Multistage synthesis gas generation process

FIELD: synthetic fuels.

SUBSTANCE: invention relates to a method for production of synthesis mainly containing H2 and CO for producing hydrogen, alcohols, ammonia, dimethyl ether, and ethylene, for Fischer-Tropsch processes, and also for use in chemical industry for processing hydrocarbon gases and in chemothermal systems for accumulation and transport of energy as well as in methane-methanol thermochemical water decomposition cycles. In the multistage process of invention, at least two consecutive stages are accomplished, in each of which stream containing lower alkanes having about 1 to 34 carbon atoms are passed through heating heat-exchanger and the through adiabatic reactor filled with catalyst packing. Before first stage and between the stages, stream is mixed with water steam and/or carbon dioxide and cooled in the end of each stage. Steam leaving last stage is treated to remove water steam.

EFFECT: increased conversion of lower alkanes and reduced H2/CO ratio in produced synthesis gas.

12 cl

 

The invention relates to a method for producing synthesis gas, containing mainly H2and, for the production of hydrogen, alcohols, ammonia, dimethyl ether, ethylene, for processes of Fischer-Tropsch and can be used in the chemical industry for processing hydrocarbon gases, and chemothermal systems storage and transport of energy and a methane-methanol thermochemical cycles for the decomposition of water.

A method of obtaining a synthesis gas containing mainly H2and, for the production of alcohols, ammonia, dimethyl ether, ethylene, for processes of Fischer-Tropsch described in the patent of Russian Federation №2228901, date of publ. 2004.05.20, IPC 01 3/38. A method of obtaining a synthesis gas with a given ratio of H2/CO in the range from 1.0 to 2.0 includes two stages: stage A) partial oxidation stage and B) conversion of residual methane products phase And on the catalyst. Stage A) partial oxidation is carried out in two stages: a) non-catalytic partial oxidation of natural gas with oxygen to produce in the reaction products of non-equilibrium content of H2O and CH4when the molar ratio of oxygen and methane, is approximately equal to 0.76 to 0,84, b) conversion of the reaction products of step (a) with corrective additives CO2and H2Oh or H2O and CH4obtaining the gas mixture, the which is conversion of the residual methane water vapor on the catalyst. The method allows to produce a synthesis gas with a composition that meets the specified value WITH/N2. The method can be used to obtain a raw material for further synthesis of alcohols, dimethyl ether, ammonia, or other large-tonnage chemical products.

However, the described method has a number of disadvantages, which include functional and economic constraints of the application of the method associated with the necessity of submission to the costs of oxygen exceeding the mass flow rate convertible natural gas), the production of which requires more energy ( up to 1000 kWh/t) and capital costs (up to 1500 dollars. USA/CGC-1). A serious problem is also the sooting, drastically reducing the catalytic activity.

A method of obtaining a synthesis gas containing mainly H2and WITH that described in the monograph "Nuclear-technological complexes based on high temperature reactors", Alastoneesti - Moscow: Energoatomizdat", 1988. - 152 C. (ISBN 5-283-03750-9), s-109. This way the technological conversion of hydrocarbons comprises multi-stage synthesis gas, containing mainly H2and in which spend at least two successive stages, in each of which a stream containing lower alkanes having orientirovochno is from one to four carbon atoms, passed through the heating heat exchanger, and then through the adiabatic reactor filled with nozzle catalyst, and after the last stage of the stream to remove water vapor prototype. The disadvantages of this solution are relatively low coefficient of conversion of alkanes (up to 90%) and a relatively high ratio of H2/CO in the synthesis gas as the product of a process that worsens the conditions of the subsequent synthesis of derivatives from synthesis gas.

The purpose of the present invention is to create a new way to increase conversion rate, lower alkanes and create technological opportunities to reduce the ratio of N2/CO in the produced synthesis gas.

The problem is solved by the fact that:

in multistage production of synthesis gas, which spend at least two successive stages, in each of which a stream containing lower alkanes having from approximately one to four carbon atoms, is passed through the heating heat exchanger, and then through the adiabatic reactor filled with nozzle catalyst, and after the last stage of the stream to remove water vapor and a stream containing lower alkanes, before the first stage and between stages is mixed with water vapor and/or carbon dioxide and at the end of each stage, carry out the cooling flow. To efficient conversion of alkanes with this method increases more than 90%, and the ratio of H2/WITH can vary from 2 to 4 depending on the destination of the final product;

the cooling flow is carried out with heat recovery for heating and evaporation of water;

after the conclusion of the flow of water vapor conduct the removal from a stream of carbon dioxide and/or hydrogen, at least part of which is directed to mix with the stream before and/or between stages;

before the stages are clean flow from sulfur compounds;

in the heating heat exchanger heat flow are due to the convective cooling fluid through a sealed heat exchange surface;

- heating of the coolant flow at each stage are parallel to another stage in the course of cooling of the coolant;

in the adiabatic reactor to keep the temperature in the range approximately from 600°900°C;

the catalyst contains as active component a metal selected from the group of rhodium, Nickel, platinum, iridium, palladium, iron, cobalt, rhenium, ruthenium, copper, zinc, iron, mixtures thereof or compounds;

- lower alkane is a methane;

- flow pressure is chosen in the range from approximately 2.0 to 9.0 MPa;

- volumetric content of carbon dioxide before the first stage of support in the range of approximately from 10 to 30% of the volume content of alkanes;

- the volume containing the s of water vapor before the first stage of support in the range of approximately from 4 to 12 times greater, than the volumetric content of alkanes;

as the coolant used helium heated in a nuclear reactor.

An example implementation of the invention is a multistage method for production of synthesis gas, as described below.

In the described example embodiment of the invention as lower alkane is used methane, which allows us to characterize the features of the invention as applied to the processing of natural and associated gas.

The methane pressure is higher than 4.0 MPa mixed with the compressed up to the pressure of the recycled methane gas, containing hydrogen, carbon monoxide and carbon dioxide, is heated to a temperature of about 400°C and the resulting gas stream serves on the stage of purification from sulfur compounds (if they are contained as impurities in the methane), which is carried out in two stages: first lead, for example, on lookbetteronline.com the catalyst for hydrogenation of organic sulfur compounds such as mercaptans, hydrogen sulfide, and then the flow is directed to the absorption of the formed hydrogen sulfide activated zinc oxide in the reactor acquisitions included in the work consistently or in parallel. The gas stream, cleaned (in terms of sulfur) to the mass concentration of sulfur is less than 0.5 mg/nm3mixed with superheated steam flow to the steam/gas, for example, equal to 5.0. With the purpose for which helicene degree of conversion of methane volumetric content of water vapor before the first stage of support in the range of approximately from 4 to 12 times greater, than the volumetric content of alkanes. When the decrease of the ratio of steam/gas below 4 decreases the efficiency of the process and grow capital costs, due either to the need to increase the flow of recirculated gases in connection with a low degree of conversion at the specified lower temperature heat flow either need to increase the temperature of the flow over 1000-1200°that will be forced to use more expensive materials for the heat exchanger. The increase in vapor-gas over 12 will also cause a decrease in the efficiency of the process due to the need to produce excess water vapor.

The resulting stream is sent to the first section of the heating heat exchanger, which is heated, for example, to a temperature of about 650°and send the first adiabatic reactor filled with nozzle catalyst, in which, for example, it is preferable to use Nickel catalyst type GIAP-16. Can also be applied catalysts based on other active metals selected from the group of rhodium, platinum, iridium, palladium, iron, cobalt, rhenium, ruthenium, copper, zinc, iron, mixtures thereof or compounds. The composition of the catalyst by changing the content of platinum, and metals that affect the kinetics of the oxidation of carbon monoxide with water vapor (response shift) will allow you to control the hydrogen content in the context of cnom product.

In the adiabatic reactor without the supply of heat to produce a partial conversion of methane to a volume fraction of methane is not more than 33%, then the flow with a temperature of about 600°With direct cooling in the HRSG to produce steam. The cooling stream can improve the heating heat exchanger by increasing sredneahtubinskogo thermal head. Before the next stage of the process, which repeats the composition of the action of the first stage, the flow of metered water vapor.

Enriched in components of the flow directed to the second section of the heating heat exchanger where the flow temperature is increased to 750°and then send the second adiabatic reactor designs repeating the first adiabatic reactor filled with nozzle catalyst that produces the further conversion of methane to reduce its content to 17% when the flow temperature on the yield of about 660°C. the thread Then again cooled in the HRSG is mixed with additional amounts of water vapor and sent for final doconversion methane in the third stage, in which the order and content of the operations do not differ from the first two stages, and the heating temperature is about 870°C. the Choice of temperature is determined primarily by the temperature potential of Teplova the source, for example, heated in a nuclear reactor helium, as well as opportunities for the creation of heat exchangers with relatively inexpensive heat-resistant heat-exchange surfaces on the basis of steels and alloys with a low content of expensive components (Nickel, cobalt, chromium, molybdenum and so on)that determines the preferred top level possible temperature 900°C. on the other hand, the equilibrium degree and rate of conversion of methane below 600°even at relatively high ratio of water vapor/gas is practically unacceptable.

After exiting the third stage with the outlet temperature of more than 750°With the flow with a methane content of about 3% are sent sequentially in the superheater, boiler, feedwater heater, and then into the heat exchanger heating water where the stream is cooled to 170°With, then finally cooled to 40°in water heat exchangers necesariamente water. The degree of methane conversion in the described process is about 80%, and the ratio of N2/(CO+CO2) is about 2.9.

The resulting synthesis gas can then be used for the production of hydrogen, which flow removes CO2in the absorption treatment, for example, an aqueous solution of activated mono - and diethanolamine, and then finally produce in the location by swing adsorption on activated carbon or zeolite, in the process which receive the products of desorption, which is directed partially incinerated and used as recycled gas.

In the second example, in embodiments, production of methanol and/or dimethyl ether, after desulfurization methane is mixed with the compressed up to the pressure of the flow of carbon dioxide, the source of which can be gases, technological processes, including fermentation, decarbonization, or, as in the Orenburg field, an integral part of the underground natural gas and recirculation flows of the production itself. The resulting stream is sent to the first section of the heating heat exchanger, which is heated, for example, to a temperature of about 650°and send the first adiabatic reactor filled with nozzle catalyst, in which, for example, it is preferable to use Nickel catalyst. Can also be applied catalysts based on other active metals. The composition of the catalyst affects the kinetics of processes involving carbon dioxide that will allow you to control the hydrogen content in the final product.

In the adiabatic reactor without the supply of heat to produce a partial conversion of methane to a volume fraction of methane is not more than 40%, then the flow with a temperature of about 600°With direct cooling in the HRSG. Before the next article is by die process, which repeats the composition of the action of the first stage, the flow dispense an additional amount of carbon dioxide, thereby shifting thermodynamic equilibrium of the process towards a greater degree of conversion of methane into synthesis gas.

Enriched in components of the flow directed to the second section of the heating heat exchanger where the flow temperature is increased to 750°and then send the second adiabatic reactor designs repeating the first adiabatic reactor filled with nozzle catalyst that produces the further conversion of methane to the reduction of its content is below 20% when the temperature of the flow at the outlet of about 650°C. the thread Then again cooled in the HRSG is mixed with an additional quantity of carbon dioxide and sent for final doconversion methane in the third stage, in which the order and content of the operations do not differ from the first two stages, and the heating temperature is about 860°C. the Choice of temperature is determined primarily by temperature potential heat source, for example, products of combustion of process gases or heated in a nuclear reactor helium, as well as opportunities for the creation of heat exchangers with relatively inexpensive heat-resistant heat-exchange surfaces on the basis of steels and alloys with low content is receiving the expensive components (Nickel, cobalt, chromium, molybdenum and so on)that determines the preferred top level possible temperature 900°C. on the other hand the equilibrium degree and rate of conversion of methane below 600°even at relatively high ratio of water vapor/gas is practically unacceptable.

After exiting the third stage with the outlet temperature of more than 750°With the flow with a methane content of about 3% are sent sequentially in the HRSG, and then into the heat exchanger heating water where the stream is cooled to 170°With, then finally cooled to 40°in water heat exchangers necesariamente water.

It is also possible third alternative implementation of the process in which instead of the three stages of heat flow is passed through two-cycle heating-cooling. This is possible by increasing the heating temperature of the flow at the first and second stages to 900°With simultaneous increase in the correlation of vapor-gas more than 8. In this case also possible to obtain the required values of the degree of conversion of methane (about 90%) or other lower alkanes with simultaneous cost reduction of the metal in the heat exchanger, but with an increased cost of the metal to generate water vapor. When using carbon dioxide to methane conversion for a two-stage process will need to increase the contents of the CO 2that would entail rising energy costs and power on the release of excess CO2and its recycling.

Possible fourth example of the method, in which the main agent of methane conversion using water vapor, but at the same time, in this example, to reduce the relationship of H2/(CO+CO2in the final synthesis gas volumetric content of carbon dioxide before the first stage of support in the range of approximately from 10 to 30% of the volume content of alkanes. In this case, all stages are conducted similar to the first described example, but the ratio of N2/(CO+CO2) receive approximately equal to 2.1, i.e. lower than in the first example, which is favourable for the production of certain products. In particular, in the case of using the obtained dried synthesis gas for subsequent synthesis of methanol or dimethyl ether stream can without purification from CO2and hydrogen immediately be sent to the columns of catalytic synthesis, which is also referred unreacted gas discharged from the Department of synthesis.

Given the need to reduce the work of compression, the process is conducted at a pressure of minimally different from the pressure of the subsequent synthesis of commercial products, which is in various technologies from 6 to 10 MPa, or pressure to be issued for subsequent use is of hydrogen or reformed gas (from 2 to 9 MPa), as is the case in nuclear chemothermal systems, described in the source cited above. Similarly, choose the pressure in the production of alcohols, ammonia, dimethyl ether, ethylene, for processes of Fischer-Tropsch and other technology which can be effectively applied method according to the invention.

Processes for the production of synthesis gas streams containing other lower alkanes (ethane, propane, butane), for example, on the basis of associated gas production, carried out analogously to the above examples.

1. The multistage method of production of synthetic gas, which spend at least two successive stages, in each of which a stream containing lower alkanes having from approximately one to four carbon atoms, is passed through the heating heat exchanger, and then through the adiabatic reactor filled with nozzle catalyst, and after the last stage of the stream to remove water vapor, wherein the stream containing lower alkanes, before the first stage and between stages is mixed with water vapor and/or carbon dioxide and at the end of each stage, carry out the cooling.

2. The method according to claim 1, characterized in that the cooling flow is carried out with heat recovery for heating and evaporation of water.

3. The method according to claim 1 or 2, characterized in that after the withdrawal from the stream of water vapor p is avodat removal from a stream of carbon dioxide and/or hydrogen, at least part of which is directed to mix with the stream before and/or between stages.

4. The method according to claim 1 or 2, characterized in that, before the stages are clean stream from the sulfur compounds.

5. The method according to claim 1 or 2, characterized in that the heating heat exchanger heat flow are due to the convective cooling fluid through the heat sealed surface.

6. The method according to claim 1 or 2, characterized in that the heating in the heat exchanger, the flow of the coolant at each stage are parallel to another stage in the course of cooling fluid.

7. The method according to claim 1 or 2, characterized in that in the adiabatic reactor to keep the temperature in the range of approximately 600 to 900°C.

8. The method according to claim 1 or 2, characterized in that the lower alkane is a methane.

9. The method according to claim 1 or 2, characterized in that the flow pressure is chosen in the range approximately from 2.0 to 9.0 MPa.

10. The method according to claim 1 or 2, characterized in that the volumetric content of carbon dioxide before the first stage of support in the range of approximately from 10 to 30% of the volume content of alkanes.

11. The method according to claim 1 or 2, characterized in that the volumetric content of water vapor before the first stage of support in the range of approximately from 4 to 12 times greater than the volume content of alkanes.

12. The way is about to claim 1 or 2, characterized in that the coolant used helium heated in a nuclear reactor.



 

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13 cl, 2 tbl, 17 ex

FIELD: electric power and chemical industries; methods of production of the electric power and liquid synthetic fuel.

SUBSTANCE: the invention presents a combined method of production of the electric power and liquid synthetic fuel with use of the gas turbine and steam-gaseous installations and is dealt with the field of electric power and chemical industries. The method provides for the partial oxidation of hydrocarbon fuel in a stream of the compressed air taken from the high-pressure compressor of the gas turbine installation with its consequent additional compression, production of a synthesis gas, its cooling and ecological purification, feeding of the produced synthesis gas in a single-pass reactor of a synthesis of a liquid synthetic fuel with the partial transformation of the synthesis gas into a liquid fuel. The power gas left in the reactor of synthesis of liquid synthetic fuel is removed into the combustion chamber of the gas-turbine installation. At that the degree of conversion of the synthesis gas is chosen from the condition of maintenance of the working medium temperature at the inlet of the gas turbine depending on the type of the gas-turbine installation used for production of the electric power, and the consequent additional compression of the air taken from the high-pressure compressor of the gas-turbine installation is realized with the help of the gas-expansion machine powered by a power gas heated at the expense of the synthesis gas cooling before the reactor of synthesis. The invention allows simultaneously produce electric power and synthetic liquid fuels.

EFFECT: the invention ensures simultaneous production of electric power and synthetic liquid fuels.

2 cl, 2 dwg

FIELD: petrochemical industry.

SUBSTANCE: the invention is dealt with petrochemical industry, in particular with a method of catalytic preliminary reforming of the hydrocarbon raw materials containing higher hydrocarbons. The method provides for the indicated hydrocarbon raw materials gating through a zone of a catalyst representing a fixed layer containing a noble metal on magnesia oxide (MgO) and-or spinel oxide (MgAl2O4) at presence of oxygen and water steam. The technical result is a decrease of a carbon share on the catalyst.

EFFECT: the invention allows to decrease a carbon share on the catalyst.

3 cl, 2 tbl, 2 ex

FIELD: technology for production of methanol from syngas.

SUBSTANCE: claimed method includes mixing of hydrocarbon raw material with water steam to provide syngas by steam conversion of hydrocarbon raw material and subsequent methanol synthesis therefrom. Conversion of hydrocarbon raw material and methanol synthesis are carried out under the same pressure from 4.0 to 12.0 MPa. In one embodiment hydrocarbon raw material is mixed with water steam and carbon dioxide to provide syngas by steam/carbonic acid conversion of hydrocarbon raw material in radial-helical reactor followed by methanol synthesis therefrom under the same pressure (from 4.0 to 12.0 MPa). In each embodiment methanol synthesis is carried out in isothermal catalytic radial-helical reactor using fine-grained catalyst with grain size of 1-5 mm. Methanol synthesis is preferably carried out in two steps with or without syngas circulation followed by feeding gas from the first or second step into gasmain or power plant.

EFFECT: simplified method due to process optimization.

12 cl, 3 tbl, 3 dwg

FIELD: methods of production a synthesis gas.

SUBSTANCE: the invention is pertaining to the process of production of hydrogen and carbon oxide, which mixture is used to be called a synthesis gas, by a selective catalytic oxidation of the hydrocarbonaceous (organic) raw material in presence of the oxygen-containing gases. The method of production of the synthesis gas includes a contacting with a catalyst at a gas hourly volumetric speed equal to 10000-10000000 h-1, a mixture containing organic raw material and oxygen or an oxygen-containing gas in amounts ensuring the ratio of oxygen and carbon of no less than 0.3. At that the process is conducted at a linear speed of the gas mixture of no less than 2.2 · 10-11 · (T1 + 273)4 / (500-T2) nanometer / s, where: T1 - a maximum temperature of the catalyst, T2 - a temperature of the gas mixture fed to the contacting. The linear speed of the gas mixture is, preferably, in the interval of 0.2-7 m\s. The temperature of the gas mixture fed to the contacting is within the interval of 100-450°C. The maximum temperature of the catalyst is within the interval of 650-1500°C. The technical effect is a safe realization of the process.

EFFECT: the invention ensures a safe realization of the process.

10 cl, 5 ex

FIELD: chemical industry; petrochemical industry; oil refining industry and other industries; methods of production a synthesis gas.

SUBSTANCE: the invention is pertaining to the field of the methods of production of a synthesis of gas and may be used in chemical, petrochemical, oil refining and other industries. The method of production of synthesis gas using a vapor or a vapor-carbon dioxide conversion of a hydrocarbonaceous raw material provides for purification of the hydrocarbonaceous raw material from sulfuric compounds, its commixing with steam or with steam and carbon dioxide with formation of a steam-gas mixture. The catalytic conversion of the steam-gas mixture is conducted in a reactor of a radially-spiral type, in which in the ring-shaped space filled with a nickel catalyst with a size of granules of 0.2-7 mm there are the hollow spiral-shaped walls forming the spiral-shaped channels having a constant cross section for conveyance of a stream of the steam-gaseous blend in an axial or in a radially-spiral direction. At that into the cavities of the walls feed a heat-transfer agent to supply a heat into the zone of reaction. The invention ensures intensification the process.

EFFECT: invention ensures intensification the process.

4 cl, 4 dwg, 2 tbl, 3 ex

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