Classifications

• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
  • C10J3/72—Other features
  • C10J3/721—Multistage gasification, e.g. plural parallel or serial gasification stages
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
  • C10J3/02—Fixed-bed gasification of lump fuel
  • C10J3/06—Continuous processes
  • C10J3/18—Continuous processes using electricity
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
  • C10J3/46—Gasification of granular or pulverulent flues in suspension
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
  • C10J3/72—Other features
  • C10J3/78—High-pressure apparatus
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J2300/00—Details of gasification processes
  • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
  • C10J2300/0913—Carbonaceous raw material
  • C10J2300/093—Coal
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J2300/00—Details of gasification processes
  • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
  • C10J2300/0953—Gasifying agents
  • C10J2300/0973—Water
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J2300/00—Details of gasification processes
  • C10J2300/12—Heating the gasifier
  • C10J2300/123—Heating the gasifier by electromagnetic waves, e.g. microwaves
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J2300/00—Details of gasification processes
  • C10J2300/12—Heating the gasifier
  • C10J2300/123—Heating the gasifier by electromagnetic waves, e.g. microwaves
  • C10J2300/1238—Heating the gasifier by electromagnetic waves, e.g. microwaves by plasma
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J2300/00—Details of gasification processes
  • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
  • C10J2300/1625—Integration of gasification processes with another plant or parts within the plant with solids treatment
  • C10J2300/1628—Ash post-treatment
  • C10J2300/1634—Ash vitrification
• • C—CHEMISTRY; METALLURGY
  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
  • C10J2300/00—Details of gasification processes
  • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
  • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
  • C10J2300/1656—Conversion of synthesis gas to chemicals
  • C10J2300/1659—Conversion of synthesis gas to chemicals to liquid hydrocarbons

Definitions

• the invention relates to a method for thermal and thermochemical conversion of coal into synthesis gas, applicable to the chemical and petrochemical industries for the production of synthesis gas, which is a raw material for obtaining various types of chemical products and synthetic motor fuels.
• a method of converting solid fuel including saturation of the coal with hydrogen at high temperatures (above 400 0 C) and pressure from 50 to 300 atm with following separation into liquid and solid intermediate products. Subsequently, the liquid products are subject to hydrogenation refinement with the following production of components of high- octane petrol, diesel fuel, propellant and gas-turbine fuel, phenols, nitrogen hydroxides and other products [Chulkov, V. V., Motor Fuels: Resources, Quality, Substitutes. Moscow, 1998].
• the mixture of hydrogen and carbon monoxide, necessary for the production is obtained by treating the coal with water vapor and oxygen.
• oxygen as an oxydizer leads to ballasting the synthesis gas with carbon dioxide that is a product from the interaction between carbon and oxygen, and moreover, to obtain oxygen also requires a special installation. AU this leads to additional, energy consumption as the synthesis gas should be purified,, and obtaining and storing oxygen in the required volume results in increased energy consumption.
• Maintaining the temperature of the synthesis gas obtained at the expense of regulating the electric arc power is low-efficient, non-reliable and complex as the release of heat in the reactor occurs at the expense of both the coal combustion in oxygen environment and the energy released by the electric arc, and at the same time only one source of heat emission is regulated, namely the electric arc.
• a method of converting coal into synthesis gas including coal preparation in the form of colloidal-dispersion fuel system with average surface size of the particles of the dispersion phase not larger than 1 ⁇ m, gasification of the obtained fuel mixture in a single stage in a reactor with pipes placed vertically, into which the fuel mixture mentioned is fed, and at that the temperature of the heat-transfer medium in the space between the pipes in the reactor being maintained within the range of 400 - 1,000 0 C, and the temperature in the pipes in the range of 200 - 800 0 C [RU2190661].
• a disadvantage of this method is its low energy efficiency in the process of producing the synthesis gas because: - the preparation of the colloidal-dispersion fuel system is accompanied by grinding not only the organic component of the coal, but also its mineral component, to average surface size of the particles of the dispersion phase not larger than 1 ⁇ m, which increases considerably the energy consumption for their grinding;
• the recommended temperature range of gasification from 200 to 800 0 C does not ensure efficient development of the process when using low-reaction coal, for instance, anthracite.
• a thermal plasma method of converting coal into synthesis gas is also known, where said method includes preparation, thermal treatment and gasification of coal by the use of plasma in a plasmoreactor, said gasification process being performed in three stages, two of which being conducted in pipe heat-exchangers, and the third final stage is performed immediately in the volume of the plasmoreactor, simultaneously with the process of high-temperature pyrolysis in the presence of a reagent.
• the preparation of the coal is carried out through its dispergation in methanol water, to which surface-active substances - alkylamides - are added, and the coal suspension obtained at the first stage of gasification is heated in pipes to 200 - 300 0 C in the flow of flue gases exhausting from the gasification column and fed into the space between the pipes of the reactor, and before the second gasification stage, said coal suspension is heated to 900 - 1,100 0 C in the flow of synthesis gas discharged from the plasmoreactor.
• Water vapor is used as a reagent in high-temparature pyrolysis, which is injected in the reaction zone with the help of plasma sources.
• the synthesis gas obtained in the plasmoreactor is cooled and purified from impurities in a centrifugal-barbotage apparatus by using atmosphere air and water, the atmosphere air being used subsequently with a part of the synthesis gas in the combustion device of the gasification column, and the water being fed to the dispergating device for preparation of the coal suspension [RU2047650].
• a disadvantage of this method is the complexity of the technological process, which is realized in three stages with preliminary heating-up of the water- coal suspension up to 200 - 300 0 C, with simultaneous burning of a part of the synthesis gas and using the synthesis gas discharged from the plasmoreactor, heated up to temperature 2,200 - 2,700 0 C.
• preliminary heating-up and realizing the first and second stages of gasification in the temparature range of 900 - 1,100 0 C it is sufficient to use the heat accumulated in the synthesis gas discharged from the plasmoreactor.
• vapor-gas- coal suspension consisting of carbon oxide, carbon dioxide, hydrogen, water vapors and non-reacted coal particles, in the plasmoreactor.
• Water vapors are used in the plasmoreactor as a reagent, which leads to additional ballasting of the gaseous products from the gasification with water vapor and simple hydrocarbons being formed at high temperatures within 2,200 - 2,700 0 C.
• the method for producing synthesis gas from a water-coal suspension is the closest to the present invention [RU2233312], said method including the preparation and gasification of the water-coal suspension, said gasification being realized in two stages, the first of which is carried out in a vertical counter-flow pipe heat-exchanger on the gasification column, and the second in a reactor for heating by means of an ultrahigh-frequency emission (UHF-reactor).
• UHF-reactor ultrahigh-frequency emission
• the water-coal suspension obtained is directed to the heat-exchanger on the gasification column under pressure of 0.5 - 10 MPa, where it is heated up to temperature 500 - 700 0 C and until a vapor-gas-coal suspension is formed. Further on, this suspension is directed into a vapor-jet mill for grinding the particles of the solid phase to a fine dispersion state of 1 - 3 ⁇ m.
• the vapor-gas-coal suspension, ground to the preset size is fed to the second gasification stage, i. e. into a reactor for heating, for example - the UHF-reactor, where it is heated to temperature 700 - 1,500 0 C in order to produce a synthesis gas.
• the synthesis gas obtained is cooled in the heat- exchanger on the gasification column with the aid of the water-coal suspension entering the heat-exchanger and purified from the ballast substances by means of water used for preparing the water-coal suspension.
• the process of gasification conducted is realized in two stages, instead of three, which enables simplifying the technology for producing a synthesis gas.
• the process of preparing the water-coal suspension is realized by grinding the coal introduced initially through dispergation in water phase in order to separate the bound organic and mineral particles of the coal (down to a size of solid phase particles within 10 - 30 ⁇ m), which permits avoiding the fragmentation of the most solid and hard-dispergating mineral coal particles to the size of the fine dispersion fraction, less than 1 ⁇ m, considerably diminishing in such a way the energy consumption in the preparation of the water-coal suspension.
• the mass concentration of the organic part of coal in the water-coal suspension represents 32 % - 48 %, which provides low values of the viscosity of the water-coal suspension even for a size of the coal particles within 10 - 30 ⁇ m, and as a result of this the efficiency of the process of producing synthesis gas is increased.
• the water-coal suspension obtained under pressure 0.5 — 10 MPa is heated in a heat-exchanger up to temperature 500 - 700 0 C, at which a vapor-gas-coal suspension is formed.
• the so realized gasification process takes place in a more intensive way as compared to the gasification performed at atmospheric pressure.
• a vapor-jet mill is not connected with additional consumption of energy for grinding because the energy used in it is accumulated in the overheated vapor-gas-coal suspension in the form of increased pressure (0.5 - 10 MPa) and inincreased temperature 500 - 700 0 C.
• additional grinding is applied mostly to porous particles from the coke residue of the organic component of the coal because this occurs both at the collision of particles into one another and as a result of the difference between the pressure inside the particles themselves and the pressure in the working chamber of the mill. Particles participating in the mineral composition of the coal are ground additionally to a considerably lesser extent as they practically lack any porousity.
• the second gasification stage takes place in an UHF-reactor, in which direct heating of the whole reacting mass of the vapor-gas-coal suspension up to temperatures 700 - 1500 0 C is realized under the effect of an ultrahigh-frequency electromagnetic emission.
• UHF-reactor in which direct heating of the whole reacting mass of the vapor-gas-coal suspension up to temperatures 700 - 1500 0 C is realized under the effect of an ultrahigh-frequency electromagnetic emission.
• a disadvantage of this method is the realization of the process within such a high-temparature range, which leads to an increase in the energy consumption, diminishment of the economical efficiency of the process, and partial melting of the mineral components of coal and soot formation.
• the task of the invention consists in creating a method of converting coal into fuels with increased efficiency of the process of producing synthesis gas from a high- viscosity water-coal fuel.
• This task is solved by creating a method of converting coal into fuels, which includes preparation of a water-coal mixture and its gasification in two stages. The first of them takes place in a vertical counter-flow pipe heat-exchanger on a gasification column, and the second in a heating reactor with production of synthesis gas and solid residues.
• a stage of catalytic conversion of the synthesis gas in motor fuels follows. It is characteristic that the vapor-gas-coal mixture in the heat-exchanger is subject to the action of modulated high-frequency fields in the frequency range from 1 MHz to 50 MHz at modulation frequencies in the range from 1 KHz to 200 KHz.
• the vapor-gas-coal mixture is subject to the action of plasma from single-electrode high-frequency discharges at temperature 600 - 800 0 C.
• the synthesis gas obtained is subject to electrochemical purification from the compounds of sulphur and nitrogen, purification from chemical impurities, compressed and subject to conversion with the help of a polyfunctionaL catalyst, containing oxides of iron, zinc and molybdenum in combination with a carrier, namely aluminium, its oxides and aluminium phosphate.
• An advantage of the invention is that the method of converting of coal into fuels is characterized by increased efficiency of the process of producing synthesis gas from high-viscosity water-coal fuel.
• the installation in the figure is a possible embodiment realizing the method.
• the vapor-gas-coal mixture is fed by means of a pump 1 into a vertical counter-flow pipe heat-exchanger 2 on the gasification column 3 and treated additionally by means of high-frequency electromagnetic fields.
• Transferring high-frequency energy into the vapor-gas-coal mixture is carried out by metal rods 4, which are covered entirely with dielectric materials (for instance, ceramics, quartz) 5.
• These metal rods 4 are connected to a high- frequency generator 6 that provides in working regime the transfer of high- frequency power into the vapor-gas-coal mixture at carrier frequency 1 - 50 MHz and modulation frequency 1- 200 KHz.
• the second stage of the method is connected with an additional process of gasification of the vapor-gas-coal mixture being fed through pipelines 7 into the reactor 8, in which the internal walls are covered with a special material on the basis of refractory coating, having not only low heat conductivity and low heat capacity, but also catalyzing properties in the reactor for the vapor conversion of carbon into synthesis gas.
• a material being a catalyst permits accelerating the process of carbon gasification at relatively low temperatures (up to 400 0 C), which under equal other conditions makes it possible to increase 1.5 to 2 times the productivity of the installation for synthesis-gas production.
• Transferring the UHF-energy to the electrodes described above is performed by high-frequency generators 10. They operate at frequency 1 - 40 MHz and modulation frequency 0.5 - 50 KHz.
• the vapor-gas-coal mixture is subject to action by both the plasma from single-electrode discharges and the high-frequency electromagnetic fields, which causes the occurrence of fullerenes and fullerites increasing the quantity of synthesis gas obtained from the mixture treated.
• the distinguishing features of the invention are: - Using high-frequency energy the both stages of producing synthesis gas from a vapor-gas-coal mixture;
• a coating on the internal walls of the reactor made of a refractory material featuring not only resistance to chemical and mechanical actions exerted by the vapor-gas-coal mixture, but also strong catalyzing properties for the vapor conversion of carbon;
• the internal walls of the reactor 8 are lined with a material that possesses not only thermoinsulating, but also catalyzing properties, which permits increasing the intensivity of the process of producing synthesis gas from the vapor-gas-coal mixture and shortening in such a way the time for treatment of the vapor-gas-coal mixture in the reactor.
• the process of gasification of the vapor-gas-coal mixture is realized in the following way:
• the prepared watercoal mixture with particles with size no larger than 30 ⁇ m is fed by means of a pump 1 at pressure 0.1 - 3.0 MPa into a vertical counter-flow pipe heat-exchanger 2 on the gasification column 3.
• the water-coal mixture is heated to 200 - 400 0 C and until a vapor-gas-coal suspension is formed, said suspension being treated by means of modulated high-frequency fields.
• Transferring the UHF-power is performed through metal rods 4 covered with dielectric material 5. Said metal rods are coupled directly to the high-frequency generators 6 that operate at carrier frequency 1 - 50 MHz and modulation frequency 1 — 200 KHz.
• the partially gasified vapor-gas-coal suspension is fed along the pipelines 7 into the reactor 8 through a static mixer 11, where, under the action of the high- frequency fields and the plasma from single-electrode discharges, the vapor-gas- coal mixture is heated to temperature 500 - 800 0 C.
• the internal walls of the reactor 8 are lined with a thermoinsulating coating, on the external surface of which a layer of catalyst used in the vapor conversion of carbon is deposited.
• the synthesis gas obtained in the reactor 8, along with the ballast substances, is introduced in the space between the pipes of the gasification column 3, where the water-coal mixture entering the pipe part of the heat- exchanger 2 is used as a coolant.
• the synthesis gas After passing through the heat-exchanger, the synthesis gas is fed to a purification device 12, for instance, a centrifugal- barbotage apparatus, in which, as a result of the direct contact with cooling water, the synthesis gas is cooled to the temperature of the environment and releases the ballast substances of the gasification products (water vapor, coal ash particles, hydrogen sulphide, carbon dioxide, etc.).
• the purified synthesis gas is compressed by a compressor and fed through pipelines to the customers.
• the purified water is fed to the pipeline for circulating water.
• Ash residues from the gasification are discharged from the lower part of the gasification column and directed for further conversion.
• the mass ratio between water and the organic part of the solid phase of the water-coal mixture is determined from the condition that the water content should exceed with 10 - 20 % the quantity of water which is needed according to the stoichiometric equation of the gasification reaction of carbon with the water vapor, and depends on the carbon content in coal [RU2233312]. For mass ratio of the carbon in coal within 0.96 - 0.6, the mass concentration of coal in the water- coal mixture is approximately 32 - 48 %.
• the synthesis gas obtained is directed for electrochemical and plasma- chemical treatment at temperature about 600 0 C for maximum removal of the compounds of sulphur and nitrogen. Then the synthesis gas is cooled, purified from chemical impurities, compressed and directed into a reactor for synthesis of hydrocarbons at temperature 300 0 C and pressure 3 MPa.
• the synthesis of liquid hydrocarbons takes place in the presence of a polyfunctional catalyst containing oxides of iron, zinc and molybdenum in combination with a carrier, namely aluminium, its oxides and aluminium phosphate.
• the total quantity of the synthetic fuels produced is 190 g/nm 3 of synthesis gas for 90-percent conversion of the carbon oxides.

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• Chemical & Material Sciences (AREA)
• Engineering & Computer Science (AREA)
• Combustion & Propulsion (AREA)
• Oil, Petroleum & Natural Gas (AREA)
• Organic Chemistry (AREA)
• Industrial Gases (AREA)
• Catalysts (AREA)
• Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

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• 2005
  • 2005-07-29 BG BG109247A patent/BG109247A/bg unknown
• 2006
  • 2006-01-17 WO PCT/BG2006/000004 patent/WO2007012151A1/en active Application Filing
  • 2006-01-17 EP EP06705065A patent/EP1996679A1/en not_active Withdrawn
  • 2006-02-09 UA UAA200600581A patent/UA79216C2/uk unknown
  • 2006-03-16 EA EA200600431A patent/EA008269B1/ru not_active IP Right Cessation

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