WO2022242598A1 - Appareil et procédé de préparation d'un produit contenant de l'hydrogène à partir de gaz naturel sur la base d'une nouvelle consommation d'énergie - Google Patents

Appareil et procédé de préparation d'un produit contenant de l'hydrogène à partir de gaz naturel sur la base d'une nouvelle consommation d'énergie Download PDF

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Publication number
WO2022242598A1
WO2022242598A1 PCT/CN2022/093069 CN2022093069W WO2022242598A1 WO 2022242598 A1 WO2022242598 A1 WO 2022242598A1 CN 2022093069 W CN2022093069 W CN 2022093069W WO 2022242598 A1 WO2022242598 A1 WO 2022242598A1
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hydrogen
natural gas
unit
preheater
inlet
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PCT/CN2022/093069
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English (en)
Chinese (zh)
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刘银河
宋虎潮
林啸龙
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西安交通大学
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Publication of WO2022242598A1 publication Critical patent/WO2022242598A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
    • C01B3/58—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
    • C01B3/58—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction
    • C01B3/586—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction the reaction being a methanation reaction
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C01B2203/045—Purification by catalytic desulfurisation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C01B2203/048—Composition of the impurity the impurity being an organic compound
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C01B2203/0485—Composition of the impurity the impurity being a sulfur compound
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency
    • Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency
    • Y02P20/133—Renewable energy sources, e.g. sunlight

Definitions

  • the invention belongs to the technical field of new energy and hydrogen production from natural gas, and in particular relates to a device and method for preparing hydrogen-containing products from natural gas absorbed by new energy.
  • the natural gas reforming hydrogen production technology has the advantages of low cost and mature technology compared with other technologies, it usually uses part of the natural gas combustion as heat energy supply in the hydrogen production process, which brings a certain degree of carbon emissions.
  • the heat energy cannot be fully utilized; in addition, the existence of the burner and the flue greatly increases the complexity of the system and reduces the stability of the system.
  • the object of the present invention is to provide a device and method for producing hydrogen-containing products from natural gas based on new energy consumption, which solves the problems of high energy consumption and poor device stability in hydrogen production from natural gas.
  • the present invention adopts the following technical solutions to achieve:
  • the invention discloses a device for preparing hydrogen-containing products from natural gas based on new energy consumption, including a natural gas raw material inlet, a refined desulfurization unit, a raw material preheater, a conversion reaction unit, an electrothermal conversion unit, a feed water preheater, a high-temperature heat pump, Hydrogenation inlet, feed water inlet and flow mixer; natural gas preheater is installed in the conversion reaction unit;
  • the inlet of the natural gas raw material is connected to the inlet of the refined desulfurization unit through the natural gas preheater, the outlet of the refined desulfurization unit is connected to the inlet of the cold end of the raw material preheater through the mixer, and the outlet of the hot end of the raw material preheater is connected to the inlet of the electrothermal conversion unit.
  • the outlet of the conversion unit is connected to the inlet of the hot end of the raw material preheater, the outlet of the cold end of the raw material preheater is connected to the inlet of the conversion reaction unit, the outlet of the conversion reaction unit is connected to the inlet of the hot end of the feed water preheater through the steam superheater, and the feed water preheater
  • the outlet of the cold end of the heater is connected with the inlet of the high-temperature side of the high-temperature heat pump, the outlet of the low-temperature side of the high-temperature heat pump is connected with the inlet of the hydrogen splitter through the pressure swing adsorption unit, and the outlet of the hydrogen splitter is connected with the hydrogenation port;
  • the feedwater inlet is connected to the inlet of the cold end of the feedwater preheater, the outlet of the hot end of the feedwater preheater is connected to the inlet of the high temperature side of the high temperature heat pump, and the outlet of the high temperature side of the high temperature heat pump is connected to the mixer through the steam superheater.
  • the outlet of the hydrogen splitter is connected to the inlet of the refining desulfurization unit;
  • a steam compressor is provided on the pipeline between the high temperature side outlet of the high temperature heat pump and the steam superheater;
  • the electrothermal conversion unit is equipped with an electrothermal furnace
  • a hydrogen three-way valve is installed on the pipeline between the outlet of the hydrogen splitter and the hydrogen refueling port, a hydrogen compressor is installed on the pipeline between the outlet of the hydrogen gas splitter and the hydrogen refueling port, and a hydrogen compressor is installed on the pipeline between the hydrogen gas splitter outlet and the hydrogen refueling port.
  • a hydrogen storage unit is installed on the pipeline.
  • a renewable power interface is also included, and the electric furnace, high-temperature heat pump, hydrogen compressor, and steam compressor use external renewable energy through the renewable power interface.
  • the invention discloses a method for using the above-mentioned natural gas based on new energy consumption to prepare hydrogen-containing products, including the following operating steps:
  • the natural gas raw material enters the natural gas preheater to obtain the reaction heat from the shift reaction unit, and the temperature rises to above 300°C; at the same time, the feed water enters the feed water preheater for preliminary preheating until it becomes saturated water;
  • the outlet gas of the electrothermal conversion unit contains CO, H 2 , CO 2 , CH 4 and water vapor, and the temperature is above 700°C.
  • the outlet gas first enters the raw material preheater to preheat the mixed raw material of natural gas and water vapor, and at the same time lower its own temperature In order to take place the shift reaction; the reaction exotherm of the shift reaction will be taken away from the reaction unit through the natural gas preheater;
  • the invention discloses a device for preparing hydrogen-containing products from natural gas based on new energy consumption, including a natural gas raw material inlet, a refined desulfurization unit, a raw material preheater, a conversion reaction unit, an electrothermal conversion unit, a feed water preheater, a high-temperature heat pump, Hydrogen-rich fuel outlet, feed water inlet and flow mixer; the shift reaction unit is equipped with a natural gas preheater;
  • the inlet of the natural gas raw material is connected to the inlet of the refined desulfurization unit through the natural gas preheater, the outlet of the refined desulfurization unit is connected to the inlet of the cold end of the raw material preheater through the mixer, and the outlet of the hot end of the raw material preheater is connected to the inlet of the electrothermal conversion unit.
  • the outlet of the conversion unit is connected to the inlet of the hot end of the raw material preheater, the outlet of the cold end of the raw material preheater is connected to the inlet of the conversion reaction unit, the outlet of the conversion reaction unit is connected to the inlet of the hot end of the feed water preheater through the steam superheater, and the feed water preheater
  • the outlet of the cold end of the heater is connected to the inlet of the high-temperature side of the high-temperature heat pump, and the low-temperature side of the high-temperature heat pump is connected to the product output unit;
  • the low-temperature side of the high-temperature heat pump is connected to the inlet of the hydrogen splitter through the CO 2 removal unit, and the outlet of the hydrogen splitter is connected to the rich The hydrogen fuel outlet is connected;
  • the feedwater inlet is connected to the inlet of the cold end of the feedwater preheater, the outlet of the hot end of the feedwater preheater is connected to the inlet of the high temperature side of the high temperature heat pump, and the outlet of the high temperature side of the high temperature heat pump is connected to the mixer through the steam superheater.
  • the outlet of the hydrogen splitter is connected to the inlet of the refining desulfurization unit;
  • a gas-liquid separation unit is also provided on the pipeline between the CO removal unit and the inlet of the hydrogen splitter;
  • a flash evaporator is provided on the high temperature side of the high temperature heat pump, and a heat storage container is provided on the low temperature side of the high temperature heat pump.
  • a steam compressor is provided on the pipeline between the high temperature side outlet of the high temperature heat pump and the steam superheater;
  • the electrothermal conversion unit is equipped with an electrothermal furnace
  • the device for preparing hydrogen-containing products from natural gas based on new energy consumption also includes a renewable power interface, and the electric furnace, high-temperature heat pump, and steam compressor use external renewable energy through the renewable power interface.
  • the invention discloses a method for using the above-mentioned natural gas based on new energy consumption to prepare hydrogen-containing products, including the following operating steps:
  • the natural gas raw material enters the natural gas preheater to obtain the reaction heat from the shift reaction unit, and the temperature rises to above 300°C; at the same time, the feed water enters the feed water preheater for preliminary preheating until it becomes saturated water;
  • the natural gas raw material enters the mixer and mixes with water vapor, and then enters the electrothermal conversion unit for conversion.
  • the electrothermal conversion unit uses electric energy to heat the furnace to 800-890°C to supply heat for the conversion reaction;
  • the outlet gas of the electrothermal conversion unit contains CO, H 2 , CO 2 , CH 4 and water vapor, and the temperature is above 700°C.
  • the outlet gas first enters the raw material preheater to preheat the mixed raw material of natural gas and water vapor, and at the same time lower its own temperature In order to take place the shift reaction; the reaction exotherm of the shift reaction will be taken away from the reaction unit through the natural gas preheater;
  • the product gas at the outlet of the high-temperature heat pump can enter the CO 2 removal unit and the gas-liquid separation unit after being cooled. After the separation is completed, it will be directly output from the hydrogen-rich fuel outlet as hydrogen-rich fuel without being compressed and stored.
  • the above-mentioned device for producing hydrogen-containing products from natural gas based on new energy consumption also includes a skid box for the equipment accommodation unit, and the natural gas raw material inlet, water supply inlet and renewable power interface are respectively provided on the skid box.
  • the present invention has the following beneficial effects:
  • the invention discloses a device for preparing hydrogen-containing products from natural gas based on new energy consumption. After natural gas passes through a natural gas preheater and a refined desulfurization unit, it mixes with preheated water vapor, and then passes through an electrothermal conversion unit and a conversion reaction unit in sequence. 1.
  • the pressure swing adsorption unit completes hydrogen production.
  • the hot fluid of the feedwater preheater is connected to the low-temperature side of the steam superheater and the high-temperature heat pump through the pipeline
  • the cold fluid of the feedwater preheater is connected to the inlet of the feedwater (de-salted water) and the high-temperature side of the high-temperature heat pump through the pipeline.
  • the waste heat of the reaction product is obtained through the steam superheater, feed water preheater and high temperature heat pump to reduce the energy consumption of production and preparation.
  • the present invention uses natural gas as fuel in the existing natural gas reforming hydrogen production technology, uses the generated high-temperature flue gas as a heat source and produces a large amount of carbon emissions, and realizes The efficient use of electric energy simplifies the structure of the original device, reduces the start-up and stop time of the device, makes the device more integrated, and improves the overall stability of the device.
  • the original natural gas hydrogen production equipment is improved by using renewable energy and electric energy through electrothermal reformer, high-temperature heat pump, steam compressor and other equipment.
  • Regenerated electric energy provides a solution to the problem of abandoning wind and solar.
  • the invention discloses a hydrogen production method using the above-mentioned device for preparing hydrogen-containing products from natural gas based on new energy consumption. After natural gas passes through a natural gas preheater and a refined desulfurization unit, it mixes with preheated water vapor, and then passes through electric heating in sequence. The conversion unit, shift reaction unit, and pressure swing adsorption unit complete hydrogen production. A solution is given to the problem of insufficient renewable energy consumption capacity and the problem of clean fuel, and at the same time, an efficient utilization method of different grades of heat energy in a highly integrated natural gas reforming hydrogen production system is given.
  • the invention discloses another device for preparing hydrogen-containing products based on natural gas absorbed by new energy sources.
  • the obtained product gas can enter the CO2 removal unit and the gas-liquid separation unit after shift reaction and multi-stage heat exchange cooling. After the separation is completed It is directly output as hydrogen-rich fuel without being compressed and stored.
  • the invention also discloses a hydrogen-rich fuel method using another device for preparing hydrogen-containing products from natural gas based on new energy consumption, which greatly reduces carbon emissions in the process of hydrogen production from natural gas and improves the energy conversion efficiency of fuel gas.
  • the device is a skid-mounted box structure, which can be transported by vehicles.
  • the skid-mounted structure is designed to efficiently integrate the equipment involved in the reaction process, effectively utilize the heat produced or waste heat in the reaction process, and improve the efficiency of the device.
  • the equipment selection and process flow of the present invention are not limited to the skid-mounted structure, and can also be suitable for large-scale hydrogen production by absorbing natural gas with electricity.
  • the device for preparing hydrogen-containing products based on new energy consumption of natural gas has the following advantages: 1. Electrification of gas hydrogen production: by introducing electrothermal conversion units, high-temperature heat pumps and steam compressors, the device can Efficient use of electric energy to participate in the reaction greatly simplifies the structure of the device, and at the same time removes the natural gas combustion link, significantly reducing carbon emissions in the process of hydrogen production from natural gas.
  • the skid-mounted structure integrates the natural gas water vapor hydrogen production device in the container to improve the integration of the device and equipment, which can effectively reduce the production cycle of the device, reduce land costs, and help to improve renewable energy. The flexibility of power consumption.
  • Cascade utilization of waste heat Design multi-stage waste heat recovery devices, including heat exchangers and high-temperature heat pumps, to effectively use the heat produced or waste heat in the reaction process, and improve the efficiency of the device.
  • the device has a renewable power interface, water supply (de-salted water) inlet, natural gas raw material inlet, and hydrogen refueling port.
  • water supply de-salted water
  • natural gas raw material inlet natural gas raw material inlet
  • hydrogen refueling port hydrogen refueling port
  • Fig. 1 is a structural schematic diagram of a skid-mounted natural gas hydrogen production device based on new energy consumption according to the present invention
  • Fig. 2 is a schematic structural diagram of a skid-mounted natural gas hydrogen-rich fuel preparation device based on new energy consumption according to the present invention.
  • 100- skid box 200- refined desulfurization unit; 201- electrothermal conversion unit; 202- conversion reaction unit; 203- pressure swing adsorption unit; 204- gas-liquid separation unit; 205- electric furnace; Removal unit; 300-steam superheater; 301-natural gas preheater; 302-feed water preheater; 303-raw material preheater; 400-high temperature heat pump; 401-flash evaporator; 402-heat storage container; 500-hydrogen split 501-Hydrogen compressor; 502-Hydrogen three-way valve; 503-Hydrogen storage unit; 504-Hydrogen refueling port; ; B-water supply inlet; C-renewable power supply interface.
  • the present invention provides a device for preparing hydrogen-containing products from natural gas based on new energy consumption, which constitutes a skid-mounted natural gas hydrogen production device based on new energy consumption, specifically including:
  • Skid box 100 refined desulfurization unit 200, electrothermal conversion unit 201, shift reaction unit 202, pressure swing adsorption unit 203, gas-liquid separation unit 204, steam superheater 300, natural gas preheater 301, feed water preheater 302, raw material Preheater 303, high temperature heat pump 400, flash evaporator 401, heat storage container 402, hydrogen splitter 500, hydrogen compressor 501, hydrogen three-way valve 502, hydrogen storage unit 503, hydrogenation port 504, flow mixer 600, vapor compression Machine 700, natural gas raw material inlet A, feed water inlet (feed water (de-salted water) inlet) B, and renewable power interface C.
  • the skid box 100 is an equipment accommodation unit; the electrothermal conversion unit 201 is provided with an electrothermal furnace 205 to ensure the reaction temperature; the inlet of the electrothermal conversion unit 201 is connected with the hot end outlet of the raw material preheater 303 through a pipeline, and the electrothermal conversion The outlet of the unit 201 is connected to the inlet of the hot end of the raw material preheater 303 through a pipeline; a natural gas preheater 301 is provided in the shift reaction unit 202 to cool down the temperature of the shift reaction while preheating the raw material; the high temperature side of the high temperature heat pump 400 is equipped with The flash evaporator 401 is used to generate steam.
  • the low temperature side of the high temperature heat pump 400 is provided with a heat storage container 402.
  • the heat storage container 402 is used as the cold end of the high temperature steam heat pump 400 to cool the reaction products and store the thermal energy of the reactants.
  • the outlet of the low temperature side of the high temperature heat pump 400 is connected to the inlet of the hydrogen splitter 500 through the pressure swing adsorption unit 203 , and the outlet of the high temperature side of the high temperature heat pump 400 is connected to the mixer 600 through the steam superheater 300 .
  • a gas-liquid separation unit 204 is also provided on the pipeline between the PSA unit 203 and the inlet of the hydrogen splitter 500 ; the PSA unit 203 is connected to the natural gas preheater 301 .
  • a steam compressor 700 is provided on the pipeline between the hot end of the high temperature heat pump 400 and the steam superheater 300 .
  • the electrothermal furnace 205, high temperature heat pump 400, hydrogen compressor 501, and steam compressor 700 in the electrothermal conversion unit 201 use external renewable energy through the renewable power interface C.
  • the feed water preheater 302 is connected to the high temperature side of the steam superheater 300 and the high temperature heat pump 400 through pipelines, the feed water inlet B is connected to the cold end inlet of the feed water preheater 302, and the hot end outlet of the feed water preheater 302 is connected to the high temperature heat pump
  • the high temperature side inlet at 400 is connected, and the feed water passes through the steam superheater 300 , the feed water preheater 302 , and the high temperature heat pump 400 to obtain the waste heat of the reaction product.
  • the high temperature heat pump 400 uses renewable electric energy, and the heat source is the heat energy of the outlet gas of the pressure swing adsorption unit 203.
  • the high temperature side inlet of the high temperature heat pump 400 is connected to the cold end outlet of the feed water preheater 302 and the flash evaporator 401 through pipelines.
  • the preheated feed water is upgraded to saturated water through the high-temperature heat pump 400, the flash evaporator 401 evaporates the saturated water to form steam, and the steam compressor 700 compresses the generated steam.
  • the high temperature heat pump 400 is provided with a heat storage container 402 to collect the waste heat of the reaction product and cool it down.
  • the hot fluid in the steam superheater 300 is connected to the feedwater preheater 302 and the shift reaction unit 202 through pipelines, and the cold fluid in the steam superheater 300 is connected to the flash evaporator 401 and the flow mixer 600 through pipelines.
  • the heat source of the natural gas preheater 301 in the shift reaction unit 202 is the heat released by the reaction in the shift reaction unit 202 , and the cold end of the natural gas preheater 301 is connected to the inlet A of the natural gas raw material and the inlet of the refined desulfurization unit 200 through pipelines.
  • the outlet of the cold end of the raw material preheater 303 is connected to the inlet of the conversion reaction unit 202, the outlet of the conversion reaction unit 202 is connected to the inlet of the hot end of the feed water preheater 302 through the steam superheater 300, and the hot fluid pipe of the raw material preheater 303 is connected to the electric heater
  • the outlet of the conversion unit 201 is connected to the inlet of the conversion reaction unit 202
  • the raw material preheater 303 is connected to the outlet of the flow mixer 600 and the inlet of the electrothermal conversion unit 201 by a cold fluid pipe.
  • the inlet of the cold end of the raw material preheater 303 is connected to the outlet of the refined desulfurization unit 200 through the mixer 600 , and the natural gas raw material inlet A is connected to the inlet of the refined desulfurization unit 200 through the natural gas preheater 301 .
  • One of the hydrogen outlets of the hydrogen splitter 500 can divert part of the hydrogen to supply the refining desulfurization unit 200 and connect with the inlet of the refining desulfurization unit 200.
  • the other hydrogen outlet of the hydrogen splitter 500 is connected to the hydrogenation port 504.
  • a hydrogen three-way valve 502 is provided on the pipeline between the hydrogen port 504, a hydrogen compressor 501 is provided on the pipeline between the outlet of the hydrogen splitter 500 and the hydrogen three-way valve 502, and a hydrogen compressor 501 is provided on the pipeline between the hydrogen three-way valve 502 and the hydrogenation port 504.
  • a hydrogen storage unit 503 is provided on the pipeline between them, and the hydrogen splitter 500 does not split when the natural gas raw material inlet A is fed with hydrogen-doped natural gas.
  • the hydrogen three-way valve 502 is used to control the external supply of the produced hydrogen or the storage in the device.
  • the present invention provides another device for preparing hydrogen-containing products from natural gas based on new energy consumption, which constitutes a skid-mounted natural gas hydrogen-rich fuel preparation device based on new energy consumption, specifically including:
  • Skid box 100 refined desulfurization unit 200, electrothermal conversion unit 201, shift reaction unit 202, gas-liquid separation unit 204, CO removal unit 206, steam superheater 300, natural gas preheater 301, feed water preheater 302, Raw material preheater 303, high temperature heat pump 400, flash evaporator 401, heat storage container 402, hydrogen splitter 500, hydrogen compressor 501, hydrogen three-way valve 502, hydrogen storage unit 503, hydrogen-rich fuel outlet 505, flow mixer 600, Steam compressor 700, natural gas raw material inlet A, feed water inlet B, and renewable power interface C.
  • the skid box 100 is an equipment accommodation unit; the electrothermal conversion unit 201 is provided with an electrothermal furnace 205 to ensure the reaction temperature; the inlet of the electrothermal conversion unit 201 is connected with the hot end outlet of the raw material preheater 303 through a pipeline, and the electrothermal conversion The outlet of the unit 201 passes through the pipeline and the hot end inlet of the raw material preheater 303; the shift reaction unit 202 is equipped with a natural gas preheater 301 for cooling the shift reaction while preheating the raw material; the high temperature side of the high temperature heat pump 400 is equipped with a flash evaporator 401 is used to generate steam.
  • the low-temperature side of the high-temperature heat pump 400 is provided with a heat storage container 402.
  • the heat storage container 402 is used as the cold end of the high-temperature steam heat pump 400 to cool the reaction products and store the heat energy of the reactants.
  • the low-temperature side outlet of the high-temperature heat pump 400 is connected to the inlet of the hydrogen splitter 500 through the CO removal unit 206
  • the high-temperature side outlet of the high-temperature heat pump 400 is connected to the flow mixer 600 through the steam superheater 300 .
  • a gas-liquid separation unit 204 is also provided on the pipeline between the CO 2 removal unit 206 and the inlet of the hydrogen splitter 500 .
  • a steam compressor 700 is provided on the pipeline between the high temperature side of the high temperature heat pump 400 and the steam superheater 300 .
  • the electrothermal furnace 205, the high temperature heat pump 400, and the steam compressor 700 in the electrothermal conversion unit 201 use external renewable energy through the renewable power interface C.
  • the hot end of the feedwater preheater 302 is connected to the cold end of the steam superheater 300 and the high temperature heat pump 400 through pipelines, the feedwater inlet B is connected to the inlet of the cold end of the feedwater preheater 302, and the outlet of the hot end of the feedwater preheater 302 is connected to and The high temperature side inlet of the high temperature heat pump 400 is connected, and the feed water passes through the steam superheater 300, the feed water preheater 302, and the high temperature heat pump 400 to obtain the waste heat of the reaction product.
  • the high-temperature heat pump 400 uses renewable electric energy, and the heat source is the medium-temperature thermal energy of the outlet gas of the pressure swing adsorption unit 203 .
  • the preheated feed water is upgraded to saturated water through the high-temperature heat pump 400, the flash evaporator 401 evaporates the saturated water to form steam, and the steam compressor 700 compresses the generated steam.
  • the high temperature heat pump 400 is provided with a heat storage container 402 to collect the waste heat of the reaction product and cool it down.
  • the hot fluid in the steam superheater 300 is connected to the feedwater preheater 302 and the shift reaction unit 202 through pipelines, and the cold fluid in the steam superheater 300 is connected to the flash evaporator 401 and the flow mixer 600 through pipelines.
  • the heat source of the natural gas preheater 301 in the shift reaction unit 202 is the heat released by the reaction in the shift reaction unit 202 , and the cold end of the natural gas preheater 301 is connected to the inlet A of the natural gas raw material and the inlet of the refined desulfurization unit 200 through pipelines.
  • the outlet of the cold end of the raw material preheater 303 is connected to the inlet of the conversion reaction unit 202, the outlet of the conversion reaction unit 202 is connected to the inlet of the hot end of the feed water preheater 302 through the steam superheater 300, and the hot end of the raw material preheater 303 is connected to the electrothermal conversion
  • the outlet of the unit 201 is connected to the inlet of the conversion reaction unit 202
  • the cold fluid pipeline of the raw material preheater 303 is connected to the outlet of the flow mixer 600 and the inlet of the electrothermal conversion unit 201 .
  • the inlet of the cold end of the raw material preheater 303 is connected to the outlet of the refined desulfurization unit 200 through the mixer 600 , and the natural gas raw material inlet A is connected to the inlet of the refined desulfurization unit 200 through the natural gas preheater 301 .
  • One of the hydrogen outlets of the hydrogen splitter 500 can divert part of the hydrogen to supply the refined desulfurization unit 200 and connect with the inlet of the refined desulfurization unit 200.
  • the other hydrogen outlet of the hydrogen splitter 500 is connected to the hydrogen-rich fuel outlet 505.
  • the hydrogen gas splitter 500 does not split the flow when the hydrogen-doped natural gas is used.
  • the multiple electrothermal conversion tubes contained in the electrothermal conversion unit 201 are not limited to two. All heat exchangers are arranged according to the heat capacity flow rate matching method, so that the heat capacity flow rates of the hot fluid and the cold fluid in the heat exchanger are as consistent as possible, reducing the heat exchange temperature difference between the cold and hot fluids, and ensuring the efficiency of the heat exchanger. In order to meet the matching of the heat capacity flow rate of the cold and hot flow of the heat exchanger and improve the conversion rate of natural gas, the reaction water-to-carbon ratio should be greater than 4.
  • the device for preparing hydrogen-containing products based on natural gas absorbed by new energy in the present invention
  • the device is a skid-packed box structure that can be transported by vehicles.
  • the equipment selection and process flow of the present invention are not limited to the skid-mounted structure, and are also suitable for large-scale hydrogen production by absorbing natural gas with electricity.
  • the present invention provides a device for preparing hydrogen-containing products based on natural gas absorbed by new energy.
  • the device for preparing hydrogen-containing products based on natural gas absorbed by new energy can realize two preparation modes: 1) including Under the operating strategy with higher purity, that is, to use the device for producing hydrogen-containing products based on new energy consumption natural gas to realize hydrogen production; 2) to use the device for producing hydrogen-containing products based on new energy consumption natural gas to realize production Take hydrogen-rich fuel.
  • the reaction path of each raw material is as follows:
  • the equipment contained in the device can be mainly divided into five modules, among which the skid box 100 is the equipment accommodation unit; the refined desulfurization unit 200, the electrothermal conversion unit 201, the conversion reaction unit 202, the pressure swing adsorption unit 203 and the gas-liquid separation unit 204 constitute the natural gas production unit.
  • Hydrogen module; steam superheater 300, natural gas preheater 301, feed water preheater 302 and raw material preheater 303 constitute a waste heat recovery module in the hydrogen production process;
  • high temperature heat pump 400, flash evaporator 401 and heat storage container 402 constitute a high temperature heat pump Module;
  • hydrogen splitter 500, hydrogen compressor 501, hydrogen three-way valve 502, hydrogen storage unit 503 and hydrogenation port 504 constitute a hydrogen processing module.
  • the reaction path sequence of natural gas raw material is natural gas preheater 301, refining desulfurization unit 200, mixer 600, raw material preheater 303, electrothermal conversion unit 201, raw material preheater 303, shift reaction unit 202, steam superheater 300, Feed water preheater 302, high temperature heat pump 400, pressure swing adsorption unit 203, gas-liquid separation unit 204, hydrogen splitter 500, hydrogen compressor 501, hydrogen three-way valve 502, hydrogenation port 504 or hydrogen storage unit 503.
  • each device is connected through a gas pipeline.
  • the sequence of feed water entering the reactor is feed water preheater 302 , high temperature heat pump 400 , flash evaporator 401 , steam compressor 700 , steam superheater 300 , and flow mixer 600 .
  • the electric heating furnace 205, high temperature heat pump 400, hydrogen compressor 501, and steam compressor 700 in the electrothermal conversion unit 201 all use external renewable energy through the renewable power interface C, and the external electric energy should be general alternating current;
  • the water supply inlet B should be The water after the desalination treatment is connected, and the pressure should not exceed 0.5MPa, so that the saturation temperature is not higher than 150°C to meet the evaporation process of the high-temperature heat pump 400;
  • the steam compressor 700 is preferably a screw-type steam compressor, which can compress water vapor to Above 1.5MPa meets the reaction pressure.
  • the design and layout of the heat exchanger follows the heat capacity flow rate matching.
  • the specific heat capacity of the reaction product is higher than the specific heat capacity of the raw material and feed water. In order to make the heat capacity of the cold and hot fluids in the heat exchanger closer, the inlet water-to-carbon ratio should be greater than 4.
  • the heat source of the high temperature heat pump 400 is the heat accumulated in the heat storage container 402.
  • the heat comes from the heat energy of the output product after the heat exchange of the feed water preheater 302.
  • the internal temperature of the heat storage container 402 should be higher than 80°C.
  • the hot end of the high-temperature heat pump 400 is connected to the feedwater preheater 302 and the flash evaporator 401 through pipelines.
  • the internal working medium of the high-temperature heat pump 400 has an evaporation temperature of around 80°C on the low-pressure side, and a high-pressure condensation temperature of 150°C; the high-temperature heat pump module includes a flash evaporator 401,
  • the flash evaporator can flash saturated water at 150°C into steam for output.
  • the high-temperature heat pump 400 improves the thermal energy grade, heats the preheated feed water into saturated water, and the flash evaporator 401 evaporates the saturated water to form steam.
  • the heat source of the natural gas preheater 301 in the shift reaction unit 202 is the heat released by the reaction in the shift reaction unit 202 , and the cold end is connected to the natural gas raw material inlet A and the refined desulfurization unit 200 through pipelines. Part of the heat of the shift reaction unit is taken away by the raw natural gas to realize the cooling of the shift reaction, which is conducive to the positive progress of the shift reaction and can realize the preheating of the natural gas raw material.
  • Hydrogen is separated from the hydrogen splitter 500 including hydrogen, and part of the hydrogen is supplied to the refining desulfurization unit 200, because the reaction in the refining desulfurization unit requires hydrogen to participate.
  • One of the reactions includes olefin saturation reactions. Due to the presence of olefin double bonds, the molecular carbon-hydrogen ratio is high. Carbon deposition is easy to form during the high-temperature conversion reaction. Converting olefins to alkanes can help reduce the carbon deposition of the catalyst in the reformer, increase the service life of the catalyst and reduce the difficulty of catalyst replacement.
  • hydrogen reacts with olefins Produces alkanes.
  • the second reaction is the conversion reaction of organic sulfur-containing compounds.
  • Hydrogen reacts with organic sulfur-containing compounds including mercaptan, sulfide, disulfide, thiophene, carbon oxysulfide, carbon disulfide, etc. under catalytic action to form H 2 S , and then solidify the sulfur by reacting with ZnO (solid).
  • the hydrogen splitter 500 does not supply hydrogen to the refining desulfurization unit 200 .
  • the hydrogen three-way valve 502 is used to control the external supply or internal storage of the produced hydrogen, which depends on the work performed by the skid-mounted device and the environment provided on site. When the hydrogen storage equipment is provided on site, it can be output externally. Hydrogen storage equipment not provided will be stored in hydrogen storage tanks in the unit.
  • the product gas can enter the CO 2 removal unit 206 and the gas-liquid separation unit 204 after the transformation reaction and multi-stage heat exchange cooling. It is directly output as hydrogen-rich fuel without being compressed and stored.
  • the invention also provides the operation steps of the device for preparing hydrogen-containing products from natural gas based on new energy consumption. It also corresponds to the operation steps in the two modes of hydrogen production and hydrogen-rich fuel production. Therefore, the specific Methods include the following:
  • the natural gas raw material enters the natural gas preheater 301 to obtain the reaction heat from the shift reaction unit 202, and the temperature rises to above 300°C; at the same time, the feed water (de-salted water) enters the feed water preheater 302 for preliminary preheating until it becomes saturated water .
  • Carbon oxysulfide COS+H 2 ⁇ CO+H 2 S
  • the natural gas raw material enters the mixer 600 to mix with water vapor, and then enters the electrothermal conversion unit 201 for conversion.
  • the electrothermal conversion unit 201 uses electric energy to heat the furnace to 800-890°C to supply the conversion reaction to absorb heat.
  • the conversion reaction equation As follows:
  • the outlet gas of the electrothermal conversion unit 201 mainly contains CO, H 2 , CO 2 , CH 4 and water vapor, and the temperature is above 700°C. After the outlet gas flows out, it first enters the raw material preheater 303 to preheat the mixed raw material of natural gas and water vapor. heat while lowering its own temperature for the shift reaction to take place. Enter conversion reaction unit 202 and take place following reaction:
  • the reaction temperature ranges from 320-420°C. This reaction is an exothermic reaction, and low temperature is conducive to the reaction. Therefore, the exothermic heat of the shift reaction will be taken away from the reaction unit through the natural gas preheater 301 .
  • the product gas after the shift reaction enters the steam superheater 300 and the feedwater preheater 302 to release heat, and then releases the heat in the heat storage container 402 provided by the high temperature heat pump 400 as a heat source for the high temperature heat pump 400 .
  • the high-temperature heat pump 400 extracts heat and uses electric energy to improve the energy grade and evaporate the saturated water at the outlet of the feed water preheater 302 .
  • the hydrogen gas enters the gas-liquid separation unit 204 after pressure swing adsorption to realize gas-liquid separation. Then enter the hydrogen splitter 500 to divert part of the hydrogen for refining and desulfurization, and most of the hydrogen enters the hydrogen compressor 501 to be compressed and then exported or stored.
  • the natural gas inlet is supplied with hydrogen-doped natural gas, it does not divert to the refined desulfurization unit 200 .
  • the working principle of the present invention is:
  • the natural gas has undergone a preheating and a prereaction before entering the electrothermal conversion unit 201.
  • the first preheating is to absorb the transformation reaction heat release in the natural gas preheater 301, and the first prereaction is to enter the refining desulfurization unit 200 to complete desulfurization;
  • Before entering the electrothermal conversion unit 201 it undergoes four stages of heating, and the required heat comes from the waste heat of the reaction process and the work of the steam compressor 700. Two of them are heated in the steam superheater 300 and the feed water preheater 302 respectively.
  • the heat source is the product waste heat of the conversion reaction unit 202.
  • the third is to use the high-temperature heat pump 400 to use the low-temperature waste heat of the product to obtain heat to complete evaporation.
  • the fourth is to use the steam compressor 700 to pressurize the steam to meet the needs of the reaction.
  • the natural gas and steam are mixed, and undergo a preheating in the raw material preheater 303 , and the heat source is the waste heat of the product of the electrothermal conversion unit 201 . After preheating, it enters the electrothermal reformer to complete the conversion. The gas at the outlet of the electrothermal conversion unit 201 undergoes four temperature drops and one exothermic reaction after being discharged.
  • the steam heated by the device 300 completes the second temperature drop; then enters the feed water preheater 302 to exchange heat with the feed water to complete the third temperature drop; then enters the high-temperature heat pump 400 to transfer heat to the feed water to complete the fourth temperature drop.
  • the lower hydrogen temperature in the gas-liquid separation unit 204 can ensure that more water can be removed and the purity of hydrogen can be improved.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
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Abstract

La présente invention se rapporte aux domaines techniques de production d'un nouvelle énergie et d'hydrogène à partir de gaz naturel, et concerne un appareil et un procédé de préparation d'un produit contenant de l'hydrogène à partir de gaz naturel sur la base d'une nouvelle consommation d'énergie. Dans l'appareil de préparation d'un produit contenant de l'hydrogène à partir de gaz naturel sur la base d'une nouvelle consommation d'énergie, du gaz naturel passe à travers un préchauffeur de gaz naturel et une unité de désulfuration fine, et est ensuite mélangé avec de la vapeur préchauffée pour former un flux, et le flux traverse séquentiellement une unité de conversion électro-thermique, une unité de réaction de conversion et une unité d'adsorption modulée en pression pour achever la production d'hydrogène ou de carburant riche en hydrogène. Au moyen de la présente invention, de nouvelles énergies peuvent être consommées de manière opportune, ce qui réduit considérablement les émissions de carbone pendant le processus de production d'hydrogène à partir de gaz naturel, et en même temps, un procédé d'utilisation efficace pour différents grades d'énergie thermique dans des conditions d'intégration élevée d'un système de production d'hydrogène au moyen d'un reformage de gaz naturel est fourni.
PCT/CN2022/093069 2021-05-21 2022-05-16 Appareil et procédé de préparation d'un produit contenant de l'hydrogène à partir de gaz naturel sur la base d'une nouvelle consommation d'énergie WO2022242598A1 (fr)

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