US2996891A - Natural gas liquefaction cycle - Google Patents

Natural gas liquefaction cycle Download PDF

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US2996891A
US2996891A US685580A US68558057A US2996891A US 2996891 A US2996891 A US 2996891A US 685580 A US685580 A US 685580A US 68558057 A US68558057 A US 68558057A US 2996891 A US2996891 A US 2996891A
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stream
gas
liquid
methane
pressure
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Shao E Tung
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Conch International Methane Ltd
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Conch International Methane Ltd
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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    • 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
    • F25J3/02—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream
    • F25J3/0228—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream
    • F25J3/0266—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream separation of carbon dioxide
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    • 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
    • F25J1/0022—Hydrocarbons, e.g. natural gas
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    • 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
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    • 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"
    • F25J1/0035—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 gas expansion with extraction of work
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    • 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
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    • F25J1/0208—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 a single-component refrigerant [SCR] fluid in a closed vapor compression cycle in combination with an internal quasi-closed refrigeration loop, e.g. with deep flash recycle loop
    • F25J1/0209—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 a single-component refrigerant [SCR] fluid in a closed vapor compression cycle in combination with an internal quasi-closed refrigeration loop, e.g. with deep flash recycle loop as at least a three level refrigeration cascade
    • F25J1/021—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 a single-component refrigerant [SCR] fluid in a closed vapor compression cycle in combination with an internal quasi-closed refrigeration loop, e.g. with deep flash recycle loop as at least a three level refrigeration cascade using a deep flash recycle loop
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    • F25J1/0243—Start-up or control of the process; Details of the apparatus used; Details of the refrigerant compression system used
    • F25J1/0244—Operation; Control and regulation; Instrumentation
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    • F25J1/0255—Operation; Control and regulation; Instrumentation controlling particular process parameter, e.g. pressure, temperature controlling the composition of the feed or liquefied gas, e.g. to achieve a particular heating value of natural gas
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    • F25J3/0228—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream
    • F25J3/0242—Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by rectification, i.e. by continuous interchange of heat and material between a vapour stream and a liquid stream characterised by the separated product stream separation of CnHm with 3 carbon atoms or more
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    • F25J2220/60—Separating impurities from natural gas, e.g. mercury, cyclic hydrocarbons
    • F25J2220/66—Separating acid gases, e.g. CO2, SO2, H2S or RSH
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    • F25J2270/60—Closed external refrigeration cycle with single component refrigerant [SCR], e.g. C1-, C2- or C3-hydrocarbons
    • 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

  • One object of the invention is to provide a liquefaction process for producing substantially pure liquid methane from a stream of natural gas which contains one or more constituents such as heavier hydrocarbons, carbon dioxide, hydrogen sulfide, or nitrogen.
  • Another object of the invention is to liquefy natural gas streams containing impurities at a maximum ethciency and a minimum cost.
  • FIGS. l and 2 together comprise a flow diagram illustrating my new liquefaction process
  • FIG. 3 is a graph showing the pressure-temperature relations of a liquid-vapor-solid carbon dioxide equilibrium in a CO2-CH4 system
  • FIG. 4 is a graph showing the temperature-composition sections of a CO2-CH., system at 7.15 p.s.i.a.;
  • FIG. 5 shows the apparatus to be inserted into the liquefaction cycle when the CO2 content exceeds the tolerance limit
  • FIG. 6 is a graph which shows the temperature-composition section of a CO2-CH., system at 673 p.s.i.a.;
  • the gaseous stream can be cooled down to minus 50 F. with no formation of solid particles by heat exchange with external refrigeration and cold expanded gas to be later recycled.
  • the stream may be reduced to a liquid by throttling the stream and withdrawing the gas subsequently evaporated.
  • the temperature of the liquid stream will be substantially reduced and the acid gases will freeze.
  • the acid gases may be separated from the methane stream during this throttling process as solid particles.
  • a pressure below that of the cricondenbar point of the combined stream (combined feed stream and the recycle stream) but above the univariant vapor-liquid-solid equilibrium curve of that same stream may be chosen so that heavy hydrocarbons will condense during the heat exchanging process and can be separated from the methane, but at the same time no solid heavy hydrocarbons will deposit in the exchanger wall.
  • heavy hydrocarbon separators may be included at appropriate points in the refrigeration stage to separate the condensed liquid from Ithe gaseous stream. While the gas rich in methane continues its path in the major liquefaction cycle, the separated liquid may be throttled down as a separate stream and the resultant liquid rich in heavy hydrocarbon recovered as a byproduct by draining it from a separator following the final throttling.
  • the invention comprises the method of liquefying and purifying a stream of natural gas which contains a suibstantial proportion of methane with portions of gases having a higher solidilication temperature than methane which comprises the following steps: reducing the temperature of the stream of gas while maintaining the pressure on such stream above the maximum value of the univariant vapor-liquid-solid equilibrium curve of the combined gas stream; then throttling the cold stream to effect liquefaction and thereby also further reduce the temperature of the stream Ito cause solidiiication of constituents of such stream other than methane, and separating such solidified constituents from the remaining liquid stream to leave a liquid now more largely methane.
  • well gas is iirst cooled by a water cooler 1, and then, if necessary, reduced in pressure by a turbo-expander 2 to a pressure slightly above the maximum value of the univariant vapor-liquid-solid equilibrium curve of the combined gas stream.
  • a turbo-expander 2 reduces in pressure by a turbo-expander 2 to a pressure slightly above the maximum value of the univariant vapor-liquid-solid equilibrium curve of the combined gas stream.
  • the maximumr value of the univariant vapor-liquid-solid equilibrium curve of a combined carbon dioxide and methane stream is 7'10 p.s.i.a. as shown in FIG. 3.
  • the separate streams of methane and heavier hydrocarbons are then independently progressively reduced to substantially atmospheric pressure either in a single or in multiple stages to lower pressure levels.
  • a multiple stage reduction may be accomplished by means of a series of throttle valves, 10, 11 and 12 in the methane stream and 13, 14, and 15 in the heavier hydrocarbon stream.
  • the solid carbon dioxide formed during throttling will probably not plug up a throttle valve of special streamline design because of the turbulent condition from the reduction of pressure.
  • a heating jacket is provided for each throttle valve so that a slight amount of heat may be added to loosen up any solid deposit if it does occur.
  • the liquid that evaporates into gas in these throttling processes is separated from the resultant liquid in separators 16, 17 ⁇ and 18 in the methane stream and 19, 20 and 21 in the heavier hydrocarbon stream and enters the heat exchanging process with the high pressure stream in heat exchangers 4, 5 and 6 either independently or with other equi-pressure recycle streams combined at equitemperature points. Then before being recycled the separate streams of expanded gas are recompressed to the pressure of the well gas stream. This is done by irst compressing in compressor 22 and cooling in water cooler 23 the gas passed oi from the liquid after the last throttling process to the pressure of the stream before the last throttling process.
  • This compressed gas is then combined with the gas passed off after the second last throttling process and this combined stream compressed to the pressure of the well ⁇ gas stream and cooled in compressor 24 and cooler 25.
  • the gas passed off after the first throttling process in the heavier hydrocarbon stream is recompressed to the well gas pressure in compressor 26, cooled in cooler 27, and then combined with the rest of the gas recompressed for recycling.
  • This combined compressed stream that is to be recycled may initially be cooled by heat exchange with the expanded gas in heat exchanger 28.
  • the carbon dioxide in the system will form solid particles when the methane stream is throttled and may conveniently be separated from the liquefaction system during the throttling process.
  • Two alternate liquid settlers may be provided to each CII separator to settle out the solid from the liquid before it passes on to the next throttling stage.
  • specific gravity of carbon dioxide solid 1.5 gm./ml. at minus 69.9 F.
  • methane liquid .42 gm./ ml. at minus 259 F.
  • settling is easy to achieve and is an appropriate process for phase separation.
  • the liquid may be drained oli. and the solid may be removed as liquid by supplying heat to a steam coil provided for each settler.
  • a slight rise is provided to each of the entrance pipes of the throttle valves to prevent it from being plugged by the solid deposition.
  • Filtration devices may be used instead of a settler if desired.
  • the gas withdrawn from each of the separators 16, 17 and 18 in the throttling process of the methane stream will be practically free from solid contamination because of the liquid-scrubbing action occurring during the throttle process.
  • two gas scrubbers which may also serve as liquid lters, may be provided for each separator.
  • the gas withdrawn from each separator before being passed in heat exchange with the high pressure stream is passed respectively through scrubbing towers 29, 30 and '31 in counter-current iiow with the liquid withdrawn from the same separator.
  • the liquid after passing through the scrubbing towers is returned to the main stream to continue the throttling process.
  • the two scrubbing towers provided for each separator may be used alternatively and the deposited solid may be removed in liquid form by applying heat to the scrubbing tower by steam coils. Then the carbon dioxide may be collected in the receivers 32, 33 and 34.
  • the liquid withdrawn from the final methane separator 18 is the desired methane product, substantially pure and approximately at atmospheric pressure.
  • methane occupies about one six hundredth of the space it does in gaseous form. This liquid methane is sent to storage tanks or transportation vessels to be shipped to points of use.
  • the liquid heavy hydrocarbon by-product may be drawn off as liquid or it may be used to provide additional refrigeration by passing it through the heat exchangers 4, 5, 6 and 28 before withdrawing it from the system.
  • the carbon dioxide content exceed the tolerance limit (13%) my liquefaction cycle can still be operated if some additional equipment is provided.
  • This additional equipment needed is shown in FIG. 5.
  • gas may be cooled down to a temperature whereby, after throttling down to 673 p.s.i.a., it will attain a temperature of minus 93 F., as indicated in FIG. 5.
  • the scrubbing liquid used in scrubber 37 may be recycling liquid methane from the lirst separator 16, may be heavy hydrocarbon condensed out in the liquefaction process, or may be some externally provided hydrocarbon liquid in an extra recycling cycle.
  • the solid carbon dioxide in the scrubbing tower 37 or in the solid settler 36 may be removed by heat supplied to steam coils provided for such purpose.
  • the method of liquefying and purifying a stream of natural gas which contains a substantial portion of methane with portions of acid gases which comprises the following stages:

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US3236057A (en) * 1962-05-28 1966-02-22 Conch Int Methane Ltd Removal of carbon dioxide and/or hydrogen sulphide from methane
US3242681A (en) * 1963-01-31 1966-03-29 Philips Corp Natural gas liquefaction and storage
US3257813A (en) * 1960-08-03 1966-06-28 Conch Int Methane Ltd Liquefaction of gases
US3260058A (en) * 1962-05-09 1966-07-12 Air Prod & Chem Method and apparatus for separating gaseous mixtures, particularly helium-containing gases
US3323315A (en) * 1964-07-15 1967-06-06 Conch Int Methane Ltd Gas liquefaction employing an evaporating and gas expansion refrigerant cycles
US3376709A (en) * 1965-07-14 1968-04-09 Frank H. Dickey Separation of acid gases from natural gas by solidification
DE1268161B (de) * 1963-02-23 1968-05-16 Linde Ag Verfahren zur Verfluessigung von Erdgas
US3398544A (en) * 1966-07-27 1968-08-27 Continental Oil Co Solidification of acidic components in natural gas
US3581510A (en) * 1968-07-08 1971-06-01 Phillips Petroleum Co Gas liquefaction by refrigeration with parallel expansion of the refrigerant
US4001116A (en) * 1975-03-05 1977-01-04 Chicago Bridge & Iron Company Gravitational separation of solids from liquefied natural gas
US4169133A (en) * 1977-02-08 1979-09-25 Krupp-Koppers Gmbh Process for recovering acidic gases collected during gas desulfurization
US5473900A (en) * 1994-04-29 1995-12-12 Phillips Petroleum Company Method and apparatus for liquefaction of natural gas
US6301927B1 (en) * 1998-01-08 2001-10-16 Satish Reddy Autorefrigeration separation of carbon dioxide
US20040055329A1 (en) * 2002-08-15 2004-03-25 Mathias James A. Process for cooling a product in a heat exchanger employing microchannels
US20040148961A1 (en) * 2001-01-30 2004-08-05 Denis Clodic Method and system for extracting carbon dioxide by anti-sublimation for storage thereof
US20060277942A1 (en) * 2003-03-04 2006-12-14 Denis Clodic Method of extracting carbon dioxide and sulphur dioxide by means of anti-sublimation for the storage thereof
NL2000292C2 (nl) * 2006-10-27 2008-04-29 Romico Hold A V V Werkwijze voor het in fracties separeren van een mediummengsel.
WO2010023238A1 (en) * 2008-08-29 2010-03-04 Shell Internationale Research Maatschappij B.V. Process and apparatus for removing gaseous contaminants from gas stream comprising gaseous contaminants
US20100147022A1 (en) * 2005-09-15 2010-06-17 Cool Energy Limited Process and apparatus for removal of sour species from a natural gas stream
EP2442056A3 (en) * 2010-10-15 2018-03-07 Daewoo Shipbuilding&Marine Engineering Co., Ltd. Method for producing pressurized liquefied natural gas and production system therefor
CN109579433A (zh) * 2019-01-18 2019-04-05 成都深冷液化设备股份有限公司 一种二氧化碳提纯液化的装置及方法
US10316260B2 (en) 2007-01-10 2019-06-11 Pilot Energy Solutions, Llc Carbon dioxide fractionalization process

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US2022165A (en) * 1934-05-09 1935-11-26 Lee S Twomey Method of separating and purifying hydrogen
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US2826266A (en) * 1956-07-30 1958-03-11 Phillips Petroleum Co Removal of co2 from natural gas
US2863296A (en) * 1955-07-19 1958-12-09 Herrick L Johnston Inc High pressure cycle for the continuous separation of a gas mixture into its components

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US668197A (en) * 1900-07-18 1901-02-19 Ernest A Le Sueur Process of extracting liquid methane from natural gas.
US2022165A (en) * 1934-05-09 1935-11-26 Lee S Twomey Method of separating and purifying hydrogen
US2500129A (en) * 1944-08-29 1950-03-07 Clark Bros Co Inc Liquefaction system
US2777299A (en) * 1953-04-13 1957-01-15 Kellogg M W Co Separating gas mixtures
US2863296A (en) * 1955-07-19 1958-12-09 Herrick L Johnston Inc High pressure cycle for the continuous separation of a gas mixture into its components
US2826266A (en) * 1956-07-30 1958-03-11 Phillips Petroleum Co Removal of co2 from natural gas

Cited By (30)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3257813A (en) * 1960-08-03 1966-06-28 Conch Int Methane Ltd Liquefaction of gases
US3260058A (en) * 1962-05-09 1966-07-12 Air Prod & Chem Method and apparatus for separating gaseous mixtures, particularly helium-containing gases
US3236057A (en) * 1962-05-28 1966-02-22 Conch Int Methane Ltd Removal of carbon dioxide and/or hydrogen sulphide from methane
US3242681A (en) * 1963-01-31 1966-03-29 Philips Corp Natural gas liquefaction and storage
DE1268161B (de) * 1963-02-23 1968-05-16 Linde Ag Verfahren zur Verfluessigung von Erdgas
US3323315A (en) * 1964-07-15 1967-06-06 Conch Int Methane Ltd Gas liquefaction employing an evaporating and gas expansion refrigerant cycles
US3376709A (en) * 1965-07-14 1968-04-09 Frank H. Dickey Separation of acid gases from natural gas by solidification
US3398544A (en) * 1966-07-27 1968-08-27 Continental Oil Co Solidification of acidic components in natural gas
US3581510A (en) * 1968-07-08 1971-06-01 Phillips Petroleum Co Gas liquefaction by refrigeration with parallel expansion of the refrigerant
US4001116A (en) * 1975-03-05 1977-01-04 Chicago Bridge & Iron Company Gravitational separation of solids from liquefied natural gas
US4169133A (en) * 1977-02-08 1979-09-25 Krupp-Koppers Gmbh Process for recovering acidic gases collected during gas desulfurization
US5473900A (en) * 1994-04-29 1995-12-12 Phillips Petroleum Company Method and apparatus for liquefaction of natural gas
US6301927B1 (en) * 1998-01-08 2001-10-16 Satish Reddy Autorefrigeration separation of carbon dioxide
US20040148961A1 (en) * 2001-01-30 2004-08-05 Denis Clodic Method and system for extracting carbon dioxide by anti-sublimation for storage thereof
AU2007203461B2 (en) * 2001-01-30 2010-06-17 Armines Method and system for extracting carbon dioxide by anti-sublimation for storage thereof
US7073348B2 (en) * 2001-01-30 2006-07-11 Armines Method and system for extracting carbon dioxide by anti-sublimation for storage thereof
US7000427B2 (en) * 2002-08-15 2006-02-21 Velocys, Inc. Process for cooling a product in a heat exchanger employing microchannels
US20040055329A1 (en) * 2002-08-15 2004-03-25 Mathias James A. Process for cooling a product in a heat exchanger employing microchannels
US20060277942A1 (en) * 2003-03-04 2006-12-14 Denis Clodic Method of extracting carbon dioxide and sulphur dioxide by means of anti-sublimation for the storage thereof
US20100147022A1 (en) * 2005-09-15 2010-06-17 Cool Energy Limited Process and apparatus for removal of sour species from a natural gas stream
NL2000292C2 (nl) * 2006-10-27 2008-04-29 Romico Hold A V V Werkwijze voor het in fracties separeren van een mediummengsel.
WO2008051079A1 (en) * 2006-10-27 2008-05-02 Romico Hold A.V.V. Method for separating a medium mixture into fractions
US10316260B2 (en) 2007-01-10 2019-06-11 Pilot Energy Solutions, Llc Carbon dioxide fractionalization process
WO2010023238A1 (en) * 2008-08-29 2010-03-04 Shell Internationale Research Maatschappij B.V. Process and apparatus for removing gaseous contaminants from gas stream comprising gaseous contaminants
US20110167869A1 (en) * 2008-08-29 2011-07-14 Geers Henricus Abraham Process and apparatus for removing gaseous contaminants from gas stream comprising gaseous contaminants
AU2009286701B2 (en) * 2008-08-29 2012-09-13 Shell Internationale Research Maatschappij B.V. Process and apparatus for removing gaseous contaminants from gas stream comprising gaseous contaminants
RU2520269C2 (ru) * 2008-08-29 2014-06-20 Шелл Интернэшнл Рисерч Маатсхаппий Б.В. Способ удаления газообразных загрязнителей из потока газа, содержащего газообразные загрязнители и устройство для его осуществления
US9396854B2 (en) 2008-08-29 2016-07-19 Shell Oil Company Process and apparatus for removing gaseous contaminants from gas stream comprising gaseous contaminants
EP2442056A3 (en) * 2010-10-15 2018-03-07 Daewoo Shipbuilding&Marine Engineering Co., Ltd. Method for producing pressurized liquefied natural gas and production system therefor
CN109579433A (zh) * 2019-01-18 2019-04-05 成都深冷液化设备股份有限公司 一种二氧化碳提纯液化的装置及方法

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NL112795C (ja) 1966-05-16

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