WO2011026170A1 - Process and apparatus for reducing the concentration of a sour species in a sour gas - Google Patents

Process and apparatus for reducing the concentration of a sour species in a sour gas Download PDF

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Publication number
WO2011026170A1
WO2011026170A1 PCT/AU2010/001063 AU2010001063W WO2011026170A1 WO 2011026170 A1 WO2011026170 A1 WO 2011026170A1 AU 2010001063 W AU2010001063 W AU 2010001063W WO 2011026170 A1 WO2011026170 A1 WO 2011026170A1
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Prior art keywords
gas
sour
sour species
species
concentration
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PCT/AU2010/001063
Other languages
French (fr)
Inventor
Nimalan Gnanendran
Simon Elliott
Allan Hart
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Cool Energy Limited
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Publication date
Priority to AU2009904160 priority Critical
Priority to AU2009904160A priority patent/AU2009904160A0/en
Application filed by Cool Energy Limited filed Critical Cool Energy Limited
Publication of WO2011026170A1 publication Critical patent/WO2011026170A1/en

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Classifications

    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/06Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation
    • F25J3/0605Processes 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
    • F25J3/061Natural gas or substitute natural gas
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10Working-up natural gas or synthetic natural gas
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10Working-up natural gas or synthetic natural gas
    • C10L3/101Removal of contaminants
    • C10L3/102Removal of contaminants of acid contaminants
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/06Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation
    • F25J3/063Processes 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
    • F25J3/0635Processes 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 CnHm with 1 carbon atom or more
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J3/00Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification
    • F25J3/06Processes or apparatus for separating the constituents of gaseous or liquefied gaseous mixtures involving the use of liquefaction or solidification by partial condensation
    • F25J3/063Processes 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
    • F25J3/067Processes 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2210/00Processes characterised by the type or other details of the feed stream
    • F25J2210/04Mixing or blending of fluids with the feed stream
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2220/00Processes or apparatus involving steps for the removal of impurities
    • F25J2220/60Separating impurities from natural gas, e.g. mercury, cyclic hydrocarbons
    • F25J2220/66Separating acid gases, e.g. CO2, SO2, H2S or RSH
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2230/00Processes or apparatus involving steps for increasing the pressure of gaseous process streams
    • F25J2230/60Processes or apparatus involving steps for increasing the pressure of gaseous process streams the fluid being hydrocarbons or a mixture of hydrocarbons
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2235/00Processes or apparatus involving steps for increasing the pressure or for conveying of liquid process streams
    • F25J2235/80Processes or apparatus involving steps for increasing the pressure or for conveying of liquid process streams the fluid being carbon dioxide
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25JLIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2245/00Processes or apparatus involving steps for recycling of process streams
    • F25J2245/02Recycle of a stream in general, e.g. a by-pass stream
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02CCAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C10/00CO2 capture or storage
    • Y02C10/12Capture by rectification and condensation

Abstract

A process and apparatus for reducing a concentration of sour species in a gas to a predetermined residual concentration is provided. The process involves cooling the sour gas in a manner to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species. A cooled gas is separated from the mixture. The residual concentration of sour species in the cooled gas is then determined. When the residual concentration of sour species in the cooled gas is above the predetermined concentration, the cooled gas is compressed and the preceding process is repeated until the residual concentration of sour species in the cooled gas is at or below the desired concentration.

Description

PROCESS AND APPARATUS FOR REDUCING THE CONCENTRATION OF A

SOUR SPECIES IN A SOUR GAS

Field

The present invention relates to a process and apparatus for reducing the concentration of sour species in a gas stream. In particular, the present invention relates to a process and apparatus for reducing the concentration of sour species in a gas in which the sour species are repeatedly removed in a solid and/or a liquid phase until a predetermined residual concentration of sour species in the gas is attained. Background

Global energy demand is projected to increase by almost 3% annually over the next twenty-five years. The increasing demand for the usage of light hydrocarbons, such as methane, as a primary energy source is driving the development of natural gas fields that had previously been considered sub- economic, including those containing significant concentrations of carbon dioxide. Additionally, methane is increasingly being sourced from coal bed and coal seam mining operations, associated gas stream sources, and anthropogenic sources such as landfill gas and biogas.

Although hydrocarbon gas combustion produces significantly lower carbon dioxide emissions than oil or coal, the advantage is lessened or even negated if the carbon dioxide removed in pre-combustion gas processing plants is vented to the atmosphere instead of being captured and stored, for example in sub-surface geological formation. Additionally, the presence of water and other compounds such as hydrogen sulphide, mercaptans, and mercury which are also referred to as "sour" species or contaminants found in hydrocarbon gas, regardless of the sources listed above, is also problematic . Water and sour contaminants promote corrosion within gas pipework and form solids under conditions commonly found in process operations and distribution networks . The formation of solids in pipe work or equipment is generally undesirable, as the accumulation of such solids eventually results in decreased operating performance and can quickly lead to total blockage, breakdown or other damage. For safety and operational reasons it is necessary to reduce concentrations of water and sour contaminants down to acceptable concentrations .

Additionally, it is necessary to comply with legal or commercial requirements concerning maximum allowable concentrations of sour contaminants within a hydrocarbon gas product stream.

Several patents discuss the separation of carbon dioxide from natural gas streams through the formation of solid carbon dioxide followed by controlled melting of the solids, such as for example as described in US Patent No. 5,819,555 by Engdahl et al., and in International Publication Nos . WO 2004/070297, and WO2007/030888. However, these all describe single stage operations, and when gas stream contains high concentrations of sour contaminants (i.e. > about 20%), it is difficult to obtain sweetened gas using these processes. The present invention seeks to overcome at least some of the aforementioned disadvantages.

Summary

In its broadest aspect, the invention provides a process and apparatus for reducing a concentration of sour species in a gas in which the sour species are repeatedly removed in a solid and/or liquid phase until a predetermined residual concentration of sour species is attained.

Accordingly, in a first aspect of the present invention there is provided a process for reducing a concentration of sour species in a sour gas comprising hydrocarbons and sour species to a concentration at or below a predetermined concentration of sour species, the process comprising the steps of:

a) cooling the sour gas in a first cooling zone in a manner to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species;

b) separating the solid and/or liquid sour species from the mixture, thereby producing a cooled gas having a residual concentration of sour species;

c) determining the residual concentration of sour species in the cooled gas; and,

d) when the residual concentration of the sour species in the cooled gas is above the predetermined concentration,

e) compressing the cooled gas; and

f) repeating steps a) to e) until the residual concentration of sour species in the cooled gas is at or below the desired concentration. The predetermined concentration of sour species may vary depending on the intended purpose of the gas and the concentration of sour species that is desirable or acceptable for that purpose. For example, if the gas must meet pipeline specifications, the predetermined concentration of sour species may be about 2%-4%, whereas the predetermined concentration of sour species in a gas which is to be liquefied may be about 50 ppm - 200 ppm. In one embodiment of the invention, at least a portion of the compressed gas may be re-directed to the first cooling zone where steps a) to c) are repeated. In a preferred embodiment the re-directed compressed gas is blended with the sour gas in a proportional manner whereby the sour species concentration of the resulting blended gas is below about 20 mole%.

In one form of the invention, the compressed gas may be blended with the sour gas before cooling the blended gas in the first cooling zone.

In an alternative form of the invention, the compressed gas may be blended with the sour gas in the first cooling zone. In this form, the compressed gas and the sour gas are introduced separately to the first cooling zone.

In an alternative form, the compressed gas and the sour gas are introduced separately to the separator in step b) . It will be appreciated that in the latter alternative form, the compressed gas may be cooled prior to introducing the compressed gas to the separator. It will be appreciated that blending the compressed gas with the sour gas results in a lower sour species concentration in the blended gas in comparison to the concentration of sour species in the sour gas, leading to lower residual sour species concentrations in the resulting cooled gas. For a given Joule-Thomson expansion, a feed gas with a lower sour species concentration will result in a lower final temperature, therefore affording a vapour phase with a lower residual sour species concentration. In comparison, for the same magnitude Joule-Thomson expansion, a gas with a higher sour species concentration will result in a relatively- higher final temperature, affording a vapour phase with a higher residual sour species concentration.

In an alternative embodiment of the invention, the compressed gas may be directed to a subsequent downstream cooling zone where steps a) to c) are repeated. The subsequent downstream cooling zone may operate under a different set of temperature and pressure conditions than the first cooling zone or a preceding cooling zone. It will be appreciated that the temperature to which the compressed gas is cooled to obtain solid and/or liquid sour species will be dictated by the composition of the compressed gas.

In a further alternative embodiment of the invention, at least a portion of the compressed gas treated in the subsequent cooling zone may be re-directed to said subsequent cooling zone where steps a) to c) are repeated. The re-directed stream may be optionally blended with a portion of compressed gas treated in the first cooling zone or another gas having a residual sour gas concentration in a proportional manner whereby the sour species concentration of the blended gas is below about 20 mole%. From the foregoing description, it will be understood that the process of the present invention is suitable to sweeten a sour gas feed having a sour species concentration of greater than about 20 mole%. Depending on the composition of the sour gas it may be necessary to repeat steps a) to e) of the above process one or more times to achieve the predetermined concentration of sour species that is desired.

In instances where the residual concentration of sour species in the cooled gas stream is at or below the predetermined concentration of sour species, but still above desirable concentrations suitable for hydrocarbon liquefaction, the cooled gas may be treated by a further process to reduce the residual concentration of sour species to acceptable concentrations for hydrocarbon liquefaction. For example, in one embodiment of the invention, the process may further comprise the step of treating the cooled gas with a liquid solvent, optionally at or below the temperature of the cooled gas . One such process is described in International Publication No. WO 2007/030888. The solvent treated gas containing ppm level sour contaminants can then be liquefied using various refrigeration schemes to produce LNG. Preferably, the sour gas that is used in the present process has been dehydrated. Generally the dehydrated gas has a water content of less than 50 ppm, and preferably less than 7 ppm for pipeline specification gas, and a water content of less than 1 ppm for LNG specification gas. Any suitable process for dehydrating the sour gas can be used. An example of a suitable dehydration process includes the adsorption of water from the sour gas with molecular sieves or silica gel. Alternatively, dehydration by absorption using glycol or methanol may be possible, or other suitable dehydration processes known in the art . In step a) , cooling is conducted under a set of temperature and pressure conditions at which the sour species solidifies and/or a liquid condensate of sour species forms . It will be appreciated that said set of temperature and pressure conditions will vary in accordance with the composition of the sour gas, compressed gas, or blended gas.

In one form of the invention, the step of cooling the sour gas comprises expanding the sour gas in one or more expansion steps. In an alternative form of the invention, the step of cooling the sour gas comprises effecting an indirect heat exchange with one or more cooling streams. Suitable cooling streams may be a process stream at a lower temperature than the sour gas or an external refrigerant stream. In another alternative form the step of cooling the sour gas comprises effecting a direct heat exchange with a cooling stream. In a preferred form of the invention, the step of cooling the sour gas comprises one or more heat exchange and/or expansion steps.

In another embodiment of the invention, the step of separating the solid and/or liquid sour species from the mixture is conducted under gravity, centrifugal force, or with other suitable separation means.

In one embodiment of the invention, the step of determining the residual concentration of sour species in the cooled gas may comprise determining an actual residual concentration of sour species in the cooled gas stream. Determining the actual residual concentration may be performed, for instance, by sampling the cooled gas and measuring the residual concentration of sour species with a sensor which is sensitive to the sour species.

In an alternative embodiment of the invention, the step of determining the residual concentration of sour species in the cooled gas may comprise determining a theoretical residual concentration of sour species in the cooled gas. Determining the theoretical residual concentration may be performed, for instance, by modeling the concentrations of components in the cooled gas under a set of temperature and pressure conditions for a given gas composition by implementing a purpose-built C02 solid phase quantification algorithm in a commercially available process simulation software. Illustrative examples of such process simulation software include AspenHYSYS™. In this way, modeling may conveniently predict the number of times the sour gas may have to be cooled to produce a residual concentration of sour species at or below the predetermined concentration of sour species in the cooled gas. As the composition of the cooled gas progressively changes, in particular as the residual concentration of sour species approaches the desired predetermined concentration of sour species and the relative concentration of hydrocarbons increases, modeling may also predict the temperature to which the compressed gas should be cooled in a subsequent cooling step.

In one embodiment of the invention, the step of compressing the cooled gas is performed using a compressor .

In some embodiments the process further comprises the step of removing the solid sour species, preferably by heating and melting the solid sour species, thereby producing a liquid rich in sour species. The resultant liquid sour species may be subsequently removed and diverted to other parts of the plant. For example, a cool liquid carbon dioxide stream may be used as one of the process streams to cool the gas stream in step a) by indirect heat exchange .

In one embodiment, the process comprises heating the solid sour species to a temperature at or just above the melting point of the solid sour species.

In a second aspect of the present invention there is provided an apparatus for reducing a concentration of sour species in a sour gas comprising hydrocarbons and sour species to a concentration at or below a predetermined concentration of sour species, the apparatus being provided with:

a first cooling zone for cooling the sour gas to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species, the cooling zone being in fluid communication with a source of sour gas; a separator for separating solid and/or liquid sour species from the mixture, thereby producing a cooled gas having a residual concentration of sour species;

a means for determining the residual concentration of sour species in the cooled gas;

a compressor configured to compress the cooled gas when the residual concentration of the sour species in the cooled gas stream is above a predetermined concentration of sour species;

optionally, one or more subsequent cooling zones for cooling the compressed gas stream to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species associated with one or more separators and compressors; and

a means to re-direct the compressed gas stream to the first cooling zone or, optionally, the one or more subsequent cooling zones. In one embodiment of the invention, the means to re-direct the compressed gas is configured to receive an amount of sour gas so as to blend the compressed gas with sour gas.

In one embodiment, the cooling zones comprise one or more cooling means for cooling the sour gas. In one form of the invention said cooling means may be a gas expander. Suitable examples of gas expanders include, but are not limited to, a Joule-Thompson valve, an orifice or venturi tube, a turbo expander, or a turbo expander in sequential combination with a Joule-Thompson valve. It will be appreciated that the gas expander can define an inlet of a vessel for cooling the sour gas or an inlet of the separator. Similarly, it will be understood that the separator may additionally function as a cooling vessel in which the sour gas is cooled.

In another form of the invention said cooling means may be a heat exchanger configured to facilitate indirect heat exchange with one or more cooling streams. Suitable examples of said heat exchangers include, but are not limited to, plate and fin type heat exchanger, tube-in- shell type heat exchanger, cooling coil, or coiled bundle. It will be appreciated that the cooling streams may be a process stream produced upstream or downstream of the heat exchanger, or an external refrigerant stream in fluid communication with an external refrigeration system. Exemplary types of external refrigeration systems include cascading refrigeration systems, single mixed refrigerant systems, double mixed refrigerant systems, ammonia absorption chillers, and so forth.

In another form of the invention said cooling means may be configured to facilitate direct heat exchange with a cooling stream.

In a preferred form of the invention, first cooling zone and, optionally, the subsequent cooling zones are respectively provided with one or more heat exchangers and/or gas expanders .

In one embodiment of the invention, the means for determining the residual concentration of sour species in the cooled gas may comprise a means for determining an actual residual concentration of sour species in the cooled gas. A suitable example of such means includes, but is not limited to, a sensor which is capable of measuring the amount of sour species in the cooled gas.

In an alternative embodiment of the invention, the means for determining the residual concentration of sour species in the cooled gas may comprise a means for determining a theoretical residual concentration of sour species in the cooled gas. A suitable example of such means may include, but is not limited to, a modeling computer program to model the concentrations of components in the cooled gas under a set of temperature and pressure conditions for a given gas composition. In this way, modeling may conveniently predict the number of cooling zones required in the apparatus to produce the cooled gas having a residual concentration of sour species at or below the predetermined concentration of sour species. It will also be appreciated, that as the composition of the cooled gas stream progressively changes as it is cooled in each subsequent cooling zone, in particular as the residual concentration of sour species approaches the predetermined concentration of sour species and the relative concentration of hydrocarbons increases, modeling may also predict the operating temperature and conditions under which each cooling zone operates.

In another embodiment, the apparatus further comprises a means for heating the solid sour species to a temperature at or just above the melting point of the solid sour species. In one form of the invention, said heating means is a heater, in particular an immersion heater.

In still another embodiments, the apparatus further

comprises a liquid gas contactor for testing the cooled gas with a liquid solvent, optionally at or below the temperature of the cooled gas .

Brief Description of the Figures

Preferred embodiments of the present invention will now be described, by way of example only, with reference to the accompanying figures, in which:

Figure 1 shows a process flow diagram in accordance with one embodiment of the present invention; and,

Figure 2 shows a process flow diagram in accordance with a further embodiment of the present invention.

Description of a Preferred Embodiment

In the description of the Figures reference is made to a natural gas stream as an example of the sour gas that may be treated in the process according to the present invention. It will be appreciated, however, that the sour gas may be any gas that comprises hydrocarbons and sour species. Illustrative examples of such sour gases include, but are not limited to, natural gas, coal seam gas, associated gas, landfill gas, and biogas. The composition of the sour gas may vary significantly but the sour gas will generally contain methane, ethane, higher hydrocarbons (C3+) , water, and other sour species. The term "sour species" means any one or more of carbon dioxide, hydrogen sulphide, carbon disulfide, carbonyl sulphide, mercaptans (R-SH, where R is an alkyl group having one to 20 carbon atoms) , sulphur dioxide, aromatic sulphur-containing compounds, and aromatic hydrocarbons such as benzene, toluene, xylene, naphthalenes, and so forth. Referring to Figure 1, there is shown an apparatus 10 in accordance with one embodiment for performing the process of the present invention. A sour feed gas is introduced to the apparatus 10 via a line 1 to a dehydrating unit 12 where it is dehydrated. The sour feed gas may be dehydrated by any suitable dehydration process. Following dehydration, the sour feed gas is passed from the dehydrating unit 12 via line 2 to a cooling zone 14. The cooling zone 14 includes a heat exchanger 16, a chiller 18, an expander valve (or other expansion device) 24, and a separator vessel 20.

The sour feed gas is directed to heat exchanger 16 and subsequently to chiller 18 via line 3 to cool the sour feed gas to a temperature marginally greater than a temperature at which solidification of the sour species in the sour feed gas occurs. Generally, the sour feed gas is cooled to a temperature in a range of about -65 °C - -70 °C. Cooling in heat exchanger 16 may be obtained from indirect heat exchange with process streams derived downstream in the apparatus 10, such as for instance, liquid carbon dioxide, or refrigerant streams from an external refrigeration system. Similarly, the chiller 18 may be a refrigerated cold box where cooling is provided by an external refrigeration system, such as for example, a propane-ethylene cascade refrigeration system. Such cooling means as described above are well known and used by persons skilled in the art. The sour feed gas is then fed via line 4 to an inlet 22 of separator vessel 20. The sour feed gas is expanded using a Joule-Thompson valve 24 or other suitable expansion means such as a turbo expander to further cool the sour feed gas as it enters the separator vessel 20.

The process of expanding the sour feed gas upon introduction to the separator vessel 20 is arranged to afford temperature and pressure conditions within the separator vessel 20 at which the sour species contained in the sour feed gas solidify and/or liquefy. The process of expansion typically cools the sour feed gas entering the separator vessel 20 at inlet 22 to about -75 to -95 °C at a typical pressure range of 15 to 20 bar.

Upon cooling the sour feed gas, as described above, a small amount of condensate of NGL may also form under the temperature and pressure conditions in the separator vessel 20.

The solid and/or liquid sour species and the condensate migrate to a lower portion of the separator vessel 20 under gravity separation, thereby forming a slurry of natural gas liquids and solid sour species. In other embodiments, separation may be achieved or enhanced by the use of centrifugal force or inlet devices designed to coalesce droplets or agglomerate solid particles .

The slurry of solid sour species is then heated to a temperature at least marginally greater than the solidification temperature of the solid sour species to convert the solid sour species to a liquid phase in the lower portion of the separator vessel 20 and afford a liquid rich in the sour species. The nature and concentration of the sour species in the liquid phase is highly dependant on the composition of the sour feed gas. In some embodiments, concentrations of carbon dioxide in the liquid phase may be > 70 mole%, and often > 90 mole%. Typically, the separator vessel 20 is provided with an immersion heater (not shown) which heats the slurry up to a temperature marginally greater than the melting point temperature of the solid sour species. The immersion heater may be a heat exchanger tube bundle which affords cooling of the sour feed gas or other process streams while heating the slurry. In small applications, the heater may be supplied by electricity.

The liquid rich in the sour species is removed from the separator vessel 20 through conduit 5. Under processing conditions where the liquid is rich in liquid carbon dioxide, the liquid may be directly pumped via pump 28 to a liquid carbon dioxide sequestration site, or disposed of for retail sale. Prior to sequestration or storage, the liquid rich in sour species may be used as a cooling stream in any one or more of the heat exchangers of the apparatus 10, such as for example heat exchanger 16, to conserve energy within the apparatus 10.

The resulting cooled gas which has been depleted of sour species may also be diverted from the separator vessel 20 via line 6 for use as a cooling stream in any one or more of the heat exchangers of the apparatus 10, such as for example heat exchanger 16, to conserve energy within the apparatus 10. A large proportion (typically about 50-80 mole%) of the sour species in the sour feed gas will have been solidified and/or liquefied in the separator vessel 20, but depending on the composition of the sour feed gas, the concentration of sour species remaining in the cooled gas may be above a desired predetermined concentration. The residual concentration of sour species in the cooled gas is determined, either by modeling or with sensors sensitive for the sour species.

When the residual concentration of the sour species in the cooled gas is at or below the predetermined concentration of sour species, the cooled gas may be passed via line 8 from the compressor 30 to sales gas export.

If, on the other hand, the residual concentration of the sour species in the cooled gas is above the desired predetermined concentration of sour species then, following compression in compressor 30, a portion of the cooled gas is recycled via line 7 to the cooling zone 14 where it is blended with incoming sour feed gas, thereby diluting the sour species concentration therein. The amount of cooled gas that is recycled and blended may be selected on the basis that the operating conditions within separator vessel 20 result in a subsequent cooled gas having a sour species at or below the determined concentration .

In the arrangement described above, the cooled compressed gas is re-directed via line 7 to the first cooling zone 14 and passes through the heat exchanger 16, chiller 18, and expander 24. It will be appreciated, however, that in alternative arrangements (not shown) the cooled compressed gas may be introduced at any point in the first cooling zone 14. Alternatively, the cooled compressed gas may be cooled externally of the first cooling zone 14 and redirected to the separator vessel 20 in an arrangement whereby it is blended with sour feed gas in separator vessel 20. The amount of cooled compressed gas that is re-directed and blended with the sour feed gas in separator vessel 20 may be selected on the basis that the operating conditions within separator vessel 20 produce a cooled gas having a sour species at or below the predetermined concentration.

Referring now to Figure 2, where like numerals refer to like features throughout, there is shown an apparatus 10" in accordance with an alternative embodiment for performing the process of the present invention.

A sour feed gas is introduced to the apparatus 10" via a line 1 to a dehydrating unit 12 where it is dehydrated as described previously. Following dehydration, the sour feed gas is passed from the dehydrating unit 12 via line 2 to a first cooling zone 14 which includes a heat exchanger 16, a chiller 18, an expansion device 24 and a separator vessel 20.

The sour feed gas is directed to heat exchanger 16 and subsequently to chiller 18 via line 3 to cool the sour feed gas to a temperature marginally greater than a temperature at which solidification of the sour species in the sour feed gas occurs, as described previously.

The sour feed gas is then fed via line 4 to an inlet 22 of separator vessel 20. The sour feed gas is expanded using a Joule-Thompson valve 24 or other suitable expansion means such as a turbo expander to further cool the stream as it enters the separator vessel 20. The process of expanding the sour feed gas upon introduction to the separator vessel 20 is arranged to afford temperature and pressure conditions within the separator vessel 20 at which the sour species contained in the sour feed gas solidify and/or liquefy. The process of expansion typically cools the sour feed gas entering the separator vessel 20 at inlet 22 to about -80 to -95 °C at a typical pressure range of 15 to 25 bar.

A slurry of solid sour species and/or liquid sour species accumulates in the lower portion of the separator vessel 20. Any solid sour species may be melted within the separator vessel 20 by heating and a liquid stream rich in sour species is removed from the separator vessel 20 through conduit 5. It may be used as a cooling stream in any one or more of the heat exchangers of the apparatus 10", such as for example heat exchanger 16, to conserve energy within the apparatus 10", before being pumped via pump 28 to a liquid carbon dioxide sequestration site, or disposed of for retail sale.

A cooled gas is separated in the separator vessel 20 and the residual concentration of sour species therein is determined either by modelling or with sensors sensitive for the sour species.

When the residual concentration of the sour species in the cooled gas is above the predetermined concentration of sour species, the cooled gas is passed via line 8 to compressor 30. The compressed cooled gas is then passed from the compressor 30 to a second cooling zone 40 via line 15. The second cooling zone includes a heat exchanger 42, a chiller 44, an expansion device 50 and a separator vessel 46.

The compressed cooled gas is directed to heat exchanger 42 and subsequently to chiller 44 via line 17 to cool the compressed cooled gas to a temperature marginally greater than a temperature at which solidification of the sour species in the compressed cooled gas occurs, as described previously. The compressed cooled gas is then fed via line 19 to an inlet 48 of separator vessel 46. The compressed cooled gas is expanded using the expansion device 50 such as a Joule-Thomson valve, turbo expander, or other suitable expansion means to further cool the gas as it enters the separator vessel 46.

The temperature and pressure conditions within the separator vessel 46 are arranged to solidify and/or condense the sour species contained in the compressed cooled gas introduced into the separator vessel 46. The process of expansion typically cools the compressed cooled gas entering the separator vessel 46 at inlet 48 to about -65 to -95 °C at a pressure range of 15 to 25 bar. Under these conditions, a slurry of solid sour species and/or liquid sour species accumulates in the lower portion of the separator vessel 46. Any solid sour species may be melted within the separator vessel 46 by heating and a liquid stream rich in sour species is removed from the separator vessel 46 through conduit 21. The liquid stream rich in sour species may be used as a cooling stream in any one or more of the heat exchangers of the apparatus 10", such as for example heat exchanger 42, to conserve energy within the apparatus 10", before being pumped via pump 54 to a liquid carbon dioxide sequestration site, or disposed of for retail sale.

The cooled sweetened gas produced in separator vessel 46 may also be used as a cooling stream in any one or more of the heat exchangers of the apparatus 10", such as for example heat exchangers 16, 42 to conserve energy within the apparatus 10".

The residual concentration of sour species in the cooled sweetened gas is determined either by modeling or with sensors sensitive for the sour species. When the residual concentration of the sour species in the cooled sweetened gas is at or below a predetrmined concentration of sour species, the cooled sweetened gas is compressed in compressor 56 and then passed to sales gas export via line 23.

If the residual concentration is above the predetermined concentration then a portion of the cooled sweetened gas is recycled via line 6 and compressor 30 to the inlet of the second cooling zone 40. The amount of cooled sweetened gas that is recycled and blended may be selected on the basis that the operating conditions within separator vessel 46 results in a cooled gas having a sour species at or below the predetermined concentration. Now that particular embodiments have been described, it will be appreciated that some embodiments have some of the following advantages:

· the processes and apparatus of the present invention are suitable for treatment of sour gases with high carbon dioxide content, in particular sour gas from gas fields which were previously economically

unviable to develop because of the high capital and operation expenditure associated with carbon dioxide separation; and

• carbon dioxide is separated in liquid form suitable for sequestration as opposed to being vented into the atmosphere as with conventional solvent extraction and/or membrane separation techniques.

In the description of the invention, except where the context requires otherwise due to express language or necessary implication, the words "comprise" or variations such as "comprises" or "comprising" are used in an inclusive sense, i.e. to specify the presence of the stated features, but not to preclude the presence or addition of further features in various embodiments of the invention.

It is to be understood that, although prior art use and publications may be referred to herein, such reference does not constitute an admission that any of these form a part of the common general knowledge in the art, in Australia or any other country. Numerous variations and modifications will suggest themselves to persons skilled in the relevant art, in addition to those already described, without departing from the basic inventive concepts. All such variations and modifications are to be considered within the scope of the present invention, the nature of which is to be determined from the foregoing description.

Claims

Claims defining the invention are as follow:
A process for reducing a concentration of sour species in a sour gas comprising hydrocarbons and sour species to a concentration at or below a predetermined concentration of sour species, the process comprising the steps of :
a) cooling the sour gas in a first cooling zone in a manner to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species; b) separating the solid and/or liquid sour species from the mixture, thereby producing a cooled gas having a residual concentration of sour species;
c) determining the residual concentration of sour species in the cooled gas; and,
d) when the residual concentration of the sour species in the cooled gas is above the predetermined concentration,
e) compressing the cooled gas stream; and
f) repeating steps a) to c) until the residual concentration of sour species in the cooled gas stream is at or below the predetermined concentration.
The process according to claim 1, wherein at least a portion of the compressed gas is re-directed to the first cooling zone where steps a) to c) are repeated.
The process according to claim 1, wherein the compressed gas is directed to a subsequent downstream cooling zone where steps a) to c) are repeated.
4. The process according to claim 3, wherein at least a portion of the compressed gas treated in the subsequent cooling zone is re-directed to said subsequent cooling zone where steps a) to c) are repeated.
5. The process according to claim 2 or claim 4, wherein the re-directed compressed gas is blended with a sour gas stream or a gas stream containing residual sour species.
6. The process according to claim 5, wherein the sour species concentration of the blended gas is below about 20 mole%.
7. The process according to claim 5 or claim 6, wherein the compressed gas stream' is blended before cooling the blended gas stream.
8. The process according to claim 5 or claim 6, wherein the compressed gas stream is blended in said cooling zone .
9. The process according to claim 8, wherein the compressed gas and the sour gas, or the gas stream containing residual sour species, are introduced separately to said cooling zone.
10. The process according to any one of the preceding claims further comprising the step of treating the cooled gas with a liquid solvent, optionally at or below the temperature of the cooled gas. The process according to any one of the preceding claims, wherein the step of determining the residual concentration of sour species in the cooled gas stream comprises determining an actual residual concentration of sour species in the cooled gas.
The process according to claim 11, wherein determining said actual residual concentration comprises sampling the cooled gas and measuring the residual concentration of sour species with a sensor which is sensitive to the sour species.
The process according to any one of claims 1 to 10, wherein the step of determining the residual concentration of sour species in the cooled gas comprises determining a theoretical residual concentration of sour species in the cooled gas by modeling the concentrations of components in the cooled gas under a set of temperature and pressure conditions for a given gas composition with process simulation software.
The process according to any one of the preceding claims, wherein the process further comprises the step of removing the solid sour species by heating and melting the solid sour species, thereby producing a liquid rich in sour species.
An apparatus for reducing a concentration of sour species in a sour gas comprising hydrocarbons and sour species to a concentration at or below a predetermined concentration of sour species, the apparatus being provided with: a first cooling zone for cooling the sour gas to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species, the cooling zone being in fluid communication with a source of sour gas;
a separator for separating solid and/or liquid sour species from the mixture, thereby producing a cooled gas having a residual concentration of sour species; a means for determining the residual concentration of sour species in the cooled gas;
a compressor configured to compress the cooled gas when the residual concentration of the sour species in the cooled gas is above a desired concentration of sour species;
optionally, one or more subsequent cooling zones for cooling the compressed gas to produce a mixture of solid and/or liquid sour species and a vapour containing gaseous hydrocarbons and a residual amount of sour species associated with one or more separators and one or more compressors; and
a means to direct the compressed gas to the first cooling zone or, optionally, to the one or more subsequent cooling zones.
The apparatus according to claim 15, wherein the means for determining the residual concentration of sour species in the cooled gas may comprise a means for determining an actual residual concentration of sour species in the cooled gas.
The apparatus according to claim 15, wherein the means for determining the residual concentration of sour species in the cooled gas may comprise a means for determining a theoretical residual concentration of sour species in the cooled gas.
The apparatus according to any one of claims 15 to 17, wherein the means to redirect the compressed gas is configured to receive an amount of sour gas so as to blend the compressed gas with the sour gas .
The apparatus according to any one of claims 15-18, wherein the apparatus further comprises a means for heating the solid species to a temperature at or just above the melting point of the sold sour species.
The apparatus according to any one of claims 15 to 19, wherein the apparatus further comprises a liquid-gas contactor for treating the cooled gas with a liquid solvent, optionally at or below the temperature of the cooled gas .
The apparatus according to any one of claims 15 to 19, wherein the first cooling zone and optionally, the one or more subsequent cooling zones comprise one of more cooling means for cooling the sour gas.
The apparatus according to claim 21, wherein the cooling means comprises a gas expander.
23. The apparatus according to claim 22, wherein the gas expander defines an inlet of a vessel for cooling the sour gas .
24. The apparatus according to claim 22, wherein the gas expander defines an inlet of the separator.
25. The apparatus according to claim 21, wherein the cooling means comprises a heat exchanger.
26. The apparatus according to any one of claims 22 to 25, wherein the first cooling zone and optionally, the one or more subsequent cooling zones are respectively provided with one or more heat exchangers and/or gas expanders .
PCT/AU2010/001063 2009-09-01 2010-08-19 Process and apparatus for reducing the concentration of a sour species in a sour gas WO2011026170A1 (en)

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