WO2006117499A1 - Synthesis gas production process - Google Patents

Synthesis gas production process Download PDF

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WO2006117499A1
WO2006117499A1 PCT/GB2005/001672 GB2005001672W WO2006117499A1 WO 2006117499 A1 WO2006117499 A1 WO 2006117499A1 GB 2005001672 W GB2005001672 W GB 2005001672W WO 2006117499 A1 WO2006117499 A1 WO 2006117499A1
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synthesis gas
reformer
gas
production
synthesis
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PCT/GB2005/001672
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French (fr)
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Alexander H. Quartey-Papafio
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Quartey-Papafio Alexander H
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    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
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    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0244—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being an autothermal reforming step, e.g. secondary reforming processes
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    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0838—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel
    • C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
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    • C01B2203/82—Several process steps of C01B2203/02 - C01B2203/08 integrated into a single apparatus

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Abstract

A method of producing synthesis gas which employs three reforming technologies namely Adiabatic Pre-Reformer (APR), Steam-Methane Reformer (SMR) and Autothermal or Partial Oxidation Reformer (ATR or POX), arranged in a unique configuration with operating conditions of each reformer selected and key parameters of the process fixed to produce synthesis gas with the optimise composition for Fischer-Tropsch Liquids, Methanol or Ammonia production.

Description

SYNTHESIS GAS PRODUCTION PROCESS
BACKGROUND OF THE INVENTION
[0001] This invention relates to a method of producing synthesis gas which when used as feedstock to the synthesis section of synthesis gas based plants such as Fischer-Tropsch, Methanol or Ammonia plants will enable significant increases in plant capacities coupled with improved plant efficiencies than currently achieved with present processes.
[0002] The synthesis gas production process employs three reforming technologies, arranged in a unique configuration to produce synthesis gas with the optimum composition for Fischer-Tropsch liquids, Methanol or Ammonia production.
DESCRIPTION OF DRAWINGS
[0003] Figure 1 outlines a simplified block flow diagram of producing synthesis gas using a Single Reforming Process (Prior Act).
[0004] Figure 2 outlines a simplified block flow diagram of producing synthesis gas using a Combined Reforming Process (Prior Act).
[0005] Figure 3 outlines a simplified block flow diagram of producing synthesis gas using the present invention.
DESCRIPTION OF PRIOR ART
[0006] The feedstock to the synthesis section of any synthesis gas based plant such as Fischer-Tropsch, Methanol or Ammonia plant is a gas containing H2, CO2, CO, CH4, N2 and H2O. This is coined synthesis gas or "syngas" and is produced by catalytic or non-catalytic processing a hydrocarbon based feedstock such as natural gas. At the heart of this processing unit (commonly known as the front end of the synthesis gas based plant) is the reformer where the hydrocarbon based feedstock is chemically broken down into the said components using water vapour, oxygen, enriched air or atmospheric air. Examples of reforming technologies used presently in synthesis gas production processes include:
> Pre-Reformer
> Steam-Methane Reformer
> Autothermal Reformer
> Partial Oxidation Reformer
> Gas Heated Reformer
> Compact Reformer
[0007] The performance of the front end section of these plants are very crucial to the overall performance of the plant and command a high percentage of the total capital cost of the plant. As a result, various front end processes for syngas based plants have been developed and commercialised over the years. Majority of these processes can be classified into either a single or combined reforming processes depending on the number of reforming technologies used. A brief description of these processes are outlined below:
SINGLE REFORMING PROCESS
[0008] For better understanding of this process, the following description should be read in conjunction with Figure 1.
[0009] Hydrogen, hydrogen rich containing gas from the synthesis section of the plant in question or imported from an external source 102 is added to natural gas feedstock 101 and the mixture 103 is heated up and desulphurised in a typical Desulphurisation Unit 201 to remove any sulphur compounds present in the natural gas.
[0010] The desulphurised gas 104 is then fed to the Saturator 202 where it is contacted with hot water (not shown) and leaves saturated with water vapour 105. Supplementary water vapour 106 is added to the saturated gas 105 to achieve a desired steam to carbon ratio. The mixture 107 is heated up and routed to the Reformer 203 were the hydrocarbons present in the natural gas reforms to produce hydrogen, carbon monoxide and carbon dioxide in the presents of water vapour or oxygen from an oxygen containing stream 108 such as pure oxygen, enriched air or atmospheric air.
[0011] The reformed gas 109 is cooled down by generating high pressure water vapour and depending on the plant in question, conditioned by shifting carbon monoxide, removing carbon dioxide and/or methanating carbon oxides in 204. The conditioned gas coined syngas 110 is cooled down further to remove water vapour in 205. Alternatively, the conditioned gas is fed to a Desaturator 205 where it is contacted with cold water (not shown) to remove the water vapour 112 present in it. The resulting dry gas 111 is fed to the synthesis section of a Fischer-Tropsch, Methanol or Ammonia Plant for further processing.
[0012] From the list of reforming technologies outlined earlier, the steam-methane, autothermal, partial oxidation and compact reformers can be used as reformers in this type of reforming process.
COMBINED REFORMING PROCESS
[0013] For better understanding of this process, the following description should be read in conjunction with Figure 2.
[0014] Similar to the single reforming process, hydrogen, hydrogen rich containing gas from the synthesis section of the plant in question or imported from an external source 102 is added to natural gas feedstock 101 and the mixture 103 is heated up and desulphurised in a typical Desulphurisation Unit 201 to remove any sulphur compounds present in the natural gas. [0015] The desulhurised gas 104 is then fed to the Saturator 202 where it is contacted with hot water (not shown) and leaves saturated with water vapour 105. Supplementary water vapour 106 is added to the saturated gas 105 to achieve a desired steam to carbon ratio. The mixture 107 is heated up and routed to the first of two reformers 203 where part of the hydrocarbons present in the natural gas reforms to produce hydrogen, carbon monoxide and carbon dioxide. The partly reformed gas 108 is then fed to a second reformer 204 where the reforming process is completed using oxygen, enriched air or atmospheric air 109.
[0016] Alternatively, a portion of the desulphurised gas 104 or saturated gas 105 is mixed with the effluents from the first reformer 203 and introduced to the second reformer 204 where the mixture is processed to completion 110 using oxygen, enriched air or atmospheric air 109 as described earlier. This alternative route has not been shown on Figure 2.
[0017] Depending on the combination of reforming technologies employed, the reformed gas 110 from the second reformer 204 is routed to the first reformer 203 to provide the heat required for reforming and leaves colder as 111.
[0018] The cooled reformed gas or the reformed gas from the secondary reformer 112 is cooled down by generating high pressure water vapour and depending on the plant in question, conditioned by shifting carbon monoxide, removing carbon dioxide and or methanating carbon oxides in 205. The conditioned gas coined syngas 113 is cooled down further to remove water vapour 115 in 206. The resulting dry gas 114 is fed to the synthesis section of a Fischer-Tropsch, Methanol or Ammonia Plant for further processing.
[0019] Alternatively, the conditioned gas is fed to a Desaturator 206 where it is contacted with cold water (not shown) to remove the water vapour present in it. The resulting dry gas 114 is fed to the synthesis section of the plants as described in the preceding paragraph for further processing.
[0020] The steam-methane, autothermal and partial oxidation reformers can be used in this reforming process with each other or with either the gas heated reformer or pre-reformer.
[0021] The single and combined reforming processes outlined in the preceding paragraphs do however have inherited drawbacks some affecting it's performance (i.e. composition of syngas produced which translate to the plants overall performance) and others limiting the capacity of the synthesis gas based plant to which it is supplying syngas. Some of these drawbacks are:
> Operating envelop of Reformers - steam to carbon ratio, operating temperatures and pressures.
> Excess production of byproducts - steam.
> Design envelop of Reformers - size, dimension, design temperatures and pressures
> Size of key equipment - heat exchangers (boilers), pressure vessels and burners
> Size of key pipe lines - refractory lined and high pressure steam pipelines. [0022] As a results of some of these drawbacks, current production capacity of Fischer- Tropsch, Methanol and Ammonia plants are limited as follows:
Fischer-Tropsch Plants
[0023] Although Fischer-Tropsch technology and plants have been around for more than 50 years, it is still considered as an emerging technology and only a small number of plants of commercial capacity are presently on stream, however the most commonly used reforming technology employed in the synthesis section of today's plants are either steam-methane, autothermal or partial oxidation reformers.
[0024] The maximum synthesis gas production from a single train of partial oxidation reformer will enable maximum plant production capacity (i.e. C5 and above hydrocarbon) of about 8,000 BPD. This increases to 10,000 BPD for a steam-methane reformer scheme and to between 15,000 -17,000 BPD when an autothermal reformer is employed.
Methanol Plants
[0025] The most commonly reforming technology used for the synthesis production section of today's methanol plants are either steam-methane reformers, a combination of pre-reformer and steam-methane reformer, a combination of steam-methane reformer and autothermal reformer or a combination of autothermal and gas heated reformer.
[0026] The use of steam-methane reformer based technology restricts the capacity of methanol plants to between 3750 to 4250 MTPD due to the maximum number of tubes that can be accommodated in the furnace box. This is currently around 1000 tubes.
[0027] The pre-reformer and steam-methane reformer or autothermal combination route increases the methanol plant's production capacity to between 4500 - 5,000 MTPD. Plant's production capacity can be increased further to around 7,000 MTPD by employing the autothermal and gas heated reformer combination.
Ammonia Plants
[0028] The synthesis production section of most of today's ammonia plants consists of a primary and secondary reformer arranged in series with the primary being a steam methane reformer and the secondary an autothermal reformer. Although the steam methane reformers are smaller than those on methanol plants and thus not limiting, the size of the autothermal reformer limits the production of synthesis gas to that equivalent to a maximum ammonia plant capacity of between 2500 - 2800 MTPD. The capacity of the biggest ammonia plant currently on stream is of the order of 2200 - 2500 MTPD.
[0029] Finally, as mentioned earlier, the synthesis gas production unit of these plants command the highest percentage of the total cost of synthesis gas based plants thus eliminating these bottlenecks will significantly improve the economics of the plants due to economic of scale effect. DESCRIPTION OF INVENTION
[0030] The three reforming technologies employed in this invention are:
> Adiabatic Pre-Reformer (APR)
> Steam-Methane Reformer (SMR)
> Autothermal or Partial Oxidation Reformer (ATR or POX).
[0031] The stated reforming technologies are well known proprietary technologies and are commercially available from a number of companies in the chemical and petrochemical industry. A brief description of each of the technologies used are:
[0032] Adiabatic Pre-Reformers (APR) are catalytic reactors which use part of the energy in the feed (i.e. hydrocarbon and steam mixture) introduced into it and the heat of any exothermic reaction of the reactants in the feed to reform heavier hydrocarbons and part of the methane present in the feed. No heat is added to or extracted from the reaction and hence the name adiabatic.
[0033] Steam-Methane Reformers (SMR) are box-type furnaces within which tubes, filled with catalyst are systematic arranged. The feed (i.e. hydrocarbon and steam mixture) is fed to the catalyst filled tubes and is reformed as it flows through the catalyst. The heat required by the endothermic reforming reaction is supplied by orderly-arranged burners located either in the roof, floor or sidewalls of the furnace box.
[0034] Autothermal Reformers (ATR) are catalytic reactors which use the heat from the highly exothermic hydrocarbon-oxygen combustion reaction to supply heat for the endothermic reforming reaction without the need for external heat. The oxygen for the reaction is supplied either as pure oxygen, enriched air or as normal atmospheric air.
[0035] Partial Oxidation Reformers (POX) are either catalytic or non-catalytic reactors which use the heat from the highly exothermic hydrocarbon-oxygen combustion reaction to supply heat for the endothermic reforming reaction without the need for external heat. The oxygen for the reaction is supplied either as pure oxygen, enriched air or as normal atmospheric air.
[0036] The present invention arranges the three reforming technologies namely APR, SMR and ATR (or POX) in a unique configuration, selects key process parameters such as steam to carbon ratios, flows and flow splits and fixes operating conditions of the reforming technologies to produce synthesis gas with the optimum composition for either Fischer- Tropsch Liquid, Methanol or Ammonia Production.
[0037] The operating envelop of the above reformers are well defined/documented and should be clear to anyone knowledgeable in this field. The operating conditions of the reformers employed in this invention are maintained within these defined envelops. [0038] A description of the invention for synthesis gas production process is as follows and should by read in conjunction with Figure 3:
[0039] Hydrogen or hydrogen rich containing gas from the synthesis section of the plant in question or imported from an external source 102 is added to natural gas feedstock 101 from the plant's battery limit and the mixture 103 is heated up and desulphurised in a typical Desulphurisation Unit 201 on said plants to remove any sulphur compounds present in the natural gas.
[0040] The desulphurised gas 104 is sent to the Saturator 202 where it is contacted with hot water heated from other parts of the plant and leaves saturated 105 with water vapour. Supplementary water vapour 106 is added to the saturated natural gas 105 to attain a desired steam to carbon ratio.
[0041] For Fischer-Tropsch plants, vapourised oxygenates from the synthesis section of the plant is added to the saturated gas prior to adding the supplementary steam.
[0042] Alternatively, the Saturator 202 can be omitted for all three plants and sufficient water vapour is added to the desulphurised gas to attain the same desired steam to carbon ratio as before.
[0043] The natural gas mixture with the desired steam to carbon ratio 107 is heated up and fed to the APR 203 where all the ethane and heavier hydrocarbons present are reformed together with some methane to hydrogen, carbon monoxide and carbon dioxide. The resulting APR products 108 is split into two streams 110 and 116 and one stream 110 is fed to the SMR train. The second stream 116 is fed to the ATR (or POX) train.
[0044] The SMR train consists of a heating train 204, a steam-methane reformer (SMR) 205 and a cooling train 206.
[0045] If required, water vapour 111 is added to the portion of APR products 110 to obtain a desired steam to carbon ratio. The mixture is heated up in the heating train 204 and fed to the SMR 205 for further reforming. The effluents from the SMR 113 is cooled down in a series of heat exchangers in 206 by generating high pressure water vapour and heating up other parts of the process. The resulting cooled gas 114 is added to the effluents from the ATR (or POX) train.
[0046] If desired a fraction of the cooled SMR effluent 126 is cooled down further in 212 and the cooled gas 127 is fed to a Hydrogen Recovery Unit 213 together with purge gas 128 from the synthesis section of the plant in question to recover hydrogen gas 129. The hydrogen gas 129 is added to the synthesis gas for conditioning.
[0047] The ATR (or POX ) train consists of a cooling/heating train 207, an Autothermal (ATR) or Partial Oxidation (POX) Reactor 208 and another cooling train 209. The portion of the APR effluent fed to the ATR (or POX) train 116, if desired is heated up (or cooled down to recover water vapour and reheated) in 207. [0048] For Fischer-Tropsch plants, the heated or reheated stream 117 is added to the tail gas from the synthesis section of the plant 118 and the mixture 119 is fed to the ATR or POX Reactor 208 where it is reformed further with oxygen or enriched air 120.
[0049] For Methanol plants, the heated or reheated stream 117 is fed to the ATR or POX Reactor 208 where it is reformed further with oxygen or enriched air 120.
[0050] For Ammonia plants, the heated or reheated stream 117 is fed to the ATR or POX Reactor 208 where it is reformed further with atmospheric air or enriched air.
[0051] If required, the effluents from the ATR or POX Reactor 208 is cooled down by generating high pressure water vapour before it is added to the effluents from the SMR as mentioned before.
[0052] In the case of Fischer-Tropsch plants, the resulting mixture 123 is fed to the Syngas Conditioning Unit 210 where the gas is cooled down by generating high pressure water vapour, interchanging heat with other parts of the synthesis process in a series of exchangers to a desired temperature and depending on the type of Fischer-Tropsch technology being employed, removing part of the carbon dioxide in the reformed gas using a typical carbon dioxide removal unit. Carbon dioxide removal units are proprietary technology and are commercially available from a number of companies world-wide.
[0053] In the case of Methanol plants, the resulting mixture 123 is fed to the Syngas Conditioning Unit 210 where the gas is cooled down by generating high pressure water vapour and interchanging heat with other parts of the synthesis process in a series of exchangers to a desired temperature.
[0054] In the case of Ammonia plants, the resulting mixture 123 is fed to the Syngas Conditioning Unit 210 where the gas is cooled down by generating high pressure water vapour and processed further by Carbon Monoxide Shifting, Carbon Dioxide Removal and Methanation to eliminate all carbon oxides from the reformed gas. The processed gas is then cooled down to a desired temperature by interchanging heat with other parts of the synthesis process in a series of exchangers. All these processing techniques are common on most ammonia plants.
[0055] For all three plants the synthesis gas is fed to a Desaturator 211 where it is contacted with cooled water to cool the gas down and remove any condensate produced.
[0056] Alternatively, for all three plants, the synthesis gas is cooled down and the condensate produced is separated in a K.O. Drum.
[0057] The resulting dry gas 125 from the Desaturator or K.O. Drum if required is conditioned further by added hydrogen gas 129 recovered from the small portion of synthesis gas and purge gas sent to the Hydrogen Recovery Unit 213 as described earlier. The conditioned mixture 129 is fed to the synthesis section of the Fischer-Tropsch, Methanol or Ammonia Plant for processing.
[0058] Though natural gas has been used as feedstock in the preceding description, it is possible to use liquid hydrocarbon feedstock (particularly in the case of Methanol and Ammonia production) or a combination of liquid and gaseous hydrocarbon feedstock. If a liquid feedstock is used, the feedstock needs to be vapourised before use.
[0059] With this invention, significantly more synthesis gas can be produced from the three reformers which when used as feedstock to the synthesis section of a Fischer-Tropsch, Methanol or Ammonia plant will enable production capacities in excess of that achieved with synthesis gas production processes available today.
[0060] Additionally the configuration of the reformers provides better control of the quantity of H2, CO, CO2 and N2 in the syngas thus permitting the production of syngas with the optimum composition for the particular synthesis gas based plant in question.
[0061] This improves the efficiency of the front end and translates into a more efficient Fisher-Tropsch, Methanol or Ammonia plant.
[0062] To accommodate the significant increase in synthesis gas production from this invention, multiple trains of the synthesis section of said plants may have to be employed to achieve said production capacities.

Claims

[0063] 1. A synthesis gas production process which employs three reforming technologies namely Adiabatic Pre-Reformer (APR), Steam-Methane Reformer (SMR) and Autothermal or Partial Oxidation Reformer (ATR or POX), arranged in a unique configuration with the APR upstream and in series with both the SMR and ATR (or POX) and the SMR and ATR (or POX) in parallel with each other to produce synthesis gas.
[0064] 2. A process according to claim 1 , in which the operating conditions of the three reformers are selected and key process parameters fixed to produce synthesis gas with the optimum composition for Fischer-Tropsch liquid production.
[0065] 3. When synthesis gas, produced according to the method described in Claim 2 is used as feedstock to the synthesis section of a Fischer-Tropsch plant will enable significant increase in production capacities than currently possible with synthesis gas production processes available today.
[0066] 4. A process according to claim 1 , in which the operating conditions of the three reformers are selected and key process parameters fixed to produce synthesis gas with the optimum composition for methanol production.
[0067] 5. When synthesis gas, produced according to the method described in Claim 4 is used as feedstock to the synthesis section of a Methanol plant will enable significant increase in production capacities than currently possible with synthesis gas production processes available today.
[0068] 6. A process according to claim 1 , in which the operating conditions of the three reformers are selected and key process parameters fixed to produce synthesis gas with the optimum composition for ammonia production.
[0069] 7. When synthesis gas, produced according to the method described in Claim 6 is used as feedstock to the synthesis section of an Ammonia plant will enable significant increase in production capacities than currently possible with synthesis gas production processes available today.
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