WO2021200727A1 - Système d'alimentation en hydrogène - Google Patents

Système d'alimentation en hydrogène Download PDF

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Publication number
WO2021200727A1
WO2021200727A1 PCT/JP2021/013056 JP2021013056W WO2021200727A1 WO 2021200727 A1 WO2021200727 A1 WO 2021200727A1 JP 2021013056 W JP2021013056 W JP 2021013056W WO 2021200727 A1 WO2021200727 A1 WO 2021200727A1
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WO
WIPO (PCT)
Prior art keywords
hydrogen
unit
gas
toluene
liquid separation
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PCT/JP2021/013056
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English (en)
Japanese (ja)
Inventor
匡 清家
壱岐　英
征児 前田
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Ｅｎｅｏｓ株式会社
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Publication of WO2021200727A1 publication Critical patent/WO2021200727A1/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
    • 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
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/26—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts

Definitions

  • This disclosure relates to a hydrogen supply system that supplies hydrogen.
  • Patent Document 1 As a conventional hydrogen supply system, for example, the one listed in Patent Document 1 is known.
  • the hydrogen supply system of Patent Document 1 includes a tank for storing hydrides of aromatic hydrocarbons as a raw material, a dehydrogenation reaction unit for obtaining hydrogen by dehydrogenating the raw material supplied from the tank, and a dehydrogenation reaction.
  • a gas-liquid separation unit for gas-liquid separation of the hydrogen obtained in the unit and a hydrogen purification unit for purifying the gas-liquid separated hydrogen are provided.
  • the dehydrogenation product which is a liquid component such as toluene separated by the gas-liquid separation unit
  • the dehydrogenation product which is a liquid component such as toluene separated by the gas-liquid separation unit
  • the dehydrogenation product may be stored in a storage unit provided in the basement of the facility.
  • hydrogen may be dissolved in the dehydrogenation product separated by the gas-liquid separation section.
  • hydrogen gas may be generated in the storage unit. It is required to reduce the amount of hydrogen gas present in such a reservoir.
  • the present disclosure has been made to solve the above problems, and an object of the present disclosure is to provide a hydrogen supply system capable of reducing the amount of hydrogen gas present in the storage portion of the dehydrogenation product.
  • the hydrogen supply system is a hydrogen supply system that supplies hydrogen, and is a dehydrogenation reaction unit that obtains a hydrogen-containing gas by dehydrogenating a raw material containing a hydride.
  • a gas-liquid separation unit that separates the dehydrogenation product, which is a liquid component, from the hydrogen-containing gas obtained in the dehydrogenation reaction unit, and a storage unit that stores the dehydrogenation product separated by the gas-liquid separation unit.
  • a removal section for removing hydrogen dissolved in the dehydrogenation product is provided between the gas-liquid separation section and the storage section.
  • the gas-liquid separation unit separates the dehydrogenation product, which is a liquid component, from the hydrogen-containing gas obtained in the dehydrogenation reaction unit.
  • the storage unit stores the dehydrogenation product separated by the gas-liquid separation unit.
  • a removing section for removing hydrogen dissolved in the dehydrogenation product is provided between the gas-liquid separation section and the storage section. Therefore, even when hydrogen is dissolved in the dehydrogenation product separated by the gas-liquid separation unit, the removal unit can remove the hydrogen. Therefore, the dehydrogenation product in a state where the dissolved hydrogen is reduced is supplied to the storage portion. As described above, the amount of hydrogen gas present in the storage portion of the dehydrogenation product can be reduced.
  • the removing part may be composed of a degassing membrane separator.
  • the removing unit can efficiently remove hydrogen from the dehydrogenation product.
  • FIG. 1 is a block diagram showing a configuration of a hydrogen supply system according to an embodiment of the present disclosure.
  • the hydrogen supply system 100 uses an organic compound (liquid at room temperature) as a raw material.
  • the dehydrogenated product organic compound (liquid at room temperature)
  • the organic compound as a raw material include organic hydride.
  • a suitable example of the organic hydride is a hydride obtained by reacting hydrogen produced in large quantities in a refinery with an aromatic hydrocarbon.
  • the organic hydride is not limited to aromatic hydrogenated compounds, but also has a 2-propanol system (hydrogen and acetone are produced).
  • the organic hydride can be transported to the hydrogen supply system 100 as a liquid fuel by a tank lorry or the like like gasoline or the like.
  • methylcyclohexane hereinafter referred to as MCH
  • MCH methylcyclohexane
  • hydrides of aromatic hydrocarbons such as cyclohexane, dimethylcyclohexane, ethylcyclohexane, decalin, methyldecalin, dimethyldecalin, and ethyldecalin can be applied as the organic hydride.
  • the aromatic compound is a suitable example having a particularly high hydrogen content.
  • the hydrogen supply system 100 can supply hydrogen to a fuel cell vehicle (FCV) or a hydrogen engine vehicle. It can also be applied to the production of hydrogen from natural gas containing methane as a main component, LPG containing propane as a main component, or liquid hydrocarbon raw materials such as gasoline, naphtha, kerosene, and light oil.
  • FCV fuel cell vehicle
  • the hydrogen supply system 100 includes a liquid transfer pump 1, a heat exchange unit 2, a dehydrogenation reaction unit 3, a heating unit 4, a gas-liquid separation unit 6, a compression unit 7, and hydrogen.
  • the purification unit 8 is provided.
  • the liquid transfer pump 1, the heat exchange unit 2, and the dehydrogenation reaction unit 3 belong to the hydrogen production unit 10 that produces a hydrogen-containing gas.
  • the gas-liquid separation unit 6, the compression unit 7, and the hydrogen purification unit 8 belong to the hydrogen purity adjusting unit 11 that enhances the purity of hydrogen.
  • the hydrogen supply system 100 includes lines L1 to L12.
  • Lines L1 to L12 are channels through which MCH, toluene, hydrogen-containing gas, off-gas, high-purity hydrogen, or a heating medium passes.
  • the line L1 is a line for the liquid transfer pump 1 to pump up the MCH from the MCH tank (not shown), and connects the liquid transfer pump 1 and the MCH tank.
  • the line L2 connects the liquid transfer pump 1 and the dehydrogenation reaction unit 3.
  • the line L3 connects the dehydrogenation reaction unit 3 and the gas-liquid separation unit 6.
  • the line L4 connects the gas-liquid separation unit 6 and a toluene tank (not shown).
  • the line L5 connects the gas-liquid separation unit 6 and the compression unit 7.
  • the line L6 connects the compression unit 7 and the hydrogen purification unit 8.
  • the line L7 connects the hydrogen purification unit 8 and the off-gas supply destination.
  • the line L8 connects the hydrogen purification unit 8 and a purification gas supply device (not shown).
  • the lines L11 and L12 connect the heating unit 4 and the dehydrogenation reaction unit 3.
  • the lines L11 and L12 circulate a heat medium.
  • the liquid transfer pump 1 supplies the raw material MCH to the dehydrogenation reaction unit 3.
  • the MCH transported from the outside by a tank lorry or the like is stored in the MCH tank.
  • the MCH stored in the MCH tank is supplied to the dehydrogenation reaction unit 3 via the lines L1 and L2 by the liquid transfer pump 1.
  • the heat exchange unit 2 exchanges heat between the MCH flowing through the line L2 and the hydrogen-containing gas flowing through the line L3.
  • the hydrogen-containing gas emitted from the dehydrogenation reaction unit 3 has a higher temperature than the MCH. Therefore, in the heat exchange unit 2, the MCH is heated by the heat of the hydrogen-containing gas. As a result, the MCH is supplied to the dehydrogenation reaction unit 3 in a state where the temperature has risen.
  • the MCH is supplied to the dehydrogenation reaction unit 3 together with the off-gas supplied from the hydrogen purification unit 8 via the line L7.
  • the dehydrogenation reaction unit 3 is a device that obtains hydrogen by dehydrogenating MCH. That is, the dehydrogenation reaction unit 3 is a device that extracts hydrogen from the MCH by a dehydrogenation reaction using a dehydrogenation catalyst.
  • the dehydrogenation catalyst is not particularly limited, and is selected from, for example, a platinum catalyst, a palladium catalyst, and a nickel catalyst. These catalysts may be supported on carriers such as alumina, silica and titania.
  • the reaction of organic hydride is a reversible reaction, and the direction of the reaction changes depending on the reaction conditions (temperature, pressure) (subject to chemical equilibrium).
  • the dehydrogenation reaction is a reaction in which the number of molecules increases due to an endothermic reaction. Therefore, high temperature and low pressure conditions are advantageous. Since the dehydrogenation reaction is an endothermic reaction, the dehydrogenation reaction unit 3 is supplied with heat from the heating unit 4 via a heat medium circulating in the lines L11 and L12. The dehydrogenation reaction unit 3 has a mechanism capable of heat exchange between the MCH flowing in the dehydrogenation catalyst and the heat medium from the heating unit 4.
  • the hydrogen-containing gas taken out by the dehydrogenation reaction unit 3 is supplied to the gas-liquid separation unit 6 via the line L3.
  • the hydrogen-containing gas of line L3 is supplied to the gas-liquid separation unit 6 in a state of containing toluene, which is a liquid, as a mixture.
  • the heating unit 4 heats the heat medium and supplies the heat medium to the dehydrogenation reaction unit 3 via the line L11.
  • the heat medium after heating is returned to the heating unit 4 via the line L12.
  • the heat medium is not particularly limited, but oil or the like may be adopted.
  • the heating unit 4 any one may be used as long as it can heat the dehydrogenation reaction unit 3.
  • the heating unit 4 may directly heat the dehydrogenation reaction unit 3, or may heat the MCH supplied to the dehydrogenation reaction unit 3 by heating the line L2, for example.
  • the heating unit 4 may heat both the dehydrogenation reaction unit 3 and the MCH supplied to the dehydrogenation reaction unit 3.
  • a burner or an engine can be adopted as the heating unit 4.
  • the gas-liquid separation unit 6 is a tank that separates toluene from the hydrogen-containing gas.
  • the gas-liquid separation unit 6 separates hydrogen as a gas and toluene as a liquid by storing a hydrogen-containing gas containing toluene as a mixture. Further, the hydrogen-containing gas supplied to the gas-liquid separation unit 6 is cooled by the heat exchange unit 2.
  • the gas-liquid separation unit 6 may be cooled by a cooling medium from a cold heat source. In this case, the gas-liquid separation unit 6 has a mechanism capable of exchanging heat between the hydrogen-containing gas in the gas-liquid separation unit 6 and the cooling medium from the cold heat source.
  • the toluene separated by the gas-liquid separation unit 6 is supplied to the toluene underground tank 23 (storage unit) described later via the line L4.
  • the toluene underground tank 23 will be described later.
  • the hydrogen-containing gas separated by the gas-liquid separation unit 6 is supplied to the hydrogen purification unit 8 via the lines L5 and L6 by the pressure of the compression unit 7.
  • the hydrogen-containing gas is cooled, a part of the gas (toluene) is liquefied and can be separated from the non-liquefied gas (hydrogen) by the gas-liquid separation unit 6.
  • the hydrogen purification unit 8 removes the dehydrogenation product (toluene in the present embodiment) from the hydrogen-containing gas obtained in the dehydrogenation reaction unit 3 and separated in the gas-liquid separation unit 6. As a result, the hydrogen purification unit 8 purifies the hydrogen-containing gas to obtain high-purity hydrogen (purified gas). The obtained purified gas is supplied to line L8. The off-gas generated in the hydrogen purification unit 8 is supplied to the dehydrogenation reaction unit 3 via the line L7.
  • the hydrogen purification unit 8 differs depending on the hydrogen purification method adopted. Specifically, when membrane separation is used as the hydrogen purification method, the hydrogen purification unit 8 is a hydrogen separation device including a hydrogen separation membrane. When the PSA (Pressure swing attachment) method or the TSA (Temperature swing attachment) method is used as the hydrogen purification method, the hydrogen purification unit 8 is provided with a plurality of adsorption towers for adsorbing impurities. It is a device.
  • the hydrogen purification unit 8 uses membrane separation.
  • dehydrogenation products are removed by permeating a film heated to a predetermined temperature with a hydrogen-containing gas pressurized to a predetermined pressure by a compression unit (not shown) to remove high-purity hydrogen gas (not shown).
  • Purified gas can be obtained.
  • the pressure of the gas permeating the membrane is lower than the pressure before permeating the membrane.
  • the pressure of the gas that did not permeate the membrane is substantially the same as the predetermined pressure before permeating the membrane. At this time, the gas that did not permeate the membrane corresponds to the off-gas of the hydrogen purification unit 8.
  • the type of membrane applied to the hydrogen purification unit 8 is not particularly limited, and is a porous membrane (separated by molecular flow, separated by surface diffusion flow, separated by capillary condensing action, separated by molecular sieving action). , Etc.) and non-porous membranes can be applied.
  • the membrane applied to the hydrogen purification unit 8 include a metal membrane (PbAg-based, PdCu-based, Nb-based, etc.), a zeolite membrane, an inorganic membrane (silica membrane, carbon membrane, etc.), and a polymer membrane (polyimide membrane, etc.). Can be adopted.
  • the adsorbent used in the PSA method has the property of adsorbing toluene contained in the hydrogen-containing gas under high pressure and desorbing the adsorbed toluene under low pressure.
  • the PSA method utilizes such properties of the adsorbent. That is, by increasing the pressure inside the adsorption tower, toluene contained in the hydrogen-containing gas is adsorbed on the adsorbent and removed to obtain a high-purity hydrogen gas (purified gas).
  • the toluene adsorbed on the adsorbent was desorbed by lowering the pressure inside the adsorption tower, and a part of the purified gas removed at the same time was backflowed to desorb the toluene.
  • the adsorption function of the adsorbent is regenerated.
  • the hydrogen-containing gas containing at least hydrogen and toluene discharged by removing toluene from the adsorption tower corresponds to the off-gas from the hydrogen purification unit 8.
  • the adsorbent used in the TSA method has the property of adsorbing toluene contained in the hydrogen-containing gas at room temperature and desorbing the adsorbed toluene at high temperature.
  • the TSA method utilizes such properties of the adsorbent. That is, by keeping the inside of the adsorption tower at room temperature, toluene contained in the hydrogen-containing gas is adsorbed on the adsorbent and removed to obtain a high-purity hydrogen gas (purified gas).
  • the toluene adsorbed on the adsorbent is desorbed by raising the temperature inside the adsorption tower, and a part of the removed high-purity hydrogen is backflowed to desorb the toluene.
  • the adsorption function of the adsorbent is regenerated.
  • the hydrogen-containing gas containing at least hydrogen and toluene discharged by removing toluene from the adsorption tower corresponds to the off-gas from the hydrogen purification unit 8.
  • the hydrogen supply system 100 further includes a toluene underground tank 23 (storage unit).
  • the gas-liquid separation unit 6 separated toluene, which is a liquid component, from the hydrogen-containing gas obtained in the dehydrogenation reaction unit 3.
  • the toluene underground tank 23 stores the toluene separated by the gas-liquid separation unit 6.
  • the toluene underground tank 23 is provided underground in the facility of the hydrogen supply system 100.
  • an underground tank is illustrated as a storage unit for storing toluene, but the position of the storage unit is not particularly limited and may be arranged on the ground.
  • the toluene in the gas-liquid separation unit 6 is transferred to the toluene underground tank 23 by its own weight. If there is a reservoir on the ground, a pump is installed on line L4 to transfer the toluene from the gas-liquid separation section 6 to the reservoir on the ground.
  • a removal unit 21 for removing hydrogen dissolved in toluene is provided between the gas-liquid separation unit 6 and the toluene underground tank 23, a removal unit 21 for removing hydrogen dissolved in toluene is provided.
  • the removing portion 21 is provided on the line L4. Therefore, the gas-liquid separation unit 6 supplies toluene to the removal unit 21 via the line L4a.
  • the removing unit 21 removes hydrogen from the toluene from the gas-liquid separation unit 6 and supplies the dissolved hydrogen to the toluene underground tank 23 via the line L4b in a state of reducing the dissolved hydrogen.
  • a valve 22 is provided on the line L4b. The valve 22 can adjust the amount of toluene supplied from the gas-liquid separation unit 6 to the toluene underground tank 23, and can switch between supply and stop.
  • the removing unit 21 is composed of a device capable of removing hydrogen from toluene.
  • the removing unit 21 may be configured by a degassing membrane separator.
  • a degassing membrane separator is a device that removes hydrogen from toluene using a degassing membrane.
  • the degassing membrane separator separates the toluene and hydrogen by passing toluene through the degassing membrane.
  • the removing unit 21 discharges the removed hydrogen from the removing unit 21 to the outside. Then, the removing unit 21 supplies the toluene from which hydrogen has been removed to the toluene underground tank 23.
  • the equipment constituting the removal unit 21 is not limited to the degassing membrane separator.
  • a device such as a centrifugal separation method or an ultrasonic separation method may be adopted as the removing unit 21.
  • the toluene separated by the gas-liquid separation unit 6 may be stored in a toluene underground tank 23 provided underground of the facility or the like.
  • hydrogen may be dissolved in the toluene separated by the gas-liquid separation unit 6.
  • hydrogen gas may be generated in the toluene underground tank 23. It is required to reduce the amount of hydrogen gas existing in such a toluene underground tank 23.
  • the hydrogen supply system 100 is a hydrogen supply system 100 that supplies hydrogen, and is a dehydrogenation reaction unit 3 that obtains a hydrogen-containing gas by dehydrogenating a raw material containing a hydride.
  • the gas-liquid separation unit 6 that separates the dehydrogenation product, which is a liquid component, from the hydrogen-containing gas obtained by the dehydrogenation reaction unit 3, and the dehydrogenation product separated by the gas-liquid separation unit 6 are stored.
  • a toluene underground tank 23 is provided, and a removing unit 21 for removing hydrogen dissolved in the dehydrogenation product is provided between the gas-liquid separation unit 6 and the toluene underground tank 23.
  • the gas-liquid separation unit 6 separates the dehydrogenation product, which is a liquid component, from the hydrogen-containing gas obtained by the dehydrogenation reaction unit 3. Further, the toluene underground tank 23 stores the dehydrogenation product separated by the gas-liquid separation unit 6.
  • a removal unit 21 for removing hydrogen dissolved in the dehydrogenation product is provided between the gas-liquid separation unit 6 and the toluene underground tank 23. Therefore, even when hydrogen is dissolved in the dehydrogenation product separated by the gas-liquid separation unit 6, the removal unit 21 can remove the hydrogen. Therefore, the dehydrogenation product in a state where the dissolved hydrogen is reduced is supplied to the toluene underground tank 23. As described above, the amount of hydrogen gas existing in the toluene underground tank 23 can be reduced.
  • the removing unit 21 may be configured by a degassing membrane separator. As a result, the removing unit 21 can efficiently remove hydrogen from the dehydrogenation product.
  • the hydrogen station for FVC is illustrated as the hydrogen supply system, but for example, it may be a hydrogen supply system for a distributed power source such as a household power source or an emergency power source.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

L'invention concerne un système d'alimentation en hydrogène pour l'alimentation en hydrogène, ledit système comprenant une unité de réaction de déshydrogénation pour soumettre un matériau de départ contenant un hydrure à une réaction de déshydrogénation afin d'obtenir un gaz contenant de l'hydrogène, une unité de séparation gaz-liquide pour séparer un produit de déshydrogénation qui est un composant liquide du gaz contenant de l'hydrogène obtenu dans l'unité de réaction de déshydrogénation, et une unité de stockage pour stocker le produit de déshydrogénation séparé dans l'unité de séparation gaz-liquide, une unité d'élimination pour éliminer l'hydrogène dissous dans le produit de déshydrogénation étant disposée entre l'unité de séparation gaz-liquide et l'unité de stockage.
PCT/JP2021/013056 2020-03-30 2021-03-26 Système d'alimentation en hydrogène WO2021200727A1 (fr)

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JP2020-060417 2020-03-30
JP2020060417A JP2021155312A (ja) 2020-03-30 2020-03-30 水素供給システム

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WO2021200727A1 true WO2021200727A1 (fr) 2021-10-07

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Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014231461A (ja) * 2013-05-29 2014-12-11 Ｊｘ日鉱日石エネルギー株式会社 水素の製造方法及び水素の製造システム

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014231461A (ja) * 2013-05-29 2014-12-11 Ｊｘ日鉱日石エネルギー株式会社 水素の製造方法及び水素の製造システム

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