WO2017000780A1 - Machine de préparation d'hydrogène par reformage de méthanol-eau et procédé de préparation d'hydrogène associé - Google Patents

Machine de préparation d'hydrogène par reformage de méthanol-eau et procédé de préparation d'hydrogène associé Download PDF

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Publication number
WO2017000780A1
WO2017000780A1 PCT/CN2016/085822 CN2016085822W WO2017000780A1 WO 2017000780 A1 WO2017000780 A1 WO 2017000780A1 CN 2016085822 W CN2016085822 W CN 2016085822W WO 2017000780 A1 WO2017000780 A1 WO 2017000780A1
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hydrogen
methanol
reforming
water
reformer
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PCT/CN2016/085822
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English (en)
Chinese (zh)
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向华
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广东合即得能源科技有限公司
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Publication of WO2017000780A1 publication Critical patent/WO2017000780A1/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
    • 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

Definitions

  • the present invention relates to the technical field of hydrogen preparation equipment, and in particular, to a methanol water reforming hydrogen generator and a hydrogen production method thereof.
  • Hydrogen is one of the most ideal energy sources in the 21st century. When burning the same weight of coal, gasoline and hydrogen, hydrogen produces the most energy, and its combustion products are water, no ash and exhaust gas. , will not pollute the environment; and coal and oil combustion is mainly generated. 0 2 and 80 2 can produce greenhouse effect and acid rain, respectively. The reserves of coal and oil are limited, and hydrogen is mainly stored in water. The only product after combustion is water, which can continuously produce hydrogen and never run out. Hydrogen is widely distributed, and water is the large "warehouse" of hydrogen, which contains 11% hydrogen. About 1.5% of the hydrogen in the soil; hydrogen, coal, natural gas, animals and plants, etc. contain hydrogen.
  • the main body of hydrogen exists in the form of compound water, and about 70% of the earth's surface is covered by water, and the amount of water stored is large. Therefore, hydrogen can be said to be an "inexhaustible and inexhaustible" source of energy. If hydrogen can be produced from a suitable method, then hydrogen will also be a relatively inexpensive energy source.
  • the patent discloses a methanol water hydrogen production system, a reforming chamber of methanol and steam reformer, passing a catalyst under the pressure of 1-5 MPa at a temperature of 350-409 ° C under the action of a catalyst.
  • the methanol cracking reaction and the carbon monoxide shift reaction generate hydrogen and carbon dioxide, which is a multi-component, multi-reaction gas-solid catalytic reaction system.
  • the reaction equation is as follows: (l) CH 3 OH ⁇ CO+2H 2 ; (2) H 2 0+CO ⁇ CO 2+H 2 ; (3) CH 3OH+H 2 0 ⁇ CO 2 +3H 2 , reforming the H 2 and CO 2 formed by the reaction, and then passing through the separation chamber of the palladium membrane separator to H ⁇ nC0 2 separation, to obtain high purity hydrogen.
  • a gasification chamber for vaporizing methanol and water into steam before entering the reformer, and a combustion chamber for releasing heat by H 2 combustion, which is a reforming chamber.
  • a reforming reaction temperature of 350-409 ° C and provides heat to the gasification chamber.
  • the above-mentioned methanol water hydrogen production system also has the following drawbacks: First, since the reformer needs to set the combustion chamber, the reformer also needs to provide an air inlet fan and an air inlet for fanning the air into the air. The passage, and the smoke window for exhausting the exhaust gas generated after combustion, the high-temperature exhaust gas is discharged from the smoke window, which not only wastes heat energy, but also easily affects the operation of various parts of the hydrogen production system; Second, the combustion temperature of the hydrogen gas in the combustion chamber tends to be short.
  • the reformer is provided with a chamber such as a gasification chamber, a combustion chamber, an inlet fan, an air inlet passage, and a smoke window, etc., which increases the structural complexity and maintenance difficulty of the reformer.
  • the reformer of the invention patent is provided with a reforming chamber and an electric heater, the electric heater provides heat energy for the reforming chamber, a catalyst is arranged in the reforming chamber, methanol and water are generated in the reforming chamber, methanol and water
  • the reforming hydrogen production reaction produces a high temperature mixed gas mainly composed of carbon dioxide and hydrogen; specifically, the electric heater includes a resistance heating body and a metal casting heat conductor.
  • the reformer of the hydrogen generator is provided with an electric heater for heating the reforming chamber, the reformer does not need to provide a combustion chamber, an inlet fan, an air inlet passage and a smoke window, and is a closed reformer as a whole. It will not emit high-temperature exhaust gas, avoiding waste of heat energy, avoiding the operation of various parts of the hydrogen production system due to high-temperature exhaust gas, avoiding the damage to the reformer due to combustion, and reducing the structural complexity and maintenance of the reformer. Difficulty, the heating temperature of the electric heater is also easier to control.
  • the electric heater used in the methanol water hydrogen generator is a resistance heating body and a metal casting heat conductor, and has the following defects: First, the service life is short, the maintenance amount is large, and the electric heater uses the resistance heating body. Heat, metal casting heat conduction heat conduction, when the temperature reaches 405-570 °C, the resistance wire is easy to be blown due to high temperature and aging, the life of the commonly used resistance heating body is less than half a year, so the maintenance workload is relatively large; Second, the use of resistance heating body heating, metal casting heat conduction heat conduction method, its thermal hysteresis is large, control The device is not easy to accurately control the temperature of the reforming chamber; thirdly, the heat of the resistance heating body and the heat conduction of the metal casting heat conductor are used, the restarting speed of the reformer is slow, and the starting time is usually more than 3 minutes; The thermal efficiency is low, usually only 50% of the electrical energy is used, and the heating is uneven.
  • the technical problem to be solved by the present invention is to provide a methanol water reforming hydrogen generator with the above-mentioned deficiencies in the prior art, and the reformer of the hydrogen generator does not need to be provided with a combustion chamber, an inlet fan, and a feed.
  • the air passage and the smoke window are simple in structure, long in service life, small in maintenance, small in thermal hysteresis, precise in control, fast in reformer, high in thermal efficiency, and uniform in heating; therefore, the present invention also provides a The hydrogen production method of the methanol water reforming hydrogen generator.
  • a methanol water reforming hydrogen generator comprising a methanol water storage container, a transfer pump, a heat exchanger and a reformer, wherein:
  • a methanol water storage container in which liquid methanol and water are stored
  • a transfer pump for conveying methanol and water in the methanol water storage container to the reforming chamber of the reformer
  • the heat exchanger is installed on a conveying pipe between the conveying pump and the reformer, and the low temperature methanol and water are exchanged in the heat exchanger with the high temperature hydrogen gas output from the reformer, and the temperature of the methanol and the water rises. High, hydrogen temperature is lowered;
  • the reformer is provided with a reforming chamber, an electromagnetic heater and a hydrogen purifying device, wherein the electromagnetic heater comprises an electromagnetic coil and a metal-receiving magnet, and the electromagnetic coil can generate a high-frequency magnetic field after being energized, so that the metal receives the magnetic field by the magnet Inductively generating heat, providing heat to the reforming chamber;
  • the reforming chamber is provided with a catalyst, and methanol and water are reacted in the reforming chamber to produce hydrogen and hydrogen to produce a high-temperature mixed gas mainly composed of carbon dioxide and hydrogen;
  • the reforming chamber and the hydrogen purifying device are connected by a connecting pipe, and all or part of the connecting pipe is disposed in the reforming chamber, and the high-temperature mixed gas output from the reforming chamber can be continuously heated by the high temperature in the reforming chamber;
  • the pipeline acts as a buffer between the reforming chamber and the hydrogen purifying device, so that the temperature of the high temperature mixed gas output from the reforming chamber is the same as or close to the temperature of the
  • the methanol water reforming hydrogen generator further includes a gas splitter, a fuel cell, and an AC/DC power conversion device.
  • the gas splitter is configured to split the hydrogen gas output from the heat exchanger, and after the gas splitter is diverted, part of the hydrogen gas enters the fuel cell; the fuel cell is used for electrochemical reaction of hydrogen and oxygen in the air to generate electric energy; After being converted by the AC/DC power conversion device, the electromagnetic heaters of the transfer pump and the reformer are powered. Further, the electric power supplied to the electromagnetic heater by the AC/DC power conversion device is a high frequency high voltage of 20-4 0 KHz.
  • the methanol water reforming hydrogen generator further comprises a hydrogen storage bottle, wherein the hydrogen storage bottle can input hydrogen into the fuel cell during the startup of the reformer, and the fuel cell operates to generate electric energy, and is a transfer pump and a reformer.
  • the electromagnetic heater is powered.
  • the reformer includes, in order from the outside to the inside, a heat preservation casing, a reforming chamber, and a hydrogen purification device, wherein the electromagnetic coil of the electromagnetic heater is disposed between the heat insulation casing and the reforming chamber, and the metal is subjected to The magnet is placed in the reforming chamber. Further, the metal is provided with a single layer or a plurality of layers by the magnet, and the metal is magnetized in a cylindrical structure or a mesh structure.
  • the outer and inner sides of the reforming chamber are also provided with vaporization coils through which methanol and water pass through the vaporization coil to vaporize methanol and water.
  • the hydrogen purification device is a membrane separation device for vacuum plating a palladium-silver alloy on a porous ceramic surface, the coating layer is a palladium-silver alloy, and the palladium-silver alloy has a mass percentage of palladium of 75%-78 ⁇ 3 ⁇ 4, and silver accounts for 22 ⁇ 3 ⁇ 4. -25%.
  • a hydrogen production method for a methanol water reforming hydrogen generator comprising the following steps:
  • a control device controls the start of the methanol water reforming hydrogen generator, the transfer pump passes the methanol and water in the methanol water storage container through the heat exchanger, and then is sent to the reforming chamber of the reformer, in the heat exchanger , methanol and water temperature increase, hydrogen temperature decreases;
  • control device controls the electromagnetic heater of the reformer, the electromagnetic coil of the electromagnetic heater is energized to generate a high-frequency magnetic field, so that the metal of the electromagnetic heater is heated by the magnetic field to induce heat, providing 350 for the reforming chamber -57 0 ° C temperature, in the reforming chamber, vaporized methanol and water under the action of a catalyst, methanol and water reforming hydrogen production reaction, to produce carbon dioxide and hydrogen-based high temperature mixed gas;
  • the high-temperature mixed gas is separated into a hydrogen purifying device of the reformer through a connecting line, and high-temperature hydrogen is obtained from the gas producing end of the hydrogen purifying device, and the high-temperature hydrogen is cooled by the heat exchanger and then output.
  • the hydrogen outputted in the step C passes through the gas splitter, part of the hydrogen enters the fuel cell.
  • the hydrogen in the hydrogen and the air reacts electrochemically to generate electric energy, and the generated electric energy is passed through the AC/DC power conversion device.
  • the AC/DC power conversion device in order to supply power to the electromagnetic heater of the transfer pump and the reformer, wherein the AC and DC power
  • the power supplied by the force conversion device to the electromagnetic heater is a high frequency high voltage of 20-40 KHZ.
  • the beneficial effects of the present invention are as follows: 1. Since the reformer of the present invention is provided with an electromagnetic heater for heating the reforming chamber, the reformer does not need to be provided with a combustion chamber, an inlet fan, an air inlet passage, and a smoke.
  • the window as a whole, is a closed reformer, which does not emit high-temperature exhaust gas, avoids waste of heat energy, and avoids the operation of various parts of the hydrogen production system due to high-temperature exhaust gas, thereby avoiding the problem of damage to the reformer due to combustion; 2.
  • the invention adopts an electromagnetic heater to the reforming chamber. Since the electromagnetic coil itself does not generate heat substantially, the service life is long, no maintenance is required, no maintenance and replacement cost, the service life is up to 10 years, and the basic maintenance cost is not later.
  • the electromagnetic coil can generate a high-frequency magnetic field after being energized, so that the metal is heated by the magnetic field and rapidly generates heat, which provides heat energy for the reforming chamber.
  • the heating method has a small thermal hysteresis, and the control device can easily and accurately control the reforming.
  • the temperature is four; the metal is magnetized by the magnetic field to induce rapid heating.
  • the reformer starts very fast and the efficiency is very high. It has been proved by experiments that the starter of the reformer can be reduced to 10 seconds; 5.
  • the electromagnetic heater has a very high thermal efficiency, can use more than 95% of electrical energy, and is evenly heated.
  • the electric energy of the electromagnetic heater and the transfer pump is provided by the fuel cell, and the hydrogen required for the fuel cell is derived from the hydrogen produced by the present invention. Therefore, the present invention does not require external commercial power, that is, The work of the electromagnetic heater and the transfer pump can be realized, so that the invention is highly adaptable and is not limited by geographical conditions and commercial power.
  • FIG. 1 is a block diagram showing the overall structure of the present invention.
  • FIG. 2 is a schematic view showing the external structure of the reformer and the heat exchanger of the present invention.
  • FIG 3 is a cross-sectional view showing the structure of a reformer according to a preferred embodiment of the present invention.
  • FIG. 4 is a schematic view showing a preferred structure of a metal-receiving magnet.
  • FIG. 5 is a schematic view showing another preferred structure of a metal-receiving magnet.
  • a methanol water reforming hydrogen generator includes a methanol water storage container 1, a transfer pump 2, a heat exchanger 3, and a reformer 4, wherein:
  • a methanol water storage container 1 which stores liquid methanol and water therein;
  • a transfer pump 2 used to transport methanol and water in the methanol water storage container 1 to the reforming chamber 41 of the reformer 4;
  • the heat exchanger 3 is installed on a conveying pipe between the transfer pump 2 and the reformer 4, and low-temperature methanol and water are exchanged in the heat exchanger 3 with the high-temperature hydrogen gas output from the reformer 4, The temperature of methanol and water increases, and the temperature of hydrogen decreases.
  • the reformer 4 is provided with a reforming chamber 41, an electromagnetic heater 42 and a hydrogen purifying device 43.
  • the electromagnetic heater 42 includes an electromagnetic coil and a metal-receiving magnet, and the electromagnetic coil can generate a high-frequency magnetic field after being energized.
  • the metal is heated by the magnetic field induced by the magnetic field, and the reforming chamber 41 is supplied with thermal energy of 350-570 ° C, preferably 350-409 ° C; the reforming chamber 41 is provided with a catalyst, methanol and water vapor are heavy.
  • a catalyst is used to generate a methanol cracking reaction and a carbon monoxide shift reaction under the action of a catalyst to generate hydrogen and carbon dioxide, which is a multi-component, multi-reaction gas-solid catalyst.
  • reaction equation is: (l) CH 3 OH ⁇ CO + 2H 2 , (2) H 2 0 + CO ⁇ CO 2 + H 2 , (3) CH 3 OH + H 2 0 ⁇ CO 2+ 3H 2 a high-temperature mixed gas mainly composed of carbon dioxide and hydrogen; the reforming chamber 41 and the hydrogen purifying device 43 are connected by a connecting pipe, and all or part of the connecting pipe is disposed in the reforming chamber 41, and can pass through the reforming chamber.
  • the high temperature in 41 continues to heat the high temperature mixed gas output from the reforming chamber 41;
  • the connecting line serves as a buffer between the reforming chamber 41 and the hydrogen purifying device 43, so that the temperature of the high-temperature mixed gas output from the reforming chamber 41 is the same as or close to the temperature of the hydrogen purifying device 43; the gas generated from the hydrogen purifying device 43 Hydrogen is obtained at the end, which is output through the heat exchanger 3, and carbon dioxide gas can be discharged from the reformer or collected.
  • the methanol water reforming hydrogen generator further includes a gas splitter 5, a fuel cell 6 and an AC/DC power conversion device 7, and the gas splitter 5 is used for splitting from the heat exchanger 3.
  • the gas splitter 5 is used for splitting from the heat exchanger 3.
  • part of the hydrogen gas enters the fuel cell 6.
  • part of the hydrogen entering the fuel cell 6 accounts for only a small portion of the hydrogen output from the reformer (for example, 20% hydrogen), most of which Hydrogen is collected or exported to other hydrogen use equipment (eg, 80% hydrogen); the fuel cell 6 is used in hydrogen and air.
  • PEM proton exchange membrane
  • the electric power supplied to the electromagnetic heater 42 by the AC/DC power conversion device 7 is a high frequency high voltage of 20-40 KHz.
  • the methanol water reforming hydrogen generator is further provided with a hydrogen storage bottle 8 which can input hydrogen into the fuel cell 6 during the startup of the reformer 4 to operate the fuel cell 6 to generate electric energy for transportation.
  • the electromagnetic heater 42 of the pump 2 and the reformer 4 is powered.
  • the reformer 4 includes an insulative housing 44, a reforming chamber 41, and a hydrogen purifying device 43 in order from the outside to the inside.
  • the electromagnetic coil 421 of the electromagnetic heater 42 is disposed.
  • the metal receiving magnet 422 is disposed in the reforming chamber 41, and the metal receiving magnet may be an iron or stainless steel magnet.
  • the metal-receiving magnet 422 is provided with a single layer or a plurality of layers, and the metal-receiving magnet 422 has a cylindrical structure (refer to Fig. 4) or a mesh structure (refer to Fig. 5).
  • the outer side and the inner side of the reforming chamber 41 are also provided with a vaporizing coil 45 through which the methanol and water pass through the vaporizing coil 45 to vaporize methanol and water.
  • the hydrogen purification device 43 is a membrane separation device for vacuum-plating palladium-silver alloy on the surface of a porous ceramic, the coating layer is a palladium-silver alloy, and the palladium-silver alloy has a mass percentage of palladium of 75%-78 ⁇ 3 ⁇ 4, and silver accounts for 22%. -25 ⁇ 3 ⁇ 4;
  • the difference between the internal and external pressure of the membrane separation device is greater than or equal to 1.1 MPa.
  • the invention patent 201210563913.5 which is applied by the applicant, Shanghai Hefei Deli Hydrogen Machinery Co., Ltd.
  • the methanol water reforming hydrogen production power generation module of the invention adopts a reformer to reform hydrogen production at a temperature of 300-570 ° C and a catalyst, and the hydrogen production rate and efficiency are high, and the methanol water raw material conversion efficiency is high. High utilization rate and good stability; Since the temperature of the hydrogen purification unit is the same as or close to the temperature of the reforming chamber, it can significantly improve the hydrogen purification efficiency and reduce the difficulty of hydrogen purification, and achieve rapid membrane separation.
  • the hydrogen production method of the methanol water reforming hydrogen generator comprises the following steps:
  • a control device controls the start of the methanol water reforming hydrogen generator, the transfer pump passes the methanol and water in the methanol water storage container through the heat exchanger, and then is sent to the reforming chamber of the reformer, in the heat exchanger , methanol and water temperature increase, hydrogen temperature decreases;
  • b control device controls the electromagnetic heater of the reformer, the electromagnetic coil of the electromagnetic heater is energized to generate a high-frequency magnetic field, so that the metal of the electromagnetic heater is heated by the magnetic field to induce heat, providing 350 for the reforming chamber -57 0 ° C temperature, in the reforming chamber, vaporized methanol and water under the action of a catalyst, methanol and water reforming hydrogen production reaction, to produce carbon dioxide and hydrogen-based high temperature mixed gas;
  • the high-temperature mixed gas is separated into a hydrogen purifying device of the reformer through a connecting line, and high-temperature hydrogen is obtained from the gas producing end of the hydrogen purifying device, and the high-temperature hydrogen is cooled by the heat exchanger and then output.
  • the hydrogen outputted in the step C passes through the gas splitter, part of the hydrogen enters the fuel cell.
  • the hydrogen in the hydrogen and the air react electrochemically to generate electric energy, and the generated electric energy is passed through the AC/DC power conversion device.
  • the electric power supplied from the AC/DC power conversion device to the electromagnetic heater is a high frequency high voltage of 20-40 KHZ.
  • the present invention is a methanol water reforming hydrogen generator and a hydrogen production method, and the reformer of the hydrogen generator does not need to be provided with a combustion chamber, an inlet fan, an air inlet passage, a smoke window, and a structure. It is simpler, has long service life, small maintenance, small thermal hysteresis, precise control, fast starter speed, high thermal efficiency and uniform heating. Therefore, it has industrial applicability.

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

La présente invention concerne une machine de préparation d'hydrogène par reformage de méthanol-eau et un procédé de préparation d'hydrogène associé. La machine de préparation d'hydrogène par reformage de méthanol-eau comprend un récipient de stockage de méthanol-eau (1), une pompe d'alimentation (2), un échangeur de chaleur (3), et un reformeur (4). Le reformeur (4) est doté d'une chambre de reformage (41), d'un dispositif de chauffage électromagnétique (42), et d'un appareil de purification d'hydrogène (43). Le dispositif de chauffage électromagnétique (42) comprend une bobine électromagnétique (421) et un aimant métallique (422). La bobine électromagnétique (421) est apte à générer un champ magnétique à haute fréquence après avoir été mise sous tension, de sorte que le champ magnétique induit l'aimant métallique à émettre de la chaleur et fournir de l'énergie thermique pour la chambre de reformage (41). La chambre de reformage (41) est utilisée pour conduire une réaction de préparation d'hydrogène par reformage avec du méthanol et de l'eau, de sorte qu'un gaz mélangé à température élevée contenant principalement de l'hydrogène et du dioxyde de carbone est obtenu. Après que le gaz mélangé à température élevée sortant de la chambre de reformage (41) soit séparé par l'appareil de purification d'hydrogène (43), l'hydrogène est obtenu à partir de l'extrémité de génération d'hydrogène de l'appareil de purification d'hydrogène (43). La machine de préparation d'hydrogène par reformage de méthanol-eau a une longue durée de vie, nécessite peu d'entretien, présente un faible retard thermique, un contrôle précis, une vitesse de démarrage rapide du reformeur, une efficacité thermique élevée et un chauffage régulier.
PCT/CN2016/085822 2015-06-29 2016-06-15 Machine de préparation d'hydrogène par reformage de méthanol-eau et procédé de préparation d'hydrogène associé WO2017000780A1 (fr)

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CN201510363608.5 2015-06-29
CN201510363608.5A CN104986731A (zh) 2015-06-29 2015-06-29 一种甲醇水重整制氢机及其制氢方法

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CN109133003A (zh) * 2018-10-29 2019-01-04 浙江氢谷新能源汽车有限公司 用于纯电动汽车一体化燃料电池的甲醇制氢系统
CN109399561B (zh) * 2018-12-19 2022-08-30 天津工业大学 一种在线制氢系统及方法
CN109956450A (zh) * 2019-04-30 2019-07-02 广西氢朝能源科技有限公司 一种甲醇水即时制氢系统及其制氢方法
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CN110649285B (zh) * 2019-09-30 2022-09-02 西安新衡科测控技术有限责任公司 一种基于ht-pem的甲醇水燃料电池重整室进液泵控制方法
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