WO2011089382A2 - Purification d'un courant riche en co2 - Google Patents

Purification d'un courant riche en co2 Download PDF

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Publication number
WO2011089382A2
WO2011089382A2 PCT/GB2011/000055 GB2011000055W WO2011089382A2 WO 2011089382 A2 WO2011089382 A2 WO 2011089382A2 GB 2011000055 W GB2011000055 W GB 2011000055W WO 2011089382 A2 WO2011089382 A2 WO 2011089382A2
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stream
pressure
liquid
temperature
rich
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PCT/GB2011/000055
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English (en)
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WO2011089382A3 (fr
Inventor
Matthew Bough
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Bp Alternative Energy International Limited
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Publication of WO2011089382A2 publication Critical patent/WO2011089382A2/fr
Publication of WO2011089382A3 publication Critical patent/WO2011089382A3/fr

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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/06—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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/506—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification at low temperatures
    • 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
    • F25J3/0655—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 hydrogen
    • 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
    • F25J3/00—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/08—Separating gaseous impurities from gases or gaseous mixtures or from liquefied gases or liquefied gaseous mixtures
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2210/00—Processes characterised by the type or other details of the feed stream
    • F25J2210/06—Splitting of the feed stream, e.g. for treating or cooling in different ways
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2215/00—Processes characterised by the type or other details of the product stream
    • F25J2215/80—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
    • 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
    • F25J2230/20—Integrated compressor and process expander; Gear box arrangement; Multiple compressors on a common shaft
    • 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
    • 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
    • F25J2270/04—Internal refrigeration with work-producing gas expansion loop
    • F25J2270/06—Internal refrigeration with work-producing gas expansion loop with multiple gas expansion loops
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/12—External refrigeration with liquid vaporising loop
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2270/00—Refrigeration techniques used
    • F25J2270/60—Closed external refrigeration cycle with single component refrigerant [SCR], e.g. C1-, C2- or C3-hydrocarbons
    • 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
    • F25J2270/66—Closed external refrigeration cycle with multi component refrigerant [MCR], e.g. mixture of hydrocarbons
    • 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
    • F25J2290/12—Particular process parameters like pressure, temperature, ratios
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry

Definitions

  • the present invention relates to the purification of a carbon dioxide (C0 2 ) rich stream. Aspects of the invention find particular application for example in relation to a C0 2 rich stream which additionally contains hydrogen, for example a stream that comprises primarily CO and hydrogen (3 ⁇ 4).
  • aspects of the present invention relate to the purification of a C0 2 rich stream that comprises at least 90 mol% of C0 2 and less than 10 mol% of 3 ⁇ 4.
  • a C0 2 stream of sufficient purity can be obtained for C0 2 sequestration for example storage in the underground strata; and/or use in a wide range of other applications, for example in the food, chemical and/or the oil and gas industry.
  • C0 2 is considered to be the most prominent of all the so-called “greenhouse gases”
  • sequestration of liquid or supercritical C0 2 is of a greater interest than ever, primarily as it is considered to be becoming more and more desirable - and necessary - to reduce the atmospheric emissions of greenhouse gases in order to slow down the rate of human- induced climate change.
  • C0 2 for example resulting from a C0 2 recovery process, such as the one described in International Patent Application No. PCT/GB2009/001810) and/or use it in other applications for example in the food industry, the said C0 2 must be of certain purity first, which is known to be very difficult and expensive to obtain.
  • the typical way to remove H 2 from a C0 2 rich stream is to flash the C0 2 rich stream, using conventional technology - however this method is both expensive and inefficient, since the typical C0 2 rich stream that exits most of the processes for C0 2 recovery, does so at a relatively high pressure for example approximately 150 Bar, and therefore needs to be flashed to a relatively low pressure for example approximately 115 Bar in order to recover at least a part of the 3 ⁇ 4; additionally, for most applications and/or for the transportation of the recovered C0 2 , the C0 2 needs to not only be of a certain purity but also needs to be of a relatively high pressure for example more than 90 bar, more than 100 bar, for example more than 120 bar, for example approximately!
  • a first aspect of the present invention provides a process for removing H 2 from a C0 2 rich stream containing H 2 , comprising the following steps:
  • step (c) recovering a gaseous H 2 fraction, and a purified C0 2 liquid fraction from step (b).
  • a further aspect of the present invention provides an integrated process for recovering and sequestrating a purified C02 from a C02 rich stream containing H2, comprising the following steps:
  • step (c) recovering a gaseous H 2 fraction, and a purified C0 2 liquid fraction from step (b); and (d) sequestrating the purified C0 2 fraction from step (c).
  • the critical point of a C02-rich stream as used in the present invention is also well known by the man skilled in the art who considers it to be essentially the same as that for pure C0 2 .
  • the critical point of the C0 2 H 2 binary mixture is preferably the arithmetic mean of the critical temperatures and pressures of the two individual components (i.e. C0 2 and 3 ⁇ 4), e.g. for the critical temperature of the binary mixture, one can use the following formulae:
  • the said C0 2 rich stream comprises more than 90 mole% of C0 2 and less than 10 mole% of H 2 .
  • the benefits of the present invention will apply throughout the composition range of the C0 2 rich stream containing H 2 as previously defined, there are some preferred composition ranges for which the advantages of the purification process according to the present invention will be more apparent.
  • the C0 2 rich stream may comprise more than 1 mole %, more than 2 mole %, or even more than 3 mole % of 3 ⁇ 4; it may comprise less than 9 mole%, less than 8 mole%, or even less than 7 mole % of H 2 .
  • the C0 2 rich stream may comprise more than 91 mole%, 92 mole %, or even more than 93 mole% of C0 2 ; it may comprise less than 99 mole%, less than 98 mole%, or even less than 97 mole % of C0 2 .
  • the stream itself can advantageously be generated by any suitable process known to those skilled in the art for recovering a C0 2 rich stream of this type e.g. a syngas separation process, as described in PCT/GB2009/001810.
  • Other components and impurities such as nitrogen, steam, argon and/or oxygen can also be tolerated in the process of examples the present invention.
  • the pressure PI , and temperature Tl which are the conditions of the C0 2 rich stream containing H 2 to be treated according to the present invention, may be respectively:
  • the pressure of the C0 2 rich stream may advantageously be greater than 7.5 MPa, preferably greater than 10 MPa, more preferably greater than 12 MPa, or most preferably greater than 14 MPa; it may also be less than 30 MPa, preferably less than 25 MPa, or most preferably less than 20 MPa.
  • the temperature of the C0 2 rich stream may advantageously be less than 50 °C, for example less than 30 °C, less than 0 °C, and even less than -20 °C; it may also be greater than -55 °C, for example greater than - 35 °C, or even greater than - 10 °C.
  • the process of aspects of the present invention is characterised by cooling the said C0 2 rich stream to a temperature T2 whilst maintaining its pressure at a pressure P2; where P2 corresponds to a pressure that is greater than the critical point pressure of the stream and T2 corresponds to a temperature where pure C0 2 is in the liquid phase at pressure P2.
  • the cooling step is such that [T1-T2] is greater than 1 °C, or greater than 5 °C, or even greater than 10 °C.
  • Said cooling step can be performed without substantial changes of the pressure conditions, e.g. with P2 which remains identical to PI.
  • pressure P2 is lower than PI, e.g. P2 could be from 0.5 to 5 MPa lower than PI . Indeed, the Applicants have found that this could
  • the pressure of the C0 2 purified stream may
  • the temperature of the C0 2 purified stream may advantageously be less than 50 °C, preferably less than 30 °C, for example less than 0 °C, and even less than -20 °C; it may also be greater than -55 °C, for example greater than - 35 °C, or even greater than - 10 °C.
  • the cooling of the C0 2 rich stream to a temperature T2 can be done by any appropriate method, e.g. by passing the said C0 2 rich stream through a heat exchanger system.
  • the heat exchanger system preferably uses an external refrigerant. Suitable external refrigerant include ethane, propane, propene, ethylene, ammonia, hydrochlorofluorocarbons (HCFCs) and mixed refrigerants; ethane is the preferred external refrigerant. It can also be done by passing the said C0 2 rich stream through a heat exchanger system in heat exchange relationship with at least one internal refrigerant stream wherein the internal refrigerant stream, i.e. a refrigerant that is produced subsequently in the process; said internal refrigerant stream is selected from the group consisting of cold hydrogen rich vapour stream and liquid C0 2 stream.
  • the heat exchanger system comprises both external and internal refrigeration.
  • the C0 2 rich stream is first passed through a heat exchanger system in heat exchange relationship with a cold liquid C0 2 internal refrigerant stream, said cold liquid C0 2 being preferably the purified liquid C0 2 stream of step (c) of the present invention; additionally, the said heat exchanger system may also comprise another internal refrigerant stream such as the cold hydrogen rich vapour stream, said cold hydrogen rich vapour stream being preferably the hydrogen of step (c) of the present invention; in addition, and preferably in a subsequent heat exchanger system, the said internally cooled C0 2 rich stream is then cooled to the final temperature T2 by external refrigeration as described hereabove.
  • refrigerant used herein preferably includes any appropriate coolant or refrigerant.
  • coolant preferably includes any appropriate coolant or refrigerant.
  • internal refrigerant stream(s) includes product streams produced in the process.
  • the internal coolant streams include C0 2 rich streams and H 2 rich streams formed in the separation step(s).
  • the term “internal coolant streams” includes any appropriate internal coolant or refrigerant stream.
  • external refrigerant or “external coolant” include a refrigerant or coolant that is provided in an external refrigeration circuit. Accordingly, liquid C0 2 that is formed in the process of the present invention will not generally be regarded as an external refrigerant.
  • step (c) is performed by passing the cooled C0 2 rich stream from step (b) either directly or indirectly to a separation apparatus for example a fractionation unit, e.g. a gas-liquid separator vessel, that is preferably operated at substantially the same pressure as the heat exchanger system, and withdrawing a high pressure (HP) hydrogen rich vapour stream from at or near the top of fractionation unit and a purified liquid C0 2 stream (which is at or above the liquid C0 2 export pressure) from at or near the bottom of the fractionation unit.
  • a separation apparatus for example a fractionation unit, e.g. a gas-liquid separator vessel, that is preferably operated at substantially the same pressure as the heat exchanger system, and withdrawing a high pressure (HP) hydrogen rich vapour stream from at or near the top of fractionation unit and a purified liquid C0 2 stream (which is at or above the liquid C0 2 export pressure) from at or near the bottom of the fractionation unit.
  • a separation apparatus for example a fractionation unit, e.g
  • the purified liquid C0 2 stream When the purified liquid C0 2 stream is above the liquid C0 2 export pressure, it may advantageously be brought to a lower pressure before being passed to the fractionation unit. It is envisaged that the energy associated with reducing the pressure of the liquid C0 2 stream to export pressure may be recovered using a hydro turbine system. Alternatively, the liquid C0 2 stream may be flashed to lower pressure across a valve before being passed to a flash separation vessel (the valve may be located at the inlet to the fractionation unit).
  • o as fuel gas feed e.g. for a combustor of a gas turbine of a power plant, o as a feed to an expander (preferably a turboexpander) which, thanks to the expansion of the hydrogen rich vapour stream, may be used to drive a rotor or shaft of a compressor and/or to drive the rotor or shaft of an electric generator, and
  • an expander preferably a turboexpander
  • C0 2 sequestration e.g. storage in the in the underground strata
  • other applications e.g. in the food, chemical and oil and gas industry
  • a further aspect of the present invention provides a process for separating a gas stream including hydrogen and carbon dioxide into a hydrogen (H 2 ) rich vapour stream and a purified liquid carbon dioxide (C0 2 ) stream in a C0 2 condensation plant that comprises a heat exchanger system, a gas-liquid separator vessel, the process comprising the steps of:
  • step (B) cooling the gas stream from step (A) to a temperature in the range of -15 to -55°C by passing the synthesis gas stream through the heat exchanger system in heat exchange relationship with at least one refrigerant stream;
  • step (C) passing the cooled gas stream from step (B), either directly or indirectly, to a gas- liquid separator vessel that is operated at substantially the same pressure as the heat exchanger system and withdrawing a hydrogen rich vapour stream from at, or near, the top of the separator vessel and a liquid C0 2 stream from at, or near, the bottom of the separator vessel, wherein said liquid C0 2 stream is a C0 2 rich stream containing H 2 which comprises more than 90 mole% of C0 2 and less than 10 mole% of H 2 and is at a temperature T 1 , and a pressure P 1 ; where P 1 corresponds to a pressure that is greater than the critical point pressure of the said C0 2 rich stream, and Tl is a temperature where at pressure PI, pure C0 2 is either in the liquid or supercritical phase;
  • step (D) the liquid C0 2 stream (the C0 2 rich stream containing hydrogen) obtained in step (C) is cooled to a temperature T2, whilst maintaining the stream pressure at a pressure P2; where P2 corresponds to a pressure that is greater than the critical point pressure of the stream, and T2 corresponds to a temperature where pure C0 2 is in the liquid phase at pressure P2; and
  • step (E) the cooled stream obtained in step (D) is separated into a hydrogen vapour and a purified C0 2 liquid.
  • the compression and cooling may be carried out in any order.
  • the feed gas stream may pass to the process at a suitable pressure in some examples, and therefore additional compression may not be necessary.
  • the gas stream may includes synthesis gas.
  • the synthesis gas may comprise shifted or partially shifted synthesis gas, for example which may have been subject to a water gas shift reaction to increase the carbon dioxide content.
  • the gas feed stream comprises less than 10%, preferably less than 5% or less than 2% of components other than carbon dioxide and hydrogen.
  • the gas stream may be provided at a suitable pressure for effecting partial condensation of the gas feed stream by cooling.
  • the pressure will be for example from 7.5 to 40 MPa.
  • the condensation plant may include an expansion system comprising at least one expander, and the process further may include the step of feeding the hydrogen rich vapour stream from step (C) to the expansion system wherein the hydrogen rich vapour stream is subjected to isentropic expansion in an expander such that a hydrogen rich vapour stream is withdrawn from the expander at reduced temperature and reduced pressure and wherein isentropic expansion of the hydrogen rich vapour in each the expander generates motive power.
  • the expansion system may include a plurality of expanders, wherein, in use, a hydrogen rich vapour stream may be withdrawn from each expander of the system at successively reduced temperature and reduced pressure.
  • the purified CO2 liquid separated in step (E) may be at or above the liquid C0 2 export pressure.
  • a further aspect of the present invention also provides a process for separating a synthesis gas stream into a hydrogen (H 2 ) rich vapour stream and a purified liquid carbon dioxide (C0 2 ) stream in a C0 2 condensation plant that comprises a heat exchanger system, a gas-liquid separator vessel, and an expansion system comprising at least one expander, the process comprising the steps of:
  • step (B) cooling the HP synthesis gas stream from step (A) to a temperature in the range of - 15 to -55°C by passing the HP synthesis gas stream through the heat exchanger system in heat exchange relationship with at least one refrigerant stream;
  • step (C) passing the cooled HP synthesis gas stream from step (B), either directly or indirectly, to a gas-liquid separator vessel that is operated at substantially the same pressure as the heat exchanger system, and withdrawing a high pressure (HP) hydrogen rich vapour stream from at, or near, the top of the separator vessel and a high pressure (HP) liquid C0 2 stream from at, or near, the bottom of the separator vessel, wherein said high pressure (HP) liquid C0 2 stream is the C0 2 rich stream containing 3 ⁇ 4 which comprises more than 90 mole% of C0 2 and less than 10 mole% of H 2 and is at a temperature Tl , and a pressure P 1 ; where PI corresponds to a pressure that is greater than the critical point pressure of the said C02 rich stream, and Tl is a temperature where at pressure PI, pure C0 2 is either in the liquid or supercritical phase;
  • step (D) feeding the HP hydrogen rich vapour stream from step (C) to the expansion system wherein the hydrogen rich vapour stream is subjected to isentropic expansion in the expander(s) such that a hydrogen rich vapour stream is withdrawn from the expander(s) at reduced temperature and at reduced pressure and wherein isentropic expansion of the hydrogen rich vapour in the expander(s) generates motive power;
  • step (E) the high pressure (HP) liquid C0 2 stream (the C0 2 rich stream containing hydrogen) obtained in step (C) is cooled to a temperature T2, whilst maintaining the stream pressure at a pressure P2; where P2 corresponds to a pressure that is greater than the critical point pressure of the stream, and T2 corresponds to a temperature where pure C0 2 is in the liquid phase at pressure P2; and
  • step (F) separating the cooled stream obtained in step (E) into a hydrogen vapour and a purified C0 2 liquid which is at or above the liquid C0 2 export pressure.
  • the motive power that is generated in step (D) can advantageously be used to drive a machine that is a component of the C0 2 condensation plant and/or driving an alternator of an electric generator.
  • the machine that is driven by the expander(s) in step (D) is preferably a compressor of the compression system (as defined hereafter) and/or a pump (for example, for pumping liquid C0 2 or supercritical C0 2 ).
  • the expander(s) are used to drive an alternator of an electric generator, the electricity is preferably used to power one or more components of the C0 2 condensation plant.
  • step (B) the cooling of the HP synthesis gas stream from step (A) to a temperature in the range of -15 to -55°C is preferably performed by passing the HP synthesis gas stream through the heat exchanger system in heat exchange relationship with at least one refrigerant stream; a plurality of refrigerant streams are preferably used.
  • said refrigerant streams are preferably "internal" i.e. produced subsequently in the process wherein the internal refrigerant streams are selected from the group consisting of cold hydrogen rich vapour streams and liquid C0 2 streams.
  • this cooling step additionally comprises an external refrigeration heat exchange.
  • Suitable external refrigerants include ethane, propanes, propene, ethylene, hydrochlorofluorocarbons (HCFC's), ammonia and/or mixed refrigerants; propane being the preferred external refrigerant.
  • the heat exchanger system may comprise both external and internal refrigeration.
  • the combination of internal refrigeration with both cold hydrogen rich vapour streams and liquid C0 2 streams together with an external refrigeration represents a preferred embodiment of the present invention.
  • the cooled HP synthesis gas stream from step (B) is preferably at a temperature Tl and a pressure PI .
  • An advantage of the process of the present invention is that at least 75%, preferably, at least 90%, more preferably, at least 95% of the carbon dioxide is separated from the synthesis gas feed stream with the carbon dioxide capture level being dependent upon the pressure of the HP synthesis gas stream, on the temperature of the cooled synthesis gas stream from step (B), and on the temperature of the purified liquid C02 stream formed in step (F).
  • the C0 2 capture level will depend on the temperature to which the HP synthesis gas stream is cooled in the heat exchanger system(s).
  • a further advantage of the present invention is that typically, at least 98%, preferably, at least 99%, more preferably, at least 99.5%, in particular, at least 99.8% of the hydrogen is recovered in the H 2 rich vapour stream.
  • the hydrogen rich vapour stream that is separated in step (C) may be at a pressure substantially above the minimum fuel gas feed pressure (inlet pressure) for a combustor(s) of at least one gas turbine(s) of a power plant. Accordingly, the HP hydrogen rich vapour stream may be reduced in pressure in step (D) to the desired inlet pressure for the combustor(s) of the gas turbine(s) by isentropically expanding the HP hydrogen rich vapour stream in at least one expander, preferably at least one turboexpander, more preferably a series of
  • turboexpanders thereby providing cold H 2 rich vapours streams (internal refrigerant streams) that may be used for heat integration in the overall process, e.g. to cool the HP synthesis gas stream in step (B) and/or to cool the HP hydrogen rich vapour stream from step (C).
  • isentropic expansion of the hydrogen rich vapour streams in each of the (turbo)expanders of the series may generate motive power that may be used for example to drive the compressor(s) of the compression system (where provided, for example as defined hereafter) and/or to drive at least one alternator of an electric generator thereby generating electricity for use in the process (for example, for operating one or more electric compressors of the compression system) and/or to drive a pump (for example, a pump for a liquid C0 2 or supercritical C0 2 stream).
  • a major portion of the compression energy may be recovered using the (turbo)expanders thereby increasing the overall energy efficiency of the process.
  • the HP hydrogen rich vapour stream may be expanded to pressures below the inlet pressure of the combustor of a gas turbine, if the hydrogen rich vapour stream is to be used for a different purpose, for example, as fuel for a low pressure burner of a fired heater, or as fuel for a reformer or boiler or as a refinery feed stream for upgrading of one or more refinery streams or as a hydrogen feed to a chemical process.
  • the synthesis gas feed stream may be generated from a solid fuel such as petroleum coke or coal in a gasifier or from a gaseous hydrocarbon feedstock in a reformer.
  • the synthesis gas from the gasifier or reformer may contain high amounts of carbon monoxide. Accordingly, depending on the desired composition of the hydrogen rich vapour stream, the synthesis gas may be treated in a shift converter unit where substantially all of the carbon monoxide contained in the synthesis gas stream is converted to carbon dioxide over a shift catalyst according to the water gas shift reaction (WGSR)
  • WGSR water gas shift reaction
  • Said WGSR may take place at a pressure sufficient to provide the synthesis gas stream at a pressure required for step (A) of the present invention.
  • the water gas shift reaction is exothermic and results in a significant temperature rise across the shift converter unit.
  • the shift converter unit may be cooled by continuously removing a portion of the shifted synthesis gas stream and cooling this stream by heat exchange with one or more process streams, for example against boiler feed water or against steam (for the generation of superheated steam).
  • the synthesis gas that exits the shift converter unit comprises primarily hydrogen, carbon dioxide and steam and minor amounts of carbon monoxide and methane. Where the synthesis gas is of sufficiently high C0 2 content, the shift conversion step may be omitted, in which case the synthesis gas comprises primarily hydrogen, carbon dioxide, carbon monoxide, and steam and minor amounts of methane.
  • the synthesis gas stream is cooled to a temperature in the range of 30 to 50°C, for example, about 40°C, upstream of the C0 2 condensation plant, by heat exchange with at least one cold process stream, to condense out a condensate (predominantly comprised of water).
  • the cold process stream is a process stream used during the generation of the synthesis gas.
  • the condensate is then separated from the cooled synthesis gas stream, for example, in a condensate drum.
  • the synthesis gas that exits the gasifier will also comprise minor amounts of hydrogen sulfide (H 2 S) as an impurity (sour synthesis gas).
  • H 2 S impurity is formed by reaction of COS with steam in the shift converter unit.
  • This 3 ⁇ 4S may be captured upstream of the CO2 condensation plant, for example, by selectively absorbing the H 2 S from the sour synthesis gas in an absorption tower.
  • SelexolTM a mixture of dimethyl ethers of polyethylene glycol
  • Any H 2 S that is captured may be either converted into elemental sulphur using the Claus Process or into industrial strength sulphuric acid.
  • the sour synthesis gas stream may be fed to the C0 2 condensation plant of the present invention where a major portion of the H 2 S partitions into the liquid C0 2 phase and may therefore be sequestered with the C0 2 .
  • any residual H 2 S in the final 3 ⁇ 4 rich vapour stream may be removed downstream of the C0 2 condensation plant by passing the final H 2 rich vapour stream through an adsorbent bed, for example, a zinc oxide bed, or by passing the final 3 ⁇ 4 rich vapour stream through a scrubber that utilises a suitable liquid absorbent.
  • an adsorbent bed for example, a zinc oxide bed
  • a scrubber that utilises a suitable liquid absorbent.
  • There is minimal pressure drop for example, a pressure drop of less than 0.5 bar across the absorbent bed.
  • the synthesis gas stream is preferably dried prior to being passed to the C0 2 condensation plant, as any moisture in the synthesis gas will freeze and potentially cause blockages in the plant.
  • the synthesis gas stream may be dried by being passed through a molecular sieve bed or an absorption tower that employs a solvent, for example, triethylene glycol, to selectively absorb the water.
  • the dried synthesis gas stream has a water content of less than 1 ppm (on a molar basis).
  • the dried synthesis gas of step (A) comprises at least 40 mole % 3 ⁇ 4, preferably, at least 50 mole% H 2 , in particular, 55 to 60 mole % H 2 . It may also comprise at least 30 mole % C0 2 , e.g. at least 35 mol % C0 2 . Even if it is not preferred, CO can be tolerated in the synthesis gas treated according to the present invention, e.g. if the WGSR is only partial.
  • the compression stage needed for bringing the synthesis gas stream of step (A) at the desired pressure can be done either during the WGSR or after the WGSR, preferably during and after the WGSR.
  • the synthesis gas is at a pressure in the range 10 to 120 barg, preferably, 20 to 95 barg, more preferably, 30 to 60 barg.
  • the temperature at which the synthesis gas is fed to the compression system is not critical. However, it is preferred that the synthesis gas is fed to the compression system at a temperature in the range of 25 to 50°C, for example, 30 to 45°C.
  • the synthesis gas is then compressed, in the compression system, to a pressure in the range of 7.5 MPa to 40 MPa; said pressure is preferably greater than 10 MPa, more preferably greater than 12 MPa, or most preferably greater than 14 MPa; it may also be less than 30 MPa, preferably less than 25 MPa, or most preferably less than 20 MPa.
  • the pressure of the synthesis gas stream just before the cooling step (B) is comprised between PI and
  • the compression system is a multistage compressor system comprising a plurality of compressors arranged in series.
  • the compressor(s) of the compression system is mounted on a shaft that may be driven by an electric motor, gas turbine or steam turbine.
  • the compressor(s) of the compression system and the (turbo)expander(s) of the (turbo)expansion system may be mounted on a common shaft so that the isentropic expansion of the hydrogen rich vapour in the (turbo)expander(s) may be used to drive the compressor(s).
  • the compressed HP synthesis gas stream is cooled to remove at least part, preferably, substantially all of the heat of compression before being passed through the heat exchanger system thereby reducing the cooling duty for the heat exchanger system.
  • at least part of the heat of compression is preferably removed from the HP synthesis gas by passing the HP synthesis gas stream through at least one heat exchanger of the compression system in heat exchange relationship with an external coolant and/or an external refrigerant.
  • the multistage compression system is provided with at least one interstage heat exchanger where the compressed gas is cooled against an external coolant and/or refrigerant before being passed to the next compressor in the series.
  • interstage heat exchangers are provided between each compressor in the series.
  • the multistage compression system is also provided with at least one heat exchanger after the final stage of compression where the HP synthesis gas stream is cooled against an external coolant and/or an external refrigerant before being passed to the heat exchanger system.
  • the compressed HP synthesis gas stream from the final stage of compression may be passed through a first heat exchanger in heat exchange relationship with an external coolant and then through a second heat exchanger in heat exchange relationship with an external refrigerant, prior to being passed to the heat exchanger system.
  • Suitable external coolants for use in the heat exchanger(s) of the compression system include air, water, or a cold process stream such as the H 2 rich vapour stream formed in step (C) or the final 3 ⁇ 4 rich vapour stream that is exported from the process of the present invention.
  • Suitable external refrigerants for use in the heat exchanger of the compression system include ethane, propane, propene, ethylene, ammonia,
  • hydrochlorofluorocarbons HCFCs
  • mixed refrigerants HCFCs
  • the HP synthesis gas that exits the compression system has not been heat exchanged with an external refrigerant, the HP synthesis gas typically exits the
  • the HP synthesis gas stream is then preferably passed through the heat exchanger system of the C0 2 condensation plant where the HP synthesis gas stream is preferably first cooled against a plurality of internal refrigerant streams i.e. cold process streams that are produced subsequently in the process.
  • the internal refrigerant streams may be selected from cold hydrogen rich vapour stream(s), in particular, cold expanded hydrogen rich vapour stream(s) from the (turbo)expander(s) of the (turbo)expansion system, and liquid C0 2 stream(s), including the purified liquid C0 2 stream.
  • the HP synthesis gas stream is cooled in the heat exchanger system to a temperature in the range -15 to -55°C, preferably, -25 to -50°C, for example, -25 to -40°C.
  • a pressure drop across the heat exchanger system for example, a pressure drop of less than 1.5 bar, preferably, less than 1.0 bar.
  • the heat exchanger system comprises at least one multichannel heat exchanger with the HP synthesis gas stream being passed through a channel of the multichannel heat exchanger in heat exchange relationship with a plurality of internal refrigerant streams that are passed through further channels in the multichannel heat exchanger.
  • the multichannel heat exchanger include those described in US 6622519, WO 2004/016347, EP 212878 and EP 292245 the disclosures of which are incorporated herein by reference.
  • the HP synthesis gas stream is passed in a counter-current direction through the multichannel heat exchanger to the internal refrigerant streams and optional external refrigerant stream(s).
  • the heat exchanger system comprises a plurality of refrigeration stages arranged in series where each stage in the series comprises either (i) a single multichannel heat exchanger, or (ii) a plurality of multichannel heat exchangers arranged in parallel, for example, 2 or 3 multichannel heat exchangers arranged in parallel.
  • the heat exchanger system comprises three refrigeration stages arranged in series with the internal refrigerant streams and optional external refrigerant stream(s) being fed to each successive stage of the series at successively lower temperatures.
  • the heat exchanger system may comprise a plurality of refrigeration stages wherein each refrigeration stage comprises either a single stand-alone heat exchanger or a plurality of stand-alone heat exchangers arranged in parallel.
  • the HP synthesis gas stream is cooled as it is passed through the refrigeration stages of the heat exchanger system by heat exchange with a plurality of internal refrigerant streams and optional external refrigerant stream(s) that are fed to the stand-alone heat exchanger(s) of each successive refrigeration stage at successively lower temperatures. It is preferred that the HP synthesis gas stream is passed through the stand- alone heat exchangers in a counter-current direction to the internal refrigerant streams and optional external refrigerant stream(s) that are fed to the stand-alone heat exchangers.
  • the heat exchanger system may comprise both multichannel and stand-alone heat exchangers.
  • the heat exchanger system may comprise a plurality of refrigeration stages arranged in series wherein each refrigeration stage comprises (i) a single multichannel heat exchanger, or (ii) a single stand-alone heat exchanger, or (iii) a plurality of multichannel heat exchangers and/or a plurality of standalone heat exchangers arranged in parallel.
  • the multichannel heat exchanger(s) of the heat exchanger system may for example be of the type employed in processes for generating liquefied natural gas such as a brazed aluminium plate-fin heat exchanger or a diffusion-bonded heat exchanger (for example, a printed circuit heat exchanger (PCHE) as supplied by Heatric).
  • a brazed aluminium plate-fin heat exchanger or a diffusion-bonded heat exchanger (for example, a printed circuit heat exchanger (PCHE) as supplied by Heatric).
  • PCHE printed circuit heat exchanger
  • the multichannel heat exchanger(s) may for example be a multiple body shell and tube heat exchanger comprising either (a) a tube arranged in the shell of the heat exchanger wherein the shell of the heat exchanger comprises a plurality of compartments and wherein the HP synthesis gas stream is passed through the tube and an internal refrigerant stream or external refrigerant stream is passed through each compartment of the shell in heat exchange relationship with the HP synthesis gas that is flowing through the tube; or (b) a plurality of tubes arranged in the shell of the heat exchanger wherein the shell comprises a single compartment and the HP synthesis gas is passed through the compartment and an internal refrigerant stream or an external refrigerant stream is passed through each of the tubes in heat exchange relationship with the HP synthesis gas that is flowing through the single compartment of the shell.
  • channel encompasses the channels formed between the plates of a brazed aluminium plate-fin heat exchanger or a diffusion-bonded heat exchanger and also the compartment(s) and tube(s) of a multiple body shell and tube heat exchanger.
  • the stand-alone heat exchanger(s) of the compression system may be of the shell and tube type (a single body shell and tube heat exchanger) with the HP synthesis gas stream passing through the tube side and an internal refrigerant stream or external refrigerant stream passing through the shell side of the heat exchanger or vice versa.
  • a process that employs stand-alone heat exchangers to pre-cool the HP synthesis gas stream may be of reduced efficiency compared with a process that employs a multichannel heat exchanger, in whole or in part, to cool the HP synthesis gas stream in step (B) of the present invention.
  • the cooled HP synthesis gas stream that exits the heat exchanger system is a two phase stream comprised of a liquid phase and vapour phase.
  • the amount of cooling that is achieved in the heat exchanger system owing to heat exchange with the plurality of internal refrigerant streams will be dependent upon the amount of cooling of the isentropically expanded hydrogen rich vapour streams that is achieved in the expansion system which, in turn, is dependent on the pressure of the HP hydrogen rich vapour stream that is formed in step (C) and the pressure of the 3 ⁇ 4 rich vapour stream that exits the final or only (turbo)expander of the (turbo)expansion system in step (D).
  • (turbo)expansion system will also be dependent on the extent to which the hydrogen rich vapour is subjected to isentropic expansion in the (turbo)expansion system which is also dependent on the pressure of the 3 ⁇ 4 rich vapour stream formed in step (C) and the pressure of the H 2 rich vapour stream that exits the final (turbo)expander of the (turbo)expansion system in step (D).
  • the cooled synthesis gas stream from the heat exchanger system may be passed directly to a gas-liquid separator vessel that is preferably operated at substantially the same pressure as the heat exchanger system.
  • the pressure drop across the separator vessel is typically in the range of 0.1 to 5 bar, preferably, 0.1 to 1 bar, in particular, 0.1 to 0.5 bar.
  • a HP hydrogen rich vapour phase is preferably withdrawn from at or near the top of the gas-liquid separator vessel and is passed to the (turbo)expander system while a HP liquid C0 2 stream is withdrawn from at or near the bottom of the gas-liquid separator vessel.
  • said HP liquid C0 2 stream may be a C0 2 rich stream containing H 2 and comprising more than 90 mole% of C0 2 and less than 10 mole% of H 2> at a temperature Tl , and a pressure P 1.
  • HP synthesis gas which has or has not already been partially or totally subjected to the internal cooling may also be passed partially (with subsequent recombination of the feeds) or totally to a heat exchanger that employs an external refrigerant.
  • Suitable external refrigerants that may be used as refrigerant in the heat exchanger(s) include ethane, propanes, propene, ethylene, ammonia, hydrochlorofluorocarbons (HCFCs) and mixed refrigerants.
  • Typical mixed refrigerants comprise at least two refrigerants selected from the group consisting of butanes, propanes, ethane, and ethylene. These refrigerants may be cooled to the desired refrigeration temperature in external refrigerant circuits using any method known to the person skilled in the art including methods known in the production of liquefied natural gas.
  • These refrigerants may also be cooled to the desired refrigeration temperature by heat exchange with one or more cold isentropically expanded 3 ⁇ 4 rich vapour streams from the (turbo)expander(s) of the (turbo)expansion system.
  • the external refrigerant is selected so as to achieve the desired operating temperature.
  • propane may be used as refrigerant when the feed temperature of the HP synthesis gas stream is in the range of -15 to greater than -30°C while ethane and/or ethylene may be used as external refrigerant when the feed temperature of the HP synthesis gas stream is in the range of -30 to -40°C.
  • the HP hydrogen rich vapour stream formed in step (C) may be thus fed to the (turbo)expansion system according to the present invention.
  • the HP hydrogen rich vapour stream formed in step (C) Prior to being fed to the (turbo)expansion system, the HP hydrogen rich vapour stream formed in step (C) may be used to cool the HP synthesis gas stream in step (B) by passing the cold HP hydrogen rich vapour stream through a further channel in a multichannel heat exchanger (or through a stand-alone heat exchanger) in heat exchange relationship with the HP synthesis gas stream.
  • the HP hydrogen rich vapour stream may be used as coolant for the heat exchanger(s) of the compression system.
  • the HP H 2 rich vapour stream may be first fed to a solvent extraction system in which the vapour stream is contacted with a solvent which absorbs any residual C0 2 contained therein.
  • Solvent extraction processes for effecting this separation include the Rectisol and Selexol processes which respectively uses refrigerated methanol and a refrigerated mixture of dimethyl ethers of polyethylene glycol as the absorbent.
  • the absorbent can be amine based for example
  • the HP hydrogen rich vapour stream formed in step (C) may be subjected to an additional cooling/separation stage before being fed to the (turbo)expansion system.
  • cooling/separation stage allows to recover a residual C0 2 liquid feed which can advantageously be recombined with the HP liquid C0 2 stream from step (C).
  • Said preferred embodiment is depicted in the appended figure 1.
  • the HP 3 ⁇ 4 rich vapour stream that is fed to the (turbo)expansion system is at elevated pressure. Accordingly, the H 2 rich vapour stream is reduced in pressure to the desired exit pressure by being passed through the (turbo)expansion system.
  • the expansion energy recovered from the H 2 rich vapour streams in the (turbo)expander(s) can be used to drive an electric turbine or can be used to directly drive the compressors of the compressor system. As discussed above, isentropic expansion of the 3 ⁇ 4 rich vapour stream results in significant cooling.
  • the operating pressures of the (turbo)expanders are set to optimise the expander efficiency and to ensure the discharge temperatures for the expanded H 2 rich vapour streams do not fall below -56°C (the freezing point of C0 2 ).
  • the discharge temperatures of the expanded streams are in the range of -15°C to -51°C, preferably, -20°C to -51°C, in particular, -30 to -51°C.
  • one or more of the cold isentropically expanded hydrogen rich vapour streams may be used as an internal refrigerant for a different purpose, for example, to cool an external refrigerant (such as propane or ethane) that is employed in the process or to cool a non-isentropically expanded H 2 rich vapour stream so that it can be used as internal refrigerant in the process of the present invention.
  • an external refrigerant such as propane or ethane
  • H 2 rich vapour stream so that it can be used as internal refrigerant in the process of the present invention.
  • the discharge temperature of the expanded stream may be below -55°C.
  • the liquid C0 2 stream (including the purified liquid C0 2 stream) is used as internal refrigerant in the heat exchanger system thereby providing further cooling for the HP synthesis gas feed stream in step (B).
  • one or all of the separated H 2 rich vapour streams of the process are preferably used as an internal refrigerant stream in the heat exchanger system thereby providing cooling of the HP synthesis gas stream in step (B).
  • the combined H 2 rich vapour stream may be routed through a channel of a multichannel heat exchanger in heat exchange relationship with the HP synthesis gas stream.
  • the purified C0 2 product stream can then be exported from the process and sequestered and/or used in a chemical process.
  • an advantage of the present invention is that the purified C0 2 product stream is produced at the desired C0 2 export pressure and C0 2 purity so that there is no requirement to provide additional C0 2 pumps.
  • the purified C0 2 stream which is at a temperature T2 can be exported and sequestrated at the same temperature, i.e. in the liquid phase; however, since this purified C0 2 stream is advantageously used as internal refrigerant, the C0 2 export and
  • sequestration can obviously be operated at a higher temperature, i.e. at a temperature where the purified C0 2 stream can be either in liquid or in supercritical phase (dense phase).
  • the purified C0 2 product stream that is exported from the process of the present invention preferably comprises at least 95 mole % C0 2 , in particular, at least 98 mole % C0 2 , the remainder being mostly hydrogen with some inerts, for example, nitrogen and/or carbon monoxide (CO).
  • the synthesis gas feed stream is a sour synthesis gas
  • the purified C0 2 product stream will also comprise minor amounts of H 2 S.
  • the purified C0 2 product stream comprises H 2 S
  • the product is either sequestered or the H 2 S is removed prior to the C0 2 being used for a different purpose, such as a feed to a chemical process.
  • the purified C0 2 product stream is sequestered, it is typically delivered to a pipeline that transfers the purified C0 2 product stream to a reception facility of an oil field where the purified C0 2 product stream may be used as an injection fluid for an oil reservoir. If necessary, the purified C0 2 product stream is pumped to above the pressure of the oil reservoir before being injected down an injection well and into the oil reservoir. The injected C0 2 displaces the hydrocarbons contained in the reservoir rock towards a production well for enhanced recovery of hydrocarbons therefrom. If any carbon dioxide is produced from the production well together with the hydrocarbons, the carbon dioxide may be separated from the hydrocarbons for re-injection into the oil reservoir. It is also envisaged that the purified C0 2 product stream may be sequestered by being injected into an aquifer or a depleted oil or gas reservoir for storage therein.
  • the amount of C0 2 contained in the H 2 rich vapour stream that is obtained from the C0 2 condensation plant is less than 10 mole %, preferably less than 5 mole %, more preferably, less than 2 mole %, in particular, less than 1 mole %.
  • the H 2 rich vapour stream may comprise up to 20 mole % carbon monoxide (CO).
  • the 3 ⁇ 4 rich vapour stream typically comprises trace amounts of CO and methane, for example, less than 500 ppm on a molar basis.
  • the remainder of the hydrogen rich vapour stream that is obtained from the C0 2 condensation plant is predominantly hydrogen.
  • the H 2 rich vapour stream obtained from the C0 2 condensation plant may be used as fuel for a low pressure burner of a fired heater, or as fuel for a reformer or boiler or as a refinery feed stream for upgrading of one or more refinery streams or as a feed to a chemical process.
  • the 3 ⁇ 4 rich vapour stream is to be used as a fuel, it is preferred that the 3 ⁇ 4 rich vapour stream contains only trace amounts of CO thereby minimizing the amount of C0 2 released to atmosphere (where the C0 2 arises from combustion of CO).
  • an advantage of some examples of the present invention is that the fuel gas stream may be obtained at above the minimum inlet pressure for the combustor(s) of the gas turbine(s).
  • the feed pressure for the fuel gas stream is in the range of 25 to 45 barg, preferably, 28 to 40 barg, in plute.
  • a compressor to compress the fuel gas stream to the inlet pressure for the combustor(s) of the gas turbine(s).
  • the 3 ⁇ 4 rich vapour stream is diluted with medium pressure nitrogen and/or medium pressure steam prior to being fed as fuel gas to the combustor(s) of the gas turbine(s).
  • the fuel gas stream that is fed to the combustor(s) of the gas turbine(s) preferably contains 35 to 65 mole % hydrogen, more preferably, 45 to 60 mole % hydrogen, for example, 48 to 52 mole % of hydrogen.
  • the expansion energy recovered from the H 2 rich vapour streams in the (turbo)expanders of the (turbo)expansion system can reduce the net power consumption of the separation process to less than 30 MW, preferably, less than 25 MW, in particular less than 23 MW when processing 28,000 kmol/hour of synthesis gas containing 56 mol% hydrogen and 43 mol% C0 2 .
  • the net power consumption is preferably defined as: [power consumption in the compression system + power consumption in the external refrigerant compression system
  • a carbon dioxide condensation plant for separating carbon dioxide and a hydrogen from a synthesis gas stream, the plant comprising:
  • a gas-liquid separator vessel for separating the partially condensed compressed synthesis gas stream into a hydrogen rich vapour stream and liquid C0 2 stream, said liquid C02 stream being the C0 2 rich stream which comprises more than 90 mole% of C0 2 and less than 10 mole% of H 2> at a temperature Tl, and a pressure PI; where PI corresponds to a pressure that is greater than the critical point pressure of the stream, and Tl is a temperature where at pressure PI, pure C0 2 is either in the liquid or supercritical phase;
  • step (g) an expander system comprising at least one expander for expanding the separated hydrogen rich vapour stream from step (d) and optionally from step (f) to a lower pressure wherein the expander system is adapted to produce a hydrogen rich vapour stream from the final expander at a pressure at or above the minimum fuel gas feed pressure to the combustor of at least one gas turbine of a power plant and wherein each expander is adapted to provide a hydrogen rich vapour stream that is preferably used as an internal refrigerant stream for the heat exchanger system.
  • step (d) When the (turbo)expander system comprises a plurality of (turbo)expanders arranged in series, the expansion of the separated hydrogen rich vapour stream from step (d) and optionally from step (f) takes preferably place at successively lower pressures.
  • the C0 2 condensation plant may optionally comprise a valve for letting down the pressure of the separated liquid C0 2 stream to the C0 2 export pressure.
  • the purified liquid C0 2 is preferably used as an internal refrigerant stream for the heat exchanger system.
  • Figure 1 contains several process configurations according to the present invention. For the avoidance of doubt, and as explained hereinbelow, these respective embodiments can be independent of each other and/or combined into integrated embodiments.
  • - [38] is at a temperature between -25 and -35C and a pressure between 13.5 and 18 MPa
  • - [202] is at a temperature between -30 and -55C, said temperature being at least 5C below the temperature of [38]; and at a pressure between 13.5 and 18 MPa, said pressure being equal or lower than the pressure of [38], and
  • [V-401] represents the gas/liquid separator vessel.
  • cooling step (b) is performed in two stages, respectively in [E-201], an internal refrigeration heat exchanger system wherein both [205] and [204] are used as internal refrigerants, and [E-202], an external refrigeration heat exchanger system wherein ethane is preferably used as the external refrigerant.
  • Figure 1 also describes another embodiment according to the present invention, i.e. the integrated process wherein a synthesis gas is efficiently separated into a purified liquid C0 2 which is at export pressure, e.g. suitable for storage and oil recovery, and a hydrogen gas which is e.g. suitable for fuel gas.
  • a synthesis gas is efficiently separated into a purified liquid C0 2 which is at export pressure, e.g. suitable for storage and oil recovery, and a hydrogen gas which is e.g. suitable for fuel gas.
  • step (A) is the synthesis gas stream of step (A) which is subjected to the cooling step (B) and becomes [20],
  • step (D) of the present invention i.e. wherein the gaseous H 2 rich fraction is subjected to expansion in turboexpanders in series.
  • Said turboexpanders are depicted by [EX-101] and [EX-102].
  • FIG. 1 also describes several embodiments on how the cooling step (B) could be performed:
  • [E-105] is a heat exchanger for cooling the synthesis gas which uses both the purified liquid C0 2 [44] and the H 2 [34] as internal refrigerants.
  • the said liquid C0 is the combination of the purified liquid C0 2 [43] and the liquid C0 2 stream [36].
  • the synthesis gas [1 1] is first cooled in [E-105] and becomes [12].
  • synthesis gas [12] is then separated into [13], [15] and [17], wherein [13] is subjected to the internal refrigeration [E- 106], [15] is subjected to the internal refrigeration [E-107], and [17] is subjected to the external refrigeration [E-108] and/or [E-109].
  • the so obtained cooled synthesis streams are then recombined before separation in [V-101].
  • figure 1 describes an additional configuration wherein the H 2 feed [21] is subjected to an additional cooling/separation step in [E-l 10] and [V-102].
  • figure 1 also describes a multiple compressions stage - at the top left of the figure - which comprises a combination of compressors/exchangers in series as depicted by [ -101]/[E101], [K-102]/[E102], [K103]/[E103], [K-104]/[E-104].
  • HYSYS software has been used to predict the properties and phase splits of the C0 2 rich mixture for the preferred embodiment.
  • HYSYS is one of a number of chemical process simulators used to simulate the heat and material balance for chemical and other processes, any of which could have been used for this purpose. It is based on widely available physical property methods and correlations for predicting chemical and mixture properties across a wide range of temperatures and pressures. An appropriate property method for the application has been selected based on temperature and pressure envelopes and components present, taking account of any other interactions. On this basis, a HYSYS simulation example has been performed on the basis of the integrated process
  • our invention provided a superior turbine output, and an improved performance e.g. on power consumption.
  • a further aspect of the invention provides a carbon dioxide condensation plant for separating carbon dioxide and hydrogen from a gas feed stream, the plant comprising:
  • a gas-liquid separator vessel for separating the partially condensed gas stream into a hydrogen rich vapour stream and liquid C0 2 stream, said liquid C0 2 stream being a C0 2 rich stream which comprises more than 90 mole% of C0 2 and less than 10 mole% of H 2j at a temperature Tl, and a pressure PI; where PI corresponds to a pressure that is greater than the critical point pressure of the stream, and Tl is a temperature where at pressure P 1 , pure C0 2 is either in the liquid or supercritical phase;
  • a gas-liquid separator vessel for separating the C0 2 rich stream into a hydrogen rich vapour stream and a purified liquid C0 2 stream.
  • the source of the gas feed stream may comprise a source of a gas feed stream including syngas.
  • the plant may further include an expander system comprising a one or more expander(s) and/or turboexpander(s), wherein the expander system is arranged to receive a hydrogen rich vapour stream from step (c) and/or from step (e) and to expand the stream to a lower pressure.
  • an expander system comprising a one or more expander(s) and/or turboexpander(s), wherein the expander system is arranged to receive a hydrogen rich vapour stream from step (c) and/or from step (e) and to expand the stream to a lower pressure.
  • the expander system may be arranged to produce a hydrogen rich vapour stream from the final or only expander or turbo expander in the series at a pressure at or above the minimum fuel gas feed pressure to the combustor of at least one gas turbine of a power plant.
  • the plant may include a plurality of expanders and/or turbo-expanders arranged in series for expanding hydrogen rich vapour streams from step (c) and/or from step (e) to a lower pressure
  • the plant may further include a compression system for compressing the gas feed stream, for example to a pressure in the range of from 5 to 40 MPa.
  • the plant may further include a heat exchanger system for cooling the gas feed stream to a temperature in the range of - 15 to -55°C.
  • the expander system may be adapted to provide a hydrogen rich vapour stream that is suitable for use as an internal refrigerant stream for the heat exchanger system of step (b) and/or for the heat exchanger system of step (d).
  • the expander system may be adapted to feed the expanded hydrogen rich vapour to a heat exchanger system for use as a coolant.

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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Thermal Sciences (AREA)
  • General Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Organic Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Separation By Low-Temperature Treatments (AREA)
  • Gas Separation By Absorption (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

La présente invention concerne la purification d'un courant riche en dioxyde de carbone (CO2) qui comporte principalement du CO2 et de l'hydrogène (H2). En particulier, la présente invention concerne la purification d'un courant riche en CO2 qui comporte au moins 90 % en mole de CO2 et moins de 10 % en mole d'H2 pour obtenir un courant de CO2 de pureté suffisante pour la séquestration de CO2, par exemple le stockage dans des strates souterraines, et/ou pour l'utilisation dans un large éventail d'autres applications, par exemple dans l'industrie agro-alimentaire, chimique et du pétrole et/ou du gaz.
PCT/GB2011/000055 2010-01-21 2011-01-19 Purification d'un courant riche en co2 WO2011089382A2 (fr)

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EP2685191A1 (fr) * 2012-07-13 2014-01-15 L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude Procédé et appareil pour la séparation d'un gaz riche en dioxyde de carbone
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WO2017184802A1 (fr) 2016-04-21 2017-10-26 Fuelcell Energy, Inc. Élimination du dioxyde de carbone de l'échappement d'anode d'une pile à combustible par refroidissement/condensation
US11211625B2 (en) 2016-04-21 2021-12-28 Fuelcell Energy, Inc. Molten carbonate fuel cell anode exhaust post-processing for carbon dioxide
US11508981B2 (en) 2016-04-29 2022-11-22 Fuelcell Energy, Inc. Methanation of anode exhaust gas to enhance carbon dioxide capture
US11975969B2 (en) 2020-03-11 2024-05-07 Fuelcell Energy, Inc. Steam methane reforming unit for carbon capture

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Cited By (18)

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CN102564066A (zh) * 2012-02-10 2012-07-11 南京柯德超低温技术有限公司 基于小型低温制冷机的用于气体分离和纯化的低温装置
CN102564066B (zh) * 2012-02-10 2013-10-16 南京柯德超低温技术有限公司 基于小型低温制冷机的用于气体分离和纯化的低温装置
US9746233B2 (en) 2012-07-13 2017-08-29 L'Air Liquide Socieété Anonyme Pour l'Étude Et l'Exploitation Des Procedes Georges Clause Process for the separation of a gas rich in carbon dioxide
WO2014009300A1 (fr) * 2012-07-13 2014-01-16 L'air Liquide,Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude Processus de séparation de gaz riche en dioxyde de carbone
CN104428615A (zh) * 2012-07-13 2015-03-18 乔治洛德方法研究和开发液化空气有限公司 用于分离富含二氧化碳的气体的方法
CN104428615B (zh) * 2012-07-13 2016-08-31 乔治洛德方法研究和开发液化空气有限公司 用于分离富含二氧化碳的气体的方法
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EP2685191A1 (fr) * 2012-07-13 2014-01-15 L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude Procédé et appareil pour la séparation d'un gaz riche en dioxyde de carbone
JP2016124730A (ja) * 2014-12-26 2016-07-11 国立研究開発法人産業技術総合研究所 高圧水素製造法および製造システム
WO2017184802A1 (fr) 2016-04-21 2017-10-26 Fuelcell Energy, Inc. Élimination du dioxyde de carbone de l'échappement d'anode d'une pile à combustible par refroidissement/condensation
CN109155419A (zh) * 2016-04-21 2019-01-04 燃料电池能有限公司 通过冷却/冷凝从燃料电池的阳极排气中除去二氧化碳
EP3446350A4 (fr) * 2016-04-21 2019-06-19 Fuelcell Energy, Inc. Élimination du dioxyde de carbone de l'échappement d'anode d'une pile à combustible par refroidissement/condensation
US11094952B2 (en) 2016-04-21 2021-08-17 Fuelcell Energy, Inc. Carbon dioxide removal from anode exhaust of a fuel cell by cooling/condensation
US11211625B2 (en) 2016-04-21 2021-12-28 Fuelcell Energy, Inc. Molten carbonate fuel cell anode exhaust post-processing for carbon dioxide
CN109155419B (zh) * 2016-04-21 2022-06-24 燃料电池能有限公司 通过冷却/冷凝从燃料电池的阳极排气中除去二氧化碳
US11949135B2 (en) 2016-04-21 2024-04-02 Fuelcell Energy, Inc. Molten carbonate fuel cell anode exhaust post-processing for carbon dioxide capture
US11508981B2 (en) 2016-04-29 2022-11-22 Fuelcell Energy, Inc. Methanation of anode exhaust gas to enhance carbon dioxide capture
US11975969B2 (en) 2020-03-11 2024-05-07 Fuelcell Energy, Inc. Steam methane reforming unit for carbon capture

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