1,P3) in order to form the liquid product.

Description

Procédé et appareil de liquéfaction de CO2  Process and apparatus for liquefying CO2
La présente invention est relative à un procédé et appareil de liquéfaction de CO2. The present invention relates to a method and apparatus for liquefying CO 2 .
Une voie industrielle envisagée pour le transport du CO2 est celle du transport par bateaux, nécessitant la liquéfaction du CO2, par exemple issu de différentes sources : gaz de centrales à charbon, d'unités sidérurgiques, de SMR, de procédés de gazéification, etc.  An industrial route envisaged for the transport of CO2 is that of transport by boats, requiring the liquefaction of CO2, for example from different sources: coal-fired power plants, iron and steel units, SMR, gasification processes, etc.
Il est parfois nécessaire de transporter le CO2 par canalisation à des pressions supercritiques et pour cela, le liquide à transporter doit être pressurisé à des pressions élevées.  It is sometimes necessary to transport the CO2 by pipeline to supercritical pressures and for this, the liquid to be transported must be pressurized at high pressures.
Cette liquéfaction peut être précédée d'un ou plusieurs traitements des fumées (ou gaz de synthèse) par des méthodes de séparation physique et/ou chimique.  This liquefaction may be preceded by one or more treatments of the fumes (or synthesis gas) by physical and / or chemical separation methods.
US-A-4699642 décrit un procédé de liquéfaction d'un gaz riche en CO2 selon le préambule de la revendication 1 .  US-A-4699642 discloses a method for liquefying a CO2-rich gas according to the preamble of claim 1.
Dans ce procédé, le liquide de cycle se vaporise à une pression substantiellement égale à celle du gaz à liquéfier.  In this process, the cycle liquid vaporizes at a pressure substantially equal to that of the gas to be liquefied.
L'invention propose des schémas optimisés pour la liquéfaction du CO2 et éventuellement le conditionnement du CO2 pour transport par canalisation à partir d'une ou plusieurs sources, minimisant les pertes de CO2 ainsi que l'énergie spécifique liée à la purification et à la liquéfaction du CO2.  The invention provides optimized schemes for the liquefaction of CO2 and optionally the conditioning of CO2 for pipeline transport from one or more sources, minimizing CO2 losses as well as the specific energy related to purification and liquefaction CO2.
Selon l'invention, le CO2 impur issu d'une ou plusieurs sources est comprimé via le compresseur de cycle à la pression désirée pour condenser le CO2 à température ambiante (ou contre un fluide froid intermédiaire). Une partie de ce CO2 peut être directement comprimée à une pression suffisante pour le transport du CO2 par canalisation, une autre partie du CO2 peut être utilisée dans la boite froide. Le CO2 liquide envoyé dans la boite froide a potentiellement deux utilités : une partie peut être purifiée pour la production de CO2 liquide, l'autre assure le bilan frigorifique par détente du CO2 liquide. L'unité peut également comporter les briques technologiques suivantes :  According to the invention, the impure CO2 from one or more sources is compressed via the cycle compressor to the desired pressure to condense the CO2 at ambient temperature (or against an intermediate cold fluid). Part of this CO2 can be directly compressed at a pressure sufficient for the transport of CO2 by pipeline, another part of the CO2 can be used in the cold box. The liquid CO2 sent into the cold box potentially has two uses: one part can be purified for the production of liquid CO2, the other ensures the refrigeration balance by expansion of the liquid CO2. The unit may also include the following technological bricks:
• Séchage du gaz par adsorption en amont du compresseur. • Elimination ou réduction des impuretés telles que le Hg par adsorption, NOx via une colonne de distillation. • Adsorption gas drying upstream of the compressor. • Elimination or reduction of impurities such as Hg by adsorption, NOx via a distillation column.
• Purification du CO2 via une colonne de distillation.  • Purification of CO2 via a distillation column.
• Amélioration du rendement CO2 via une compression intermédiaire dans la boite froide.  • Improved CO2 efficiency via intermediate compression in the cold box.
Cet arrangement permet ainsi une utilisation fiable du liquéfacteur même si une des sources de CO2 est perdue.  This arrangement thus allows a reliable use of the liquefier even if one of the sources of CO2 is lost.
Si au moins une source de CO2 impur est à la bonne pression pour la liquéfaction du CO2, le gaz de cette source est préférentiellement choisi pour la production de CO2 liquide.  If at least one source of impure CO2 is at the right pressure for the liquefaction of CO2, the gas from this source is preferably chosen for the production of liquid CO2.
Eventuellement la compression du gaz de l'une des sources peut être nécessaire pour égaler au moins la pression du CO2 liquide produit.  Eventually compression of the gas from one of the sources may be necessary to equal at least the pressure of the liquid CO2 produced.
Il est connu de liquéfier un débit de CO2 en le comprimant et en le refroidissant selon JP-A-582081 17, EP-A-0646756 et SU-A-1479802.  It is known to liquefy a flow of CO2 by compressing it and cooling it according to JP-A-58208117, EP-A-0646756 and SU-A-1479802.
Selon un objet de l'invention, il est prévu un procédé de liquéfaction d'un gaz contenant au moins 60% mol. de CO2 , voire au moins 80% de CO2, pour produire au moins un produit liquide dans lequel un gaz d'alimentation est comprimé depuis une première pression jusqu'à une deuxième pression et refroidi pour former un débit liquide ou supercritique, au moins une partie du débit liquide ou supercritique est refroidie dans un échangeur de chaleur pour former un liquide de cycle à la deuxième pression, le liquide de cycle ou un liquide dérivé du liquide de cycle est divisé en au moins deux fractions y compris une fraction auxiliaire, au moins une fraction étant vaporisée dans l'échangeur par échange de chaleur avec la partie du débit liquide ou supercritique, la au moins une fraction étant vaporisée, et pour le cas où il y a au moins deux fractions chacune est vaporisée à une pression différente, et le ou les gaz formés étant ensuite comprimé(s) et mélangé(s) avec le premier gaz d'alimentation, la fraction auxiliaire soit constituant le produit liquide ou un des produits liquides soit étant traitée par séparation à température subambiante dans au moins un moyen de séparation pour former le produit liquide ou un des produits liquides caractérisé en ce que le gaz d'alimentation est comprimé depuis la première pression jusqu'à la deuxième pression après avoir été mélangé avec au moins un gaz formé par vaporisation du liquide de cycle, le gaz formé par vaporisation ayant été comprimé depuis sa pression de vaporisation jusqu'à la première pression sans avoir été mélangé avec le premier gaz. According to one object of the invention, there is provided a method of liquefying a gas containing at least 60 mol%. of CO2, or even at least 80% CO2, to produce at least one liquid product in which a feed gas is compressed from a first pressure to a second pressure and cooled to form a liquid or supercritical flow, at least one part of the liquid or supercritical flow is cooled in a heat exchanger to form a cycle liquid at the second pressure, the cycle liquid or a liquid derived from the cycle liquid is divided into at least two fractions including an auxiliary fraction, at at least one fraction being vaporized in the exchanger by heat exchange with the part of the liquid or supercritical flow, the at least one fraction being vaporized, and for the case where there are at least two fractions each is vaporized at a different pressure, and the formed gas (s) being then compressed (s) and mixed with the first feed gas, the auxiliary fraction constituting the liquid product or one of the products its liquids either being treated by separation at subambient temperature in at least one separation means to form the liquid product or one of the liquid products characterized in that the feed gas is compressed from the first pressure to the second pressure after having mixed with at least one gas formed by vaporization of the cycle liquid, the vaporized gas having been compressed from its vaporization until the first pressure without having been mixed with the first gas.
Ainsi le liquide de cycle se vaporise à une pression plus basse que la première pression.  Thus the cycle liquid vaporizes at a lower pressure than the first pressure.
De préférence le liquide de cycle se vaporise à deux pressions différentes, chacune plus basse que la première pression.  Preferably the cycle liquid vaporizes at two different pressures, each lower than the first pressure.
Eventuellement :  Eventually :
le liquide dérivé du liquide de cycle est dérivé par séparation dans un séparateur de phases pour produire une fraction gazeuse et une fraction liquide, la fraction liquide constituant le liquide dérivé du liquide de cycle.  the liquid derived from the cycle liquid is derived by separation in a phase separator to produce a gaseous fraction and a liquid fraction, the liquid fraction constituting the liquid derived from the cycle liquid.
le liquide de cycle vaporisé dans l'échangeur a la même composition que le débit liquide ou supercritique refroidi dans l'échangeur  the vaporized cycle liquid in the exchanger has the same composition as the liquid or supercritical flow cooled in the exchanger
la fraction du débit liquide ou supercritique n'est pas refroidie dans l'échangeur de chaleur et sert de produit.  the fraction of the liquid or supercritical flow is not cooled in the heat exchanger and serves as a product.
un deuxième gaz d'alimentation est épuré dans le moyen de séparation ou au moins un des moyen de séparation, sans avoir été comprimé avec le premier gaz d'alimentation.  a second feed gas is purified in the separation means or at least one of the separation means, without being compressed with the first feed gas.
au moins une fraction du gaz de cycle est vaporisée à une pression inférieure à la première pression et comprimé jusqu'à la première pression avant d'être mélangé au premier gaz d'alimentation.  at least a fraction of the cycle gas is vaporised at a lower pressure than the first pressure and compressed to the first pressure before being mixed with the first feed gas.
la fraction auxiliaire et/ou le deuxième gaz d'alimentation est/sont épuré(s) pour former le produit liquide ou un des produits liquides par séparation dans au moins un séparateur de phases et/ou au moins une colonne de distillation.  the auxiliary fraction and / or the second feed gas is / are purified to form the liquid product or one of the liquid products by separation in at least one phase separator and / or at least one distillation column.
le gaz d'alimentation mélangé au gaz de cycle à la deuxième pression est refroidi en amont de l'échangeur de chaleur pour fournir le débit liquide ou supercritique et le débit liquide ou supercritique est ensuite envoyé à l'échangeur de chaleur.  the feed gas mixed with the cycle gas at the second pressure is cooled upstream of the heat exchanger to provide the liquid or supercritical flow and the liquid or supercritical flow is then fed to the heat exchanger.
le gaz d'alimentation à la deuxième pression est refroidi en amont de l'échangeur de chaleur pour former un seul débit liquide ou supercritique et aucun débit gazeux.  the feed gas at the second pressure is cooled upstream of the heat exchanger to form a single liquid or supercritical flow and no gas flow.
le débit liquide ou supercritique est sous-refroidi dans l'échangeur (E1 ). Selon un autre objet de l'invention, il est prévu un appareil de liquéfaction d'un gaz contenant au moins 60% mol. de CO2 pour produire au moins un produit liquide, comprenant un échangeur de chaleur, un moyen de compression comprenant au moins deux étages en série dont un premier étage et un deuxième étage en aval du premier étage, une conduite pour envoyer un gaz d'alimentation à l'entrée du deuxième étage du moyen de compression pour être comprimé depuis une prem ière pression jusqu'à une deuxième pression, des moyens pour refroidir le gaz à la deuxième pression pour former un débit liquide ou supercritique, éventuellement une conduite pour amener une partie du débit liquide ou supercritique pour servir de produit sans passer par l'échangeur de chaleur, une conduite pour amener au moins une partie du débit liquide ou supercritique se refroidir dans l'échangeur pour former un liquide de cycle à la deuxième pression, au moins une conduite pour envoyer au moins une fraction du liquide se vaporiser dans l'échangeur, pour le cas où plusieurs fractions s'y vaporisent des moyens permettant de vaporiser les au moins deux fractions chacune à une pression différente, et au moins une conduite pour envoyer le(s) gaz formé(s) au moyen de compression et une conduite d'une fraction auxiliaire du liquide de cycle reliée à l'échangeur de chaleur pour transporter soit le ou un des produits liquides ou un liquide à traiter pour former le ou un des produits liquides caractérisé en ce que la conduite pour envoyer le gaz formé au moyen de compression est une conduite pour envoyer au moins un gaz formé à l'entrée du premier étage pour former un gaz comprimé, l'appareil comprenant une conduite pour envoyer le gaz comprimé dans le premier étage au deuxième étage. the liquid or supercritical flow rate is subcooled in the exchanger (E1). According to another object of the invention, there is provided an apparatus for liquefying a gas containing at least 60 mol%. of CO2 to produce at least one liquid product, comprising a heat exchanger, a compression means comprising at least two stages in series including a first stage and a second stage downstream of the first stage, a conduit for supplying a feed gas at the inlet of the second stage of the compression means to be compressed from a first pressure to a second pressure, means for cooling the gas at the second pressure to form a liquid or supercritical flow, optionally a pipe to bring a part of the liquid or supercritical flow to serve as a product without passing through the heat exchanger, a pipe for causing at least a portion of the liquid or supercritical flow to cool in the exchanger to form a cycle liquid at the second pressure, at the least a pipe to send at least a fraction of the liquid to vaporize in the exchanger, in the case where several fractions vaporize there mo yens for vaporizing the at least two fractions each at a different pressure, and at least one line for sending the gas (s) formed to the compression means and a conduit for an auxiliary fraction of the cycle liquid connected to the heat exchanger for conveying either the one or one of the liquid products or a liquid to be treated to form the or one of the liquid products characterized in that the pipe for sending the gas formed to the compression means is a pipe for sending at least one gas formed at the inlet of the first stage to form a compressed gas, the apparatus comprising a conduit for supplying the compressed gas in the first stage to the second stage.
Selon d'autres caractéristiques facultatives :  According to other optional features:
au moins une dite conduite pour envoyer un gaz formé par vaporisation au moyen de compression est reliée à un point du moyen de compression en amont de l'entrée du premier gaz d'alimentation dans le moyen de compression.  at least one said pipe for sending a gas formed by vaporization to the compression means is connected to a point of the compression means upstream of the inlet of the first feed gas in the compression means.
l'appareil comprend une boîte froide contenant l'échangeur et des moyens de détente d'un liquide à vaporiser dans l'échangeur, ainsi que des moyens de traitement de la fraction auxiliaire du liquide de cycle, constitués par au moins un séparateur de phase et/ou au moins une colonne de distillation. l'appareil comprend une conduite pour envoyer un deuxième gaz d'alimentation aux moyens de traitement sans avoir été comprimé dans les moyens de compression. the apparatus comprises a cold box containing the exchanger and means for expanding a liquid to be vaporized in the exchanger, and means for treating the auxiliary fraction of the cycle liquid, constituted by at least one phase separator and / or at least one distillation column. the apparatus comprises a pipe for sending a second feed gas to the processing means without having been compressed in the compression means.
la condu ite pour envoyer un deuxième gaz d'alimentation aux moyens de traitement est reliée à l'échangeur.  the condu ite to send a second feed gas to the treatment means is connected to the exchanger.
l'échangeur est constitué par un seul corps d'échange,  the exchanger is constituted by a single exchange body,
l'appareil ne comprend pas de moyen pour enrichir le liquide de cycle de CO2 avant de le diviser.  the apparatus does not include means for enriching the CO2 cycle liquid before dividing it.
L'invention sera décrite en plus de détail en se référant aux figures.  The invention will be described in more detail with reference to the figures.
Dans la Figure 1 , l'appareil comprend un échangeur de chaleur E1 en aluminium brasé à plaques, une pompe 42, un compresseur à quatre étages C1 , C2, C3, C4 et une série de séparateurs de phase P1 , P2, P3.  In Figure 1, the apparatus comprises a plate brazed aluminum heat exchanger E1, a pump 42, a four-stage compressor C1, C2, C3, C4 and a series of phase separators P1, P2, P3.
Les séparateurs de phase, l'échangeur de chaleur et les vannes de détente se trouvent dans une boîte froide.  The phase separators, the heat exchanger and the expansion valves are in a cold box.
Un mélange de gaz de trois sources différentes est liquéfié pour former un débit de CO2 supercritique et purifié pour former un débit liquide de CO2 pur.  A mixture of gases from three different sources is liquefied to form a supercritical CO2 flow and purified to form a pure liquid flow of CO2.
Le gaz 1 contenant au moins 60% mol. de CO2, voire au moins 90% mol. de CO2 ou éventuellement au moins 95% mol. de CO2 ainsi qu'au moins un autre gaz, pouvant être par exemple l'azote, le méthane, le monoxyde de carbone est à liquéfier. Dans cet exemple chiffré, le gaz contient 99% de CO2, et 1 % d'azote. Le gaz 1 à une première pression est mélangé avec les gaz 1A, 1 B et le mélange formé est envoyé au troisième étage C3 d'un compresseur à quatre étages. Le gaz est refroidi par le refroidisseur R3, comprimé dans le quatrième étage C4 jusqu'à une deuxième pression au-delà de la pression critique, par exemple 83 bars abs et puis refroidi dans les échangeurs E3, E4 pour former un fluide supercritique. Eventuellement une partie 40 du fluide n'est pas envoyée à l'échangeur de chaleur E1 mais est pressurisée par la pompe 42 jusqu'à une pression de 1 50 bars pour former un produit, par exemple à envoyer dans une canalisation. Le reste du fluide ou le fluide à la pression de sortie de l'étage C4 est refroidi jusqu'à environ -50°C dans l'échangeur E1 pour former un liquide de cycle, puisqu'il n'est plus supercritique. Le liquide est divisé en éventuellement cinq fractions. Une fraction à très haute pression 4 est détendue dans la vanne 6, vaporisée dans l'échangeur E1 et envoyée au troisième étage C4 du compresseur. Une fraction à haute pression 5 est détendue dans la vanne 15, vaporisée dans l'échangeur E1 et envoyée au troisième étage C3 du compresseur. Une fraction à moyenne pression 7 est détendue dans une vanne vaporisée dans l'échangeur E1 et envoyée à l'entrée du deuxième étage C2 du compresseur. Une fraction à basse pression est détendue dans une vanne 43 à 6,9 bars a et envoyée à un séparateur de phases 35. Cette fraction basse pression sera à 5,6 bars abs, si la concentration en azote est réduite à environ 100 ppm, le facteur limitant la baisse de pression est la température : il faut éviter que ce fluide ne soit trop froid (par exemple -54,5°C) pour éviter qu'il ne s'approche de la température à laquelle le CO2 va geler. Seule est nécessaire la vaporisation d'un débit dans l'échangeur, par exemple la vaporisation de la fraction à basse pression. Ceci étant, la vaporisation à plusieurs pressions permet d'améliorer l'échange et de réduire la consommation énergétique. Le liquide formé 39 et le gaz formé 37 sont vaporisé et réchauffés dans l'échangeur E1 , mélangés et envoyés à l'entrée du premier étage C1 du compresseur. The gas 1 containing at least 60 mol%. of CO2, or even at least 90 mol%. of CO2 or possibly at least 95 mol%. of CO2 and at least one other gas, which may be for example nitrogen, methane, carbon monoxide is to be liquefied. In this example, the gas contains 99% of CO2, and 1% of nitrogen. The gas 1 at a first pressure is mixed with the gases 1A, 1B and the mixture formed is sent to the third stage C3 of a four-stage compressor. The gas is cooled by the cooler R3, compressed in the fourth stage C4 to a second pressure above the critical pressure, for example 83 bar abs and then cooled in the exchangers E3, E4 to form a supercritical fluid. Optionally a portion 40 of the fluid is not sent to the heat exchanger E1 but is pressurized by the pump 42 to a pressure of 1 50 bar to form a product, for example to be sent in a pipe. The remainder of the fluid or the fluid at the outlet pressure of stage C4 is cooled to about -50 ° C in exchanger E1 to form a cycle liquid, since it is no longer supercritical. The liquid is divided into possibly five fractions. A fraction at very high pressure 4 is expanded in the valve 6, vaporized in the exchanger E1 and sent to the third stage C4 of the compressor. A high pressure fraction 5 is expanded in the valve 15, vaporized in the exchanger E1 and sent to the third stage C3 of the compressor. A medium-pressure fraction 7 is expanded in a vaporized valve in the exchanger E1 and sent to the inlet of the second stage C2 of the compressor. A low-pressure fraction is expanded in a valve 43 at 6.9 bar a and sent to a phase separator 35. This low-pressure fraction will be at 5.6 bar abs, if the nitrogen concentration is reduced to about 100 ppm, the factor limiting the pressure drop is the temperature: it must be avoided that this fluid is too cold (for example -54.5 ° C) to prevent it from approaching the temperature at which the CO 2 will freeze . Only the vaporization of a flow rate in the exchanger is required, for example the vaporization of the low-pressure fraction. This being the case, multi-pressure vaporization improves exchange and reduces energy consumption. The formed liquid 39 and the formed gas 37 are vaporized and heated in the exchanger E1, mixed and sent to the inlet of the first stage C1 of the compressor.
Le reste du liquide 13 est détendu dans une vanne 19 (ou une turbine liquide), sans passer par l'échangeur E1 , et envoyé à un séparateur de phases P1 . Dans le séparateur de phases, il forme un liquide 23 et un gaz 21 . Le liquide 23 est chauffé dans l'échangeur puis envoyé au troisième séparateur de phases P3. Le liquide de ce séparateur est le produit riche en dioxyde de carbone 25 de l'appareil, à -50°C et 7 bar abs. Les gaz des séparateurs P1 et P3 sont mélangés, refroidis dans l'échangeur E1 , comprimés par un compresseur C5, par exemple à 20 bars a, refroidis dans un refroidisseur 31 puis partiellement condensés dans l'échangeur E1 et envoyés au deuxième séparateur de phases P2. Le gaz 33 de ce séparateur contient 39% de dioxyde de carbone et 61 % d'azote et est réchauffé dans l'échangeur E1 . Le liquide est réchauffé dans l'échangeur comme débit 36 puis mélangé avec la fraction 13 envoyée au séparateur P1 .  The remainder of the liquid 13 is expanded in a valve 19 (or a liquid turbine), without passing through the exchanger E1, and sent to a phase separator P1. In the phase separator, it forms a liquid 23 and a gas 21. The liquid 23 is heated in the exchanger and then sent to the third phase separator P3. The liquid of this separator is the carbon dioxide-rich product of the apparatus at -50 ° C and 7 bar abs. The gases of the separators P1 and P3 are mixed, cooled in the exchanger E1, compressed by a compressor C5, for example at 20 bar, cooled in a cooler 31 and then partially condensed in the exchanger E1 and sent to the second phase separator P2. The gas 33 of this separator contains 39% of carbon dioxide and 61% of nitrogen and is heated in the exchanger E1. The liquid is reheated in the exchanger as flow 36 and then mixed with fraction 13 sent to separator P1.
Il est évident que le procédé ne comprend pas obligatoirement le traitement de la fraction 13 ou des phases gazeuses des pots P1 et P3 et donc que ces fractions gazeuses peuvent être simplement renvoyées au compresseur après réchauffage dans l'échangeur E1 . Dans ce cas, le liquide 20 et/ou les liquides 22 ou 25 constitue(nt) un des produits liquides du procédé. Il est également possible de traiter la fraction 13 par distillation pour produire un produit liquide riche en dioxyde de carbone ou de la traiter tout simplement pour enlever une partie gazeuse. It is obvious that the process does not necessarily include the treatment of the fraction 13 or the gaseous phases of pots P1 and P3 and therefore that these gaseous fractions can simply be returned to the compressor after reheating in the exchanger E1. In this case, the liquid 20 and / or the liquids 22 or 25 constitute (s) one of the liquid products of the process. It is also possible to treat the fraction 13 by distillation to produce a liquid product rich in carbon dioxide or to treat it simply to remove a gaseous part.
Selon la Figure 2, les éléments déjà décrits dans la Figure 1 ne seront pas décrits de nouveau. A la différence du procédé de la Figure 1 , une portion 1 du débit d'alimentation est déjà à une pression suffisamment élevée pour être sous-refroidi dans l'échangeur E1 . Deux débits 1A, 1 B à la première pression sont donc comprimés jusqu'à la deuxième pression en étant envoyés au troisième étage du compresseur, comme décrit précédemment et l'autre débit 1 à la deuxième pression est envoyé directement à l'échangeur E1 où il se sous- refroidit au moins partiellement avant d'être envoyé au séparateur de phases. Il sera apprécié que le débit 1 peut être le seul débit traité dans le séparateur de phases ou sinon qu'il peut être mélangé avec la fraction 13 après détente. Cette façon de procéder permet également de gérer le cas dans lequel le débit 1 et les débits 1 A, 1 B ont des puretés très différentes. Par exemple le débit 1 peut être envoyé soit au séparateur P1 , soit au séparateur P2, soit au séparateur P3 selon sa composition.  According to Figure 2, the elements already described in Figure 1 will not be described again. Unlike the method of Figure 1, a portion 1 of the feed rate is already at a sufficiently high pressure to be subcooled in the exchanger E1. Two flows 1A, 1B at the first pressure are compressed to the second pressure by being sent to the third stage of the compressor, as previously described and the other flow 1 at the second pressure is sent directly to the exchanger E1 where it sub-cools at least partially before being sent to the phase separator. It will be appreciated that flow 1 may be the only flow rate treated in the phase separator or else it may be mixed with fraction 13 after expansion. This way of proceeding also makes it possible to manage the case in which the flow 1 and the flows 1 A, 1 B have very different purities. For example, the flow rate 1 can be sent either to the separator P1 or to the separator P2 or to the separator P3 according to its composition.
Selon la Figure 3, autrement que dans la Figure 2, même si le débit 1 doit être comprimé dans un compresseur auxiliaire C6 pour atteindre la pression nécessaire, il est possible d'envoyer du gaz d'une source directement au traitement par épuration et d'autres gaz au cycle de liquéfaction de CO2. Cette façon de procéder permet également de gérer le cas dans lequel le débit 1 et les débits 1A, 1 B ont des puretés très différentes. Par exemple le débit 1 peut être envoyé soit au séparateur P1 , soit au séparateur P2, soit au séparateur P3 selon sa composition. According to Figure 3, other than in Figure 2, even if the flow 1 has to be compressed in an auxiliary compressor C6 to reach the required pressure, it is possible to send gas from a source directly to treatment by purification and other gases in the CO 2 liquefaction cycle. This way of proceeding also makes it possible to manage the case in which the flow 1 and the flows 1A, 1B have very different purities. For example, the flow rate 1 can be sent either to the separator P1 or to the separator P2 or to the separator P3 according to its composition.
Il sera noté que le débit liquide refroidi dans l'échangeur E1 est divisé en quatre parties 4, 5, 7 et 41 qui sont ensuite réchauffées dans l'échangeur E1 pour être envoyées au compresseur C1 , C2, C3, C4, en plus des débits destinés à la production liquide. Il y a donc autant de débits vaporisés chacun à une pression différente qu'il y a d'étages de compresseurs, chaque pression de vaporisation correspondant à une pression d'entrée d'étage de compresseur. Ceci correspond à un optimum et il est évidemment possible de ne vaporiser qu'un seul débit destiné au compresseur (par exemple celui à la pression la plus basse) ou moins de débits qu'il y a d'étages de compresseur. Selon les puretés désirées, il est possible de récupérer du liquide 20 provenant directement de l'échangeur E1 et de ne pas traiter le reste du liquide en séparateur de phases ou de le traiter, selon les besoins du client. It will be noted that the cooled liquid flow rate in the exchanger E1 is divided into four parts 4, 5, 7 and 41 which are then reheated in the exchanger E1 to be sent to the compressor C1, C2, C3, C4, in addition to the flow rates for liquid production. There are therefore as many vaporized flow rates each at a different pressure as there are compressor stages, each vaporization pressure corresponding to a compressor stage inlet pressure. This corresponds to an optimum and it is obviously possible to vaporize only one flow rate for the compressor (for example the one at the lowest pressure) or less flow rates than there are compressor stages. Depending on the purities desired, it is possible to recover liquid 20 directly from the exchanger E1 and not to treat the rest of the liquid phase separator or treat it, according to the needs of the customer.
Il est également possible de récupérer du liquide 22 à la sortie du séparateur de phases P1 comme seul produit ou comme un des produits.  It is also possible to recover liquid 22 at the outlet of the phase separator P1 as sole product or as one of the products.
Finalement le liquide 25 provenant du séparateur de phases P3 peut être le seul ou un des produits.  Finally, the liquid from the P3 phase separator may be the only one or one of the products.
Pour obtenir des produits plus purs, au moins un des séparateur de phases P1 , P3 peut être remplacé par une colonne de distillation.  To obtain purer products, at least one of the phase separator P1, P3 can be replaced by a distillation column.

Claims

Revendications claims
1 . Procédé de liquéfaction d'un gaz contenant au moins 60% mol. de CO2, voire au moins 80% de CO2, pour produire au moins un produit liquide dans lequel un gaz d'alimentation est comprimé depuis une première pression jusqu'à une deuxième pression et refroidi pour former un débit liquide ou supercritique, au moins une partie du débit liquide ou supercritique est refroidie dans un échangeur de chaleur (E1 ) pour former un l iquide de cycle à la deuxième pression, le liquide de cycle ou un liquide dérivé du liquide de cycle est divisé en au moins deux fractions y compris une fraction auxiliaire, au moins une fraction étant vaporisée dans l'échangeur par échange de chaleur avec la partie du débit liquide ou supercritique, et pour le cas où il y a au moins deux fractions chacune est vaporisée à une pression différente, et le ou les gaz formés étant ensuite comprimé(s) et mélangé(s) avec le premier gaz d'alimentation, la fraction auxiliaire (13) soit constituant le produit liquide ou un des produ its l iqu ides soit étant traitée par séparation à température subambiante dans au moins un moyen de séparation (P1 , P3) pour former le produit liquide ou un des produ its liquides caractérisé en ce que le gaz d'alimentation est comprimé depuis la première pression jusqu'à la deuxième pression après avoir été mélangé avec au moins un gaz formé par vaporisation du liquide de cycle, le gaz formé par vaporisation ayant été comprimé depuis sa pression de vaporisation jusqu'à la première pression sans avoir été mélangé avec le premier gaz. 1. Process for liquefying a gas containing at least 60 mol% of CO2, or even at least 80% CO2, to produce at least one liquid product in which a feed gas is compressed from a first pressure to a second pressure and cooled to form a liquid or supercritical flow, at least one part of the liquid or supercritical flow is cooled in a heat exchanger (E1) to form a cycle liquid at the second pressure, the cycle liquid or a liquid derived from the cycle liquid is divided into at least two fractions including a auxiliary fraction, at least a fraction being vaporized in the exchanger by heat exchange with the part of the liquid or supercritical flow, and for the case where there are at least two fractions each is vaporized at a different pressure, and the formed gases being then compressed and mixed with the first feed gas, the auxiliary fraction (13) constituting the liquid product or one of the liquefied products being either by separating at subambient temperature in at least one separating means (P1, P3) to form the liquid product or one of the liquid products characterized in that the feed gas is compressed from the first pressure to the second pressure after being mixed with at least one gas formed by vaporizing the cycle liquid, the vaporized gas having been compressed from its vaporization pressure to the first pressure without having been mixed with the first gas.
2. Procédé selon la revendication 1 dans lequel le liquide dérivé du liquide de cycle est dérivé par séparation dans un séparateur de phases pour produire une fraction gazeuse et une fraction liquide, la fraction liquide constituant le liquide dérivé du liquide de cycle. 2. The method of claim 1 wherein the liquid derived from the cycle liquid is derived by separation in a phase separator to produce a gaseous fraction and a liquid fraction, the liquid fraction constituting the liquid derived from the cycle liquid.
3. Procédé selon l'une des revendications précédentes dans lequel une fraction (42) du débit liquide ou supercritique n'est pas refroidie dans l'échangeur de chaleur et sert de produit. 3. Method according to one of the preceding claims wherein a fraction (42) of the liquid or supercritical flow is not cooled in the heat exchanger and serves as a product.
4. Procédé selon l'une des revendications précédentes dans lequel un deuxième gaz d'alimentation est épuré dans le moyen de séparation (P1 , P3) ou au moins un des moyen de séparation, sans avoir été comprimé avec le premier gaz d'alimentation. 4. Method according to one of the preceding claims wherein a second feed gas is purified in the separation means (P1, P3) or at least one of the separation means, without being compressed with the first feed gas .
5. Procédé selon l'une des revendications précédentes dans lequel au moins une fraction du gaz de cycle est vaporisée à une pression inférieure à la première pression et comprimé jusqu'à la première pression avant d'être mélangé au premier gaz d'alimentation. 5. Method according to one of the preceding claims wherein at least a fraction of the cycle gas is vaporized at a pressure lower than the first pressure and compressed to the first pressure before being mixed with the first feed gas.
6. Procédé selon l'une des revendications précédentes dans lequel la fraction auxiliaire et/ou le deuxième gaz d'alimentation sont épurés pour former le produit liquide ou un des produits liquides par séparation dans au moins un séparateur de phases et/ou au moins une colonne de distillation. 6. Method according to one of the preceding claims wherein the auxiliary fraction and / or the second feed gas are purified to form the liquid product or liquid products by separation in at least one phase separator and / or at least a distillation column.
7. Procédé selon l'une des revendications précédentes dans lequel le gaz d'alimentation mélangé au gaz de cycle (3) à la deuxième pression est refroidi en amont de l'échangeur de chaleur (E1 ) pour fournir le débit liquide ou supercritique et le débit liquide ou supercritique est ensuite envoyé à l'échangeur de chaleur. 7. Method according to one of the preceding claims wherein the feed gas mixed with the cycle gas (3) at the second pressure is cooled upstream of the heat exchanger (E1) to provide the liquid or supercritical flow and the liquid or supercritical flow is then sent to the heat exchanger.
8. Procédé selon la revendication 7 dans lequel le gaz d'alimentation mélangé au gaz de cycle (3) à la deuxième pression est refroidi en amont de l'échangeur de chaleur (E1 ) pour former un seul débit liquide ou supercritique et aucun débit gazeux. 8. The method of claim 7 wherein the feed gas mixed with the cycle gas (3) at the second pressure is cooled upstream of the heat exchanger (E1) to form a single liquid or supercritical flow and no flow gaseous.
9. Procédé selon l'une des revendications 7 ou 8 dans lequel le débit liquide ou supercritique est sous-refroidi dans l'échangeur (E1 ). 9. Method according to one of claims 7 or 8 wherein the liquid or supercritical flow is subcooled in the exchanger (E1).
10. Appareil de liquéfaction d'un gaz contenant au moins 60% mol. de CO2 pour produire au moins un produit liquide, comprenant un échangeur de chaleur (E1 ), un moyen de compression (C1 , C2, C3, C4) comprenant au moins deux étages en série dont un premier étage et un deuxième étage en aval du premier étage, une conduite pour envoyer un gaz d'alimentation à l'entrée du deuxième étage du moyen de compression pour être comprimé depuis une première pression jusqu'à une deuxième pression, des moyens pour refroidir le gaz à la deuxième pression pour former un débit liquide ou supercritique, éventuellement une conduite pour amener une partie du débit liquide ou supercritique pour servir de produit sans passer par l'échangeur de chaleur, une conduite pour amener au moins une partie du débit liquide ou supercritique se refroidir dans Γ échangeur pour former un liquide de cycle à la deuxième pression, au moins une conduite pour envoyer au moins une fraction du liquide se vaporiser dans l'échangeur, pour le cas où plusieurs fractions s'y vaporisent des moyens permettant de vaporiser les au moins deux fractions chacune à une pression différente, et au moins une conduite pour envoyer le(s) gaz formé(s) au moyen de compression et une conduite d'une fraction auxiliaire du liquide de cycle reliée à l'échangeur de chaleur pour transporter soit le ou un des produits liquides ou un liquide à traiter pour former le ou un des produits liquides caractérisé en ce que la conduite pour envoyer le gaz formé au moyen de compression est une conduite pour envoyer au moins un gaz formé à l'entrée du premier étage pour former un gaz comprimé, l'appareil comprenant une conduite pour envoyer le gaz comprimé dans le premier étage au deuxième étage. 10. Apparatus for liquefying a gas containing at least 60 mol%. of CO 2 for producing at least one liquid product, comprising a heat exchanger (E1), a compression means (C1, C2, C3, C4) comprising at least two stages in series of which a first stage and a second stage downstream first stage, a pipe to send a feed gas to the inlet of the second stage of the compression means for being compressed from a first pressure to a second pressure, means for cooling the gas at the second pressure to form a liquid or supercritical flow, optionally a pipe to bring a part of the liquid or supercritical flow to serve as a product without passing through the heat exchanger, a pipe for causing at least a portion of the liquid or supercritical flow to cool in the exchanger to form a cycle liquid at the second pressure, at least one pipe for sending at least a fraction of the liquid vaporize in the exchanger, in the case where several fractions vaporize means for vaporizing the at least two fractions each at a different pressure, and at least one pipe to send the (s) gas formed (s) by means of compression and a conduit of an auxiliary fraction of the cycle liquid connected to the heat exchanger to convey s whereinthe or one of the liquid products or a liquid to be treated to form the liquid or one of the liquid products characterized in that the pipe for sending the gas formed to the compression means is a pipe for sending at least one gas formed to the inlet of the first stage for forming a compressed gas, the apparatus comprising a conduit for supplying the compressed gas in the first stage to the second stage.
1 1 . Appareil selon la revendication 10 dans lequel au moins une dite conduite pour envoyer un gaz formé par vaporisation au moyen de compression (C1 , C2, C3, C4) est reliée à un point du moyen de compression en amont de l'entrée du premier gaz d'alimentation dans le moyen de compression. 1 1. Apparatus according to claim 10 wherein at least one said conduit for supplying a gas formed by vaporization to the compression means (C1, C2, C3, C4) is connected to a point of the compression means upstream of the inlet of the first gas feeding in the compression means.
12. Appareil selon la revendication 10 ou 1 1 comprenant une boîte froide contenant l'échangeur et des moyens de détente (6, 15, 16, 43) d'un liquide à vaporiser dans l'échangeur, ainsi que des moyens de traitement de la fraction auxiliaire du liquide de cycle, constitués par au moins un séparateur de phase (P1 , P2) et/ou au moins une colonne de distillation. 12. Apparatus according to claim 10 or 1 1 comprising a cold box containing the exchanger and means (6, 15, 16, 43) of a liquid to be vaporized in the exchanger, and means for treating the auxiliary fraction of the cycle liquid, constituted by at least one phase separator (P1, P2) and / or at least one distillation column.
13. Appareil selon la revendication 12 comprenant une conduite pour envoyer un deuxième gaz d'alimentation aux moyens de traitement (P1 , P2) sans avoir été comprimé dans les moyens de compression. 13. Apparatus according to claim 12 comprising a conduit for sending a second feed gas to the processing means (P1, P2) without having been compressed in the compression means.
14. Appareil selon la revendication 13 dans lequel la conduite pour envoyer un deuxième gaz d'alimentation aux moyens de traitement est reliée à l'échangeur (E1 ). 14. Apparatus according to claim 13 wherein the conduit for sending a second feed gas to the processing means is connected to the exchanger (E1).
15. Appareil selon l'une des revendications 10 à 14 ne comprenant pas de moyen pour enrichir le liquide de cycle de CO2 avant de le diviser. 15. Apparatus according to one of claims 10 to 14 not including means for enriching the CO2 cycle liquid before dividing it.
PCT/FR2012/050562 2011-03-16 2012-03-16 Method and apparatus for the liquefaction of co2 WO2012123690A2 (en)

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EP12714804.7A EP2791602A2 (en) 2011-03-16 2012-03-16 Method and apparatus for the liquefaction of co2
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FR2972792B1 (en) 2017-12-01

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