WO2021186663A1 - Dispositif de production de monoxyde de carbone et système de production de monoxyde de carbone - Google Patents

Dispositif de production de monoxyde de carbone et système de production de monoxyde de carbone Download PDF

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Publication number
WO2021186663A1
WO2021186663A1 PCT/JP2020/012234 JP2020012234W WO2021186663A1 WO 2021186663 A1 WO2021186663 A1 WO 2021186663A1 JP 2020012234 W JP2020012234 W JP 2020012234W WO 2021186663 A1 WO2021186663 A1 WO 2021186663A1
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Prior art keywords
carbon monoxide
water
monoxide production
reverse shift
flow path
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PCT/JP2020/012234
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English (en)
Japanese (ja)
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晃平 吉川
篤 宇根本
杉政　昌俊
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株式会社日立製作所
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Priority to PCT/JP2020/012234 priority Critical patent/WO2021186663A1/fr
Publication of WO2021186663A1 publication Critical patent/WO2021186663A1/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
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/40—Carbon monoxide

Definitions

  • the present invention relates to a carbon monoxide production apparatus and a carbon monoxide production system.
  • Patent Document 1 describes at least one kind of alkaline earth selected from the group consisting of Ca, Sr and Ba, which is a catalyst for a reverse shift reaction used to generate carbon monoxide and water vapor from carbon dioxide and hydrogen. It contains at least one alkaline earth metal selected from the group consisting of metal carbonates, Ca, Sr and Ba, and at least one component selected from the group consisting of Ti, Al, Zr, Fe, W and Mo.
  • a catalyst for a reverse shift reaction which is characterized by containing a composite oxide, is described.
  • An object to be solved by the present invention is to provide a carbon monoxide production apparatus and a carbon monoxide production system that can sustain the production of carbon monoxide.
  • the carbon monoxide production apparatus of the present invention includes a reverse shift catalyst that promotes a reverse shift reaction that produces carbon monoxide and water from a raw material gas containing carbon dioxide and hydrogen, an inlet for the raw material gas, and the produced carbon monoxide.
  • the reverse shift catalyst is arranged while being partitioned by a first partition wall that is formed between a discharge port that discharges a product gas containing at least carbon and contains at least a part of a water permeation wall that selectively permeates water. It is provided with a gas flow path.
  • the present invention is not limited to the following contents and the illustrated contents, and can be arbitrarily modified and carried out within a range that does not significantly impair the effects of the present invention.
  • the present invention can be implemented by combining different embodiments.
  • the same members will be designated by the same reference numerals in different embodiments, and redundant description will be omitted.
  • the same name is used for those having the same function, and duplicate explanations are omitted.
  • hatching may be omitted for the sake of simplification.
  • FIG. 1 is a perspective view of the carbon monoxide production apparatus 100 of the first embodiment.
  • the carbon monoxide production apparatus 100 produces carbon monoxide and water from a raw material gas containing carbon dioxide and hydrogen by the reverse shift reaction represented by the above formula (1).
  • the reverse shift reaction is an endothermic reaction.
  • the first source gas further contains hydrogen.
  • Hydrogen can be produced, for example, by electrolyzing water using renewable energy.
  • hydrogen for example, hydrogen generated by reforming can be used to carry out a Fischer-Tropsch reaction, and surplus hydrogen at that time can also be used.
  • the produced carbon monoxide can be used, for example, as a Fischer-Tropsch reaction, methanol production, iron making, gas fuel and the like.
  • the carbon monoxide production apparatus 100 includes a plurality of (two in the illustrated example) unit production apparatus 100a and 100b having the same performance and structure in the illustrated example. However, the carbon monoxide production apparatus 100 may include only a single unit production apparatus 100a. In the following example, the carbon monoxide production apparatus 100 will be described by taking the unit production apparatus 100a as an example.
  • the carbon monoxide production apparatus 100 includes a reverse shift catalyst 20, a gas flow path 15, and a discharge space 51.
  • the reverse shift catalyst 20 promotes the reverse shift reaction.
  • the reverse shift catalyst 20 is supported on the surface of the partition member 41 facing the gas flow path 15, which will be described in detail later.
  • the reverse shift catalyst 20 exhibits catalytic activity at, for example, 550 ° C or lower (preferably 500 ° C or lower).
  • 550 ° C or lower preferably 500 ° C or lower.
  • the reverse shift catalyst 20 preferably contains at least one element of Cu, Co, or Mn as an active ingredient. By having these elements, carbon monoxide can be selectively produced, and the reverse shift reaction can proceed efficiently.
  • the precursor of the active ingredient include nitrates, acetates, chlorides, hydroxides and the like of each element.
  • an impregnation method, a coprecipitation method, a kneading method, a mechanical alloying method, a vapor deposition method and the like can be considered.
  • the form of the active ingredient is preferably an oxide or a metal alone.
  • Examples of the method for obtaining the oxide of the active ingredient include firing in a gas atmosphere containing oxygen such as in the atmosphere.
  • Examples of the method for obtaining the active component of a simple substance include a method in which firing is performed in the atmosphere to form an oxide, and then a reduction treatment is performed in a gas atmosphere containing hydrogen.
  • the active ingredient may be filled in the catalytic reaction vessel in the oxide state, and hydrogen gas may be circulated and reduced before the reverse shift reaction to be changed to the metallic state. ..
  • the reverse shift catalyst 20 preferably further contains an oxide containing at least one element selected from Si, Al, Zr, and Ce as a carrier component in addition to the active ingredient.
  • oxides containing Ce in particular promote redox. Therefore, from the viewpoint of promoting the oxidation and reduction of the active ingredient and improving the catalytic performance, the carrier component preferably contains an oxide containing Ce.
  • the carrier component is an oxide containing Ce and an oxide containing rare earth elements such as Zr, Y, La, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Tb and Lu. Is more preferable.
  • the combination of the oxide containing Ce and the oxide containing a rare earth element can further promote the redox reaction.
  • the active ingredient is preferably 0.1% by mass or more, more preferably 1% by mass or more, and the upper limit thereof is preferably 30% by mass or less, based on the carrier component. More preferably, it is 10% by mass or less.
  • the reaction temperature is, for example, 550 ° C. or lower, preferably 500 ° C. or lower, and the lower limit thereof is, for example, 200 ° C. or higher, preferably 300 ° C. or higher.
  • the reaction pressure is, for example, 800 hPa or more, preferably 900 hPa or more, and the upper limit thereof is, for example, 1200 hPa or less, preferably 1100 hPa or less.
  • the reverse shift reaction can proceed by, for example, heating the raw material gas flowing through the gas flow path 15 from the outside with a heating device (not shown) such as a burner so as to reach the above reaction temperature.
  • a heating device such as a burner
  • the reaction conditions such as reaction temperature and reaction pressure differ depending on the type of reverse shift catalyst. Therefore, the reaction conditions may be appropriately determined depending on the type of reverse shift catalyst used.
  • the reverse shift catalyst 20 was prepared, and the catalytic activity of the reverse shift catalyst 20 was evaluated.
  • the specific surface area 100 m 2 / g or more powdered CeO 2 10 g, and the nitrate Cu aqueous solution was impregnated and dried so as to be 10% by mass with respect to CeO 2 by weight of metal Cu terms.
  • a reduction treatment was carried out at 500 ° C. for 1 hour in a hydrogen atmosphere.
  • the production rates were 5%, 25%, and 50%, respectively, and it was found that carbon monoxide was produced from carbon dioxide by using the reverse shift catalyst 20.
  • the gas flow path 15 is formed between the introduction port 11 of the raw material gas containing carbon dioxide and hydrogen and the discharge port 12 for discharging the produced gas containing at least the produced carbon monoxide.
  • the gas flow path 15 is formed by being partitioned from the outside by a first partition wall 40 including at least a part of a water permeation wall 30 that selectively permeates water.
  • the water permeation wall 30 is flat or flat.
  • the thickness of the water permeable wall 30 is, for example, 1 cm or more and 10 cm or less.
  • the reverse shift catalyst 20 is arranged in the gas flow path 15. Therefore, when the raw material gas flows through the gas flow path 15, carbon monoxide and water are generated in the gas flow path 15. Therefore, in order to sustain the production of carbon monoxide, the produced water selectively permeates through the water permeation wall 30 and is removed from the gas flow path 15. As a result, the chemical equilibrium in the reaction formula (1) can be easily moved to the right, and the production of carbon monoxide is sustained. The water does not have to be completely removed, and only a part of the generated water may permeate through the water permeation wall 30.
  • the water permeation wall 30 is preferably made of a material that is resistant to the reaction temperature of the reverse shift reaction. Specifically, the water permeation wall 30 is preferably at least one of graphene oxide, a zeolite (Si—Al composite oxide) film, a porous silica film, a porous alumina film, and the like. In the water permeation wall 30 made of these materials, when water (for example, water vapor) existing in the gas flow path 15 enters between the layers or the pores of the water permeation wall 30, water interacts with each other to cause the layers or the inside of the pores. Is filled with water.
  • water for example, water vapor
  • the water in the gas flow path 15 starts to be adsorbed on the water permeation wall 30 due to the interaction between the water in the gas flow path 15 and the water permeation wall 30.
  • the partial pressure of water vapor becomes lower than the partial pressure of water vapor in the gas flow path 15 on the side opposite to the gas flow path 15 of the water permeation wall 30, from the side opposite to the gas flow path 15 of the water permeation wall 30. Water is released. In this way, the water in the gas flow path 15 selectively permeates the water permeation wall 30.
  • the gas flow path 15 is formed as a space surrounded by a water permeation wall 30 and a partition member 41 arranged so as to form a convex space on the surface of the water permeation wall 30.
  • the partition member 41 is a part of the first partition wall 40.
  • the partition member 41 is formed in a mountain shape that narrows in a direction away from the water permeation wall 30.
  • the reverse shift catalyst 20 is supported on the surface of the partition member 41 facing the gas flow path 15.
  • a dispersion liquid in which the particulate reverse shift catalyst 20 is dispersed in a solvent is prepared, and the surface of the partition member 41 facing the gas flow path 15 is coated and dried. ,It can be carried out.
  • the discharge space 51 is partitioned by the second partition wall 50 on the opposite side of the water permeation wall 30 from the gas flow path 15, and the water that has permeated through the water permeation wall 30 is discharged.
  • the discharge space 51 it is possible to easily control the partial pressure of water vapor on the side of the water permeation wall 30 opposite to the gas flow path 15, and it is possible to easily permeate the water of the water permeation wall 30 driven by the difference in partial pressure of water vapor. ..
  • the second partition wall 50 is formed in a mountain shape that narrows in a direction away from the water permeation wall 30.
  • a low partial pressure gas having a lower partial pressure of water vapor than the partial pressure of water vapor of the gas flowing through the gas flow path 15 flows in the discharge space 51.
  • the low partial pressure gas is, for example, air, dry air, nitrogen, etc., and is air in the illustrated example. Therefore, in the illustrated example, air is introduced into the discharge space 51 from the introduction port 13. Then, the air flowing through the discharge space 51 receives the water (usually water vapor) that has passed through the water permeation wall 30, and is discharged as water-containing air from the discharge space 51 through the discharge port 14.
  • the discharge space 51 extends in the direction intersecting the gas flow path 15. Therefore, the flow direction of the low partial pressure gas intersects with the flow direction of the raw material gas and the produced gas. In the illustrated example, they are orthogonal. By making the extending direction of the discharge space 51 intersect with the gas flow path 15, the permeation of water through the water permeation wall 30 can be promoted, and the production of carbon monoxide can be maintained.
  • a support plate 31 is interposed between the plurality of unit manufacturing devices 100a and the unit manufacturing device 100b.
  • the reverse shift reaction proceeds in each of the unit manufacturing apparatus 100a and 100b.
  • the water generated during the reverse shift reaction can be removed from the gas flow path 15, and the production of carbon monoxide can be sustained for a long period of time. That is, when water is generated by the contact between the raw material gas and the reverse shift catalyst 20, the amount of water (for example, the amount of water vapor) in the gas flow path 15 increases. Above all, for example, the water generated near the introduction port 11 comes into contact with the reverse shift catalyst 20 from the introduction port 11 to the discharge port 12 in the process of flowing through the gas flow path 15. As a result, the water flowing through the gas flow path 15 is on the right side of the chemical equilibrium in the reaction formula (1) in the reverse shift catalyst 20 arranged from the introduction port 11 to the discharge port 12 in the process of flowing through the gas flow path 15. Make it difficult to move to.
  • the difference between the partial pressure of water vapor in the gas flow path 15 and the partial pressure of water vapor in the discharge space 51 becomes large due to the generation of water in the gas flow path 15.
  • the water in the gas flow path 15 permeates through the water permeation wall 30 by using the water vapor partial pressure difference as a driving force.
  • the chemical equilibrium tends to move to the right, and carbon monoxide can be continuously produced.
  • FIG. 2 is a perspective view of the carbon monoxide production apparatus 110 of the second embodiment.
  • the reverse shift catalyst 20 is also supported on the water permeation wall 30. That is, in the carbon monoxide production apparatus 110, the reverse shift catalyst 20 is supported on the surface of the water permeation wall 30 facing the gas flow path 15.
  • the reverse shift catalyst 20 is preferably supported on the partition member 41, but may not be supported on the partition member 41.
  • the water generated on the surface of the reverse shift catalyst 20 can easily permeate through the water permeation wall 30. That is, the water generated on the surface of the reverse shift catalyst 20 reaches the water permeation wall 30 with almost no intervention of the gas phase. Therefore, the diffusion of water (water vapor) caused through the gas phase can be suppressed, and the generated water can be smoothly permeated through the water permeation wall 30. As a result, an excessive increase in the amount of water in the gas flow path 15 can be suppressed, and the production of carbon monoxide can be sustained for a long period of time.
  • FIG. 3 is a cross-sectional view of the carbon monoxide production apparatus 120 of the third embodiment.
  • the carbon monoxide production apparatus 120 has an inner cylinder 42 formed of a tubular first partition wall 40 and an outer cylinder 52 which is a tubular second partition wall 50 arranged so as to surround the inner cylinder 42. It is composed of double pipes.
  • the first partition wall 40 is formed in a cylindrical shape by the water permeation wall 30. By configuring the first partition wall 40 in this way, water can permeate through the entire tubular first partition wall 40, and water can be quickly removed from the gas flow path 15.
  • the reverse shift catalyst 20 is formed in a granular shape, and the granular reverse shift catalyst 20 is housed in a gas flow path 15 formed by a cylindrical first partition wall 40. By doing so, the reverse shift catalyst 20 can be arranged in the gas flow path 15 by packing the granular reverse shift catalyst 20 in the gas flow path 15, and the arrangement of the reverse shift catalyst 20 can be facilitated.
  • the introduction port 11 and the discharge port 12 are closed by a mesh-shaped plate material (not shown). As a result, it is possible to achieve both the flow of the raw material gas and the produced gas and the suppression of the reverse shift catalyst 20 from falling off.
  • the reverse shift catalyst 20 is preferably packed tightly so that the pressure loss does not become excessively large.
  • the reverse shift catalyst 20 is densely packed in the gas flow path 15 so as to come into contact with the water permeation wall 30.
  • FIG. 4 is a cross-sectional view of the carbon monoxide production apparatus 130 of the fourth embodiment.
  • the water permeation wall 30 becomes thinner toward the downstream side due to the gas flow flowing through the gas flow path 15.
  • FIG. 5 is a system diagram of the carbon monoxide production system 1000 of the fifth embodiment.
  • the carbon monoxide production system 1000 includes the carbon monoxide production apparatus 100 described above in the illustrated example. However, the carbon monoxide production system 1000 may include carbon monoxide production devices 110, 120, 130 in place of the carbon monoxide production device 100, or together with the carbon monoxide production device 100. This point also applies to the carbon monoxide production systems 1100, 1200, and 1300 described later.
  • the carbon monoxide production system 1000 includes a compression device 200.
  • the compression device 200 compresses the raw material gas supplied to the carbon monoxide production device 100.
  • the compression device 200 By providing the compression device 200, it is possible to increase the density of the raw material gas, increase the amount of substances of carbon monoxide and hydrogen per unit flow rate in contact with the reverse shift catalyst 20, and increase the amount of carbon monoxide produced.
  • the partial pressure of water vapor in the gas flow path 15 (FIG. 1) rises rapidly. Therefore, the water vapor partial pressure difference from the discharge space 51 (FIG. 1) on the opposite side of the gas flow path 15 via the water permeation wall 30 rapidly increases, and the water permeation wall 30 driven by the water vapor partial pressure difference Water can be permeated quickly. Further, the actual flow velocity of the raw material gas can be slowed down by the compression device 200, and the pressure loss in the carbon monoxide production device 100 can be reduced.
  • the degree of pressurization of the raw material gas by the compression device 200 is not particularly limited, but the pressure of the raw material gas can be, for example, higher than the atmospheric pressure, for example, 10 MPa or less.
  • the carbon monoxide production system 1000 includes a distribution device 300.
  • the distribution device 300 flows a low partial pressure gas having a water vapor partial pressure lower than the water vapor partial pressure of the gas flowing through the gas flow path 15 through the discharge space 51.
  • the difference in water vapor partial pressure between the water vapor partial pressure of the gas flowing through the gas flow path 15 and the discharge space 51 on the opposite side of the gas flow path 15 via the water permeation wall 30 can be increased.
  • the distribution device 300 is, for example, a blower, a blower fan, or the like, and is a blower in the illustrated example.
  • the low partial pressure gas is, for example, air, dry air, nitrogen, etc. as described above, and is air in the illustrated example.
  • the flow velocity of the low partial pressure gas is not particularly limited.
  • the water vapor partial pressure of the low partial pressure gas can be set to, for example, a water vapor partial pressure lower than the water vapor partial pressure in the produced gas.
  • FIG. 6 is a system diagram of the carbon monoxide production system 1100 of the sixth embodiment.
  • the carbon monoxide production system 1100 includes a decompression device 400.
  • the decompression device 400 decompresses the discharge space 51 (FIG. 1) of the carbon monoxide production apparatus 100.
  • the discharge space 51 can be decompressed, and the low partial pressure gas such as air can be taken into the discharge space 51 by the decompression.
  • the difference in water vapor partial pressure between the gas flow path 15 and the discharge space 51 can be increased, and the permeation of water through the water permeation wall 30 using the water vapor partial pressure difference as a driving force can be promoted.
  • FIG. 7 is a system diagram of the carbon monoxide production system 1200 of the seventh embodiment.
  • the carbon monoxide production system 1200 includes a decompression device 400 similar to the carbon monoxide production system 1100 (FIG. 6) described above. However, unlike the carbon monoxide production system 1100 (FIG. 6), the carbon monoxide production system 1200 includes a valve 101 that makes the discharge space 51 airtight. Therefore, in the carbon monoxide production system 1200, the discharge space 51 becomes airtight by closing the valve 101.
  • the pressure in the discharge space 51 decreases.
  • the degree of depressurization is not particularly limited, but can be, for example, 1 kPa or more and 10 kPa or less. Water vapor is extracted by the reduced pressure, and the partial pressure of water vapor in the discharge space 51 decreases. This makes it possible to promote the permeation of water through the water permeation wall 30 (FIG. 1).
  • FIG. 8 is a system diagram of the carbon monoxide production system 1300 according to the eighth embodiment.
  • the carbon monoxide production system 1300 includes a heat utilization facility 500 in addition to the configuration of the carbon monoxide production system 1200 (FIG. 7) described above.
  • the heat utilization facility 500 is a facility that utilizes the heat of the water that has passed through the water permeation wall 30 (FIG. 1).
  • the water that has permeated through the water permeation wall 30 of the carbon monoxide production apparatus 100 is usually water vapor due to the reaction temperature of the reverse shift reaction. Then, the steam discharged from the carbon monoxide production apparatus 1 is adiabatically compressed in the decompression apparatus 400 and changed to high temperature steam. Therefore, in the carbon monoxide production system 1300, the heat of the high-temperature steam can be used in the heat utilization facility 500. Thereby, the thermal efficiency in the carbon monoxide production system 1300 can be improved.
  • the heat utilization facility 500 is, for example, a reboiler (not shown) that can be used when recovering carbon dioxide contained in a raw material gas from, for example, combustion exhaust gas by a chemical absorption method.
  • the heat utilization equipment 500 may be, for example, a heat exchanger (not shown) installed in front of the compression device 200 in the carbon monoxide production system 1300. By providing such a heat exchanger, the raw material gas can be preheated by the heat of water vapor.

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Abstract

L'invention concerne un dispositif de production de monoxyde de carbone qui peut maintenir la production de monoxyde de carbone. L'invention concerne un dispositif de production de monoxyde de carbone (100) qui comprend un catalyseur de conversion inverse (20) et des canaux de gaz (15) qui reçoivent le catalyseur de conversion inverse. Le catalyseur de conversion inverse accélère une réaction de conversion inverse qui génère du monoxyde de carbone et de l'eau à partir d'un gaz de matière première qui comprend du dioxyde de carbone et de l'hydrogène. Les canaux de gaz : sont formés entre des ouvertures d'introduction (11) pour le gaz de matière première et des ouvertures de décharge (12) qui déchargent un gaz produit qui comprend au moins le monoxyde de carbone qui a été généré ; et sont délimités par des premières parois de démarcation (40). Au moins une partie des premières parois de démarcation sont des parois perméables à l'eau (30) qui sont sélectivement perméables à l'eau.
PCT/JP2020/012234 2020-03-19 2020-03-19 Dispositif de production de monoxyde de carbone et système de production de monoxyde de carbone WO2021186663A1 (fr)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114486470A (zh) * 2021-12-31 2022-05-13 南京理工大学 一种多路气体产烟布撒一体化装置

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH0769615A (ja) * 1993-08-31 1995-03-14 Tokyo Gas Co Ltd 炭酸ガスから一酸化炭素を製造する方法
JP2000233918A (ja) * 1999-02-16 2000-08-29 Mitsui Eng & Shipbuild Co Ltd Ｃｏの製造方法
JP2006176400A (ja) * 2004-12-21 2006-07-06 Boc Group Inc:The 改良された一酸化炭素製造法
JP2010525118A (ja) * 2007-04-27 2010-07-22 サウディ ベーシック インダストリーズ コーポレイション 二酸化炭素の合成ガスへの接触水素化
JP2012232274A (ja) * 2011-05-09 2012-11-29 Hitachi Zosen Corp Ｃｏ２のゼオライト膜分離回収システム

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH0769615A (ja) * 1993-08-31 1995-03-14 Tokyo Gas Co Ltd 炭酸ガスから一酸化炭素を製造する方法
JP2000233918A (ja) * 1999-02-16 2000-08-29 Mitsui Eng & Shipbuild Co Ltd Ｃｏの製造方法
JP2006176400A (ja) * 2004-12-21 2006-07-06 Boc Group Inc:The 改良された一酸化炭素製造法
JP2010525118A (ja) * 2007-04-27 2010-07-22 サウディ ベーシック インダストリーズ コーポレイション 二酸化炭素の合成ガスへの接触水素化
JP2012232274A (ja) * 2011-05-09 2012-11-29 Hitachi Zosen Corp Ｃｏ２のゼオライト膜分離回収システム

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114486470A (zh) * 2021-12-31 2022-05-13 南京理工大学 一种多路气体产烟布撒一体化装置

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