WO2022138162A1 - 安定同位体濃縮装置および安定同位体濃縮方法 - Google Patents
安定同位体濃縮装置および安定同位体濃縮方法 Download PDFInfo
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- WO2022138162A1 WO2022138162A1 PCT/JP2021/045097 JP2021045097W WO2022138162A1 WO 2022138162 A1 WO2022138162 A1 WO 2022138162A1 JP 2021045097 W JP2021045097 W JP 2021045097W WO 2022138162 A1 WO2022138162 A1 WO 2022138162A1
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Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/02—Separation by phase transition
- B01D59/04—Separation by phase transition by distillation
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B21/00—Nitrogen; Compounds thereof
- C01B21/20—Nitrogen oxides; Oxyacids of nitrogen; Salts thereof
- C01B21/24—Nitric oxide (NO)
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07B—GENERAL METHODS OF ORGANIC CHEMISTRY; APPARATUS THEREFOR
- C07B59/00—Introduction of isotopes of elements into organic compounds ; Labelled organic compounds per se
- C07B59/001—Acyclic or carbocyclic compounds
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C17/00—Preparation of halogenated hydrocarbons
- C07C17/38—Separation; Purification; Stabilisation; Use of additives
- C07C17/383—Separation; Purification; Stabilisation; Use of additives by distillation
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2006/00—Physical properties of inorganic compounds
- C01P2006/88—Isotope composition differing from the natural occurrence
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07B—GENERAL METHODS OF ORGANIC CHEMISTRY; APPARATUS THEREFOR
- C07B2200/00—Indexing scheme relating to specific properties of organic compounds
- C07B2200/05—Isotopically modified compounds, e.g. labelled
Definitions
- the present invention relates to a stable isotope enricher and a stable isotope enrichment method for concentrating stable isotopes containing stable isotope atoms.
- Stable isotopes are used in the fields of organic chemistry and biochemistry to obtain information on various reactions, structures and functions of organic and biological substances. Specifically, stable isotopes are used for NMR analysis as tracers in the fields of natural science and medical care, for drug discovery and organic synthesis using the kinetic isotope effect in which the reaction rate changes due to isotope substitution, and further. It is used in infrared / Raman spectroscopy, etc., which utilizes the difference in spectral properties.
- the distillation separation method is suitable for mass production of isotopes of light elements. Therefore, for example, as an industrial stable isotope separation method for oxygen, a method such as distillation separation of water or distillation separation of oxygen is adopted.
- Patent Document 1 discloses a method and an apparatus for producing heavy oxygen water in which oxygen distillation and water distillation are combined.
- oxygen gas and water vapor having a reduced concentration of the target isotope weight component oxygen molecule containing 17 O or 18 O
- oxygen gas is released into the atmosphere and water vapor is treated as wastewater.
- Patent Document 2 discloses a carbon monoxide stable isotope concentrator and a concentrating method for concentrating 13 CO. Even when the carbon stable isotope is concentrated using the technique disclosed in Patent Document 2, the concentration of 13 CO from the top of the first distillation column is higher than the natural abundance ratio, as in the case of Patent Document 1 described above.
- a large amount of reduced CO gas is released to the outside of the system (hereinafter, the exhaust gas or effluent whose target stable isotope concentration is lower than the natural abundance ratio, which is discharged from the stable isotope concentrator, is referred to as " It may be referred to as “isotope-depleted gas” or “isotope-depleted liquid”).
- the industrial method of abatement treatment include a method using a flare stack and a method using an oxidation treatment by a catalytic reaction.
- Patent Document 3 discloses a carbon monoxide removing unit and a removing method for converting carbon monoxide into carbon dioxide by a catalytic reaction as a method of oxidation treatment by a catalytic reaction. Both methods described above convert carbon monoxide into carbon dioxide by oxidizing it. As a result, a large amount of carbon dioxide is released into the atmosphere, which is accompanied by an environmental load.
- nitric oxide distillation can be mentioned as a method for concentrating a stable isotope of nitrogen.
- This method is a highly convenient method for obtaining an isotope of oxygen at the same time as an isotope of nitrogen.
- Non-Patent Document 1 it is known that there was a plant in the United States that co-produces a heavy component of oxygen having a high concentration of 95% or more and nitrogen.
- nitric oxide is considered to be a cause of acid rain and photochemical smog as a nitrogen oxide, and is toxic. Therefore, like carbon monoxide, it cannot be directly released into the atmosphere, so a detoxification treatment by an ammonia catalytic reduction method or the like is required.
- the present invention has been made in view of the above problems, and it is possible to reduce the amount of emissions of substances having toxicity and flammability, or substances that cause an environmental load in the atmosphere, and it is possible to reduce the amount of raw materials used. It is an object of the present invention to provide a stable isotope enrichment apparatus and a stable isotope enrichment method.
- the inventors of the present invention have made extensive studies to solve the above problems. As a result, when concentrating stable isotopes containing stable isotope atoms, isotope-damaged gas or isotope-damaged liquid in which the concentration of the target stable isotope is lower than the natural abundance is naturally produced by an isotope exchange reaction. It was found that these can be reused as raw materials by regenerating them to a concentration close to the abundance ratio. We have found that this makes it possible to reduce the amount of raw materials used while reducing the amount of substances that cause an environmental load in the atmosphere, and completed the present invention.
- the present invention provides the following stable isotope enrichment apparatus and stable isotope enrichment method.
- a stable isotope concentrator that concentrates stable isotopes containing stable isotope atoms by distillation.
- a group of distillation columns in which multiple distillation columns are connected in cascade A raw material supply line that supplies raw materials to one of the distillation columns, A product out-licensing line that derives products from another distillation column located on the secondary side of the one distillation column in the distillation column group. From the one distillation column in the distillation column group or another distillation column located on the primary side of the one distillation column, the concentration of the target stable isotope molecule is lower than the natural abundance ratio.
- An isotope-impaired fluid extraction line for extracting body-depleted gas or isotope-depleted liquid
- the isotope-damaged gas or the isotope-damaged liquid introduced by the isotope-depleted fluid extraction line is subjected to an isotope exchange reaction with another substance having the same stable isotope atom as the stable isotope.
- the isotope-damaged gas or the isotope-damaged solution is regenerated so that the concentration of the stable isotope molecule in the isotope-damaged gas or the isotope-damaged solution approaches the natural abundance ratio, and the isotope-regenerated gas or the isotope isotope.
- the isotope exchange reactor that produces the regenerated liquid and A stable isotope concentrator comprising an isotope regeneration fluid return line that resupplyes the isotope regeneration gas or the isotope regeneration liquid regenerated by the isotope exchange reactor to the one distillation column. Is.
- the isotope exchange reaction in the isotope exchange reactor may be a catalytic heating reaction, a discharge reaction, an ion exchange method, or a photochemical reaction.
- a stable isotope enrichment method for concentrating stable isotopes containing stable isotope atoms by distillation The concentration of the desired stable isotope molecule extracted from one of the distillation towers in which a plurality of distillation towers are cascaded is one of the distillation towers or the other distillation tower located on the primary side of the one distillation tower.
- the isotope-depleted gas or the isotope-damaged gas or the isotope-damaged liquid is subjected to an isotope exchange reaction with another substance having the same stable isotope atom as the stable isotope by causing the isotope-damaged gas or the isotope-damaged liquid having a lower than the natural abundance ratio.
- a stable isotope enrichment method comprising a resupply step of resupplying.
- the concentration of the target stable isotope molecule extracted from one distillation column or another distillation column located on the primary side of one distillation column is higher than the natural abundance ratio.
- the stable isotope concentrator of the present invention since the isotope exchange reactor is provided, an isotope-depleted gas or isotope containing a substance having toxicity or flammability, or a substance causing an environmental load in the atmosphere is provided.
- the amount of impaired liquid discharged can be reduced, and these substances can be reused as raw materials. Therefore, it is possible to reduce the amount of raw materials used while reducing the environmental load in the stable isotope enrichment process, so that a high-purity stable isotope containing the stable isotope molecule of the desired concentration can be used in a good process. It will be possible to obtain it efficiently at low cost while maintaining the environment.
- the concentration of the target stable isotope molecule extracted from one distillation column or another distillation column located on the primary side of the one distillation column is naturally present.
- isotope-damaged gas or isotope-damaged liquid by isotope-exchange reaction of a lower isotope-damaged gas or isotope-damaged solution with another substance having the same stable isotope atom as a stable isotope is naturally present.
- FIG. 1 see also FIG. 2 if necessary.
- FIG. 2 in order to make the features easy to understand, the featured portions may be enlarged or simplified for convenience.
- the materials and the like exemplified in the following description are examples, and the present invention is not limited to them, and the present invention can be appropriately modified without changing the gist thereof.
- isotope-depleted gas or “isotope-depleted liquid” is a gas or liquefied gas discharged from a distillation column in which the concentration of the target stable isotope molecule is lower than the natural abundance ratio.
- the “isotope-regenerated gas” or “isotope-regenerated liquid” is a gas or liquefied gas obtained by regenerating the above-mentioned “isotope-damaged gas” or “isotope-damaged liquid” as a reusable raw material by an isotope exchange reaction.
- isotope exchange reaction Means that.
- FIG. 1 is a system diagram showing a main part of the stable isotope concentrator 100 of the present embodiment.
- the stable isotope concentrator 100 of the present embodiment concentrates a stable isotope containing a stable isotope atom by distillation.
- the stable isotope concentrator 100 includes a group of distillation columns in which a plurality of distillation columns are cascaded, a raw material supply line 30, a product lead-out line 31, an isotope-depleted fluid extraction line 32, and an isotope exchange reactor 22.
- the isotope regeneration fluid purifier 23 and the isotope regeneration fluid return line 33 are provided, and are roughly configured. Further, the stable isotope concentrator 100 of the illustrated example further includes a plurality of capacitors 20, a plurality of reboilers 21, an isotope exchange reaction raw material supply line 34, and an isotope exchange reactor drainage fluid line 35.
- the stable isotope concentrator 100 of the present embodiment is, for example, an apparatus for concentrating a stable isotope of hydrogen, carbon, oxygen or nitrogen by distillation. Further, the stable isotope concentrator 100 of the present embodiment is preferably applied to, for example, the cases shown in the following (1) to (3).
- the raw material is a substance that leads to supply instability, such as when the market supply is small or it has a rare value.
- the substance used as a raw material in the stable isotope concentrator 100 of the present embodiment is not particularly limited, and is, for example, CO, CH 4 , CF 4 , CHF 3 , NO, and so on.
- NH 3 , NF 3 , BF 3 , etc. can be exemplified.
- the distillation column group is a group of distillation columns connected in cascade.
- the nth distillation column from the upstream end of the distillation column group is referred to as the nth distillation column.
- the nth distillation column In the example shown in FIG. 1, among the first distillation columns 1 to n, only the first distillation column 1 to which the stable isotope molecule as a raw material is supplied and the nth distillation column n. Is illustrated.
- the first distillation column 1 to the nth distillation column n are cascaded in the order of the column numbers.
- the first distillation column 1 to the sixth distillation column 6 are connected in cascade.
- the first distillation towers 1 to n of the first distillation tower n concentrate the stable isotope molecules having a high vapor pressure on the top side of the column by distilling the cooled stable isotope molecules at a low temperature or an extremely low temperature. It is configured to concentrate stable isotope molecules with low vapor pressure on the bottom side.
- n is a number of 2 or more.
- n should be 1 (that is, one distillation column). Can be done.
- the tower for supplying the raw material and the tower for collecting the product are the same.
- the diameter of the first distillation column 1 to which the raw material is supplied is usually the largest, and the diameter gradually decreases toward the end.
- the distillation column group is generally designed in this way because the first distillation column 1 on the upstream side has a large distillation load, and the nth distillation column n on the downstream side has a first distillation column. This is because the distillation load is smaller than that of 1.
- each distillation column constituting the distillation column group is, for example, a packed column filled with an irregular packed bed, a packed column filled with an irregular packed bed, or a shelf provided with a rectification stage (shelf). It may be any of a stepped tower and the like.
- One capacitor 20 is provided for each distillation column (first distillation column 1 to nth distillation column n).
- the condenser 20 is provided on a circulation line 36 having both ends connected to different positions on the top of each distillation column.
- the condenser 20 has a function of liquefying the gas that has risen in the distillation column by heat exchange and lowering the inside of the distillation column again.
- the capacitor 20 may be configured to be provided once every several columns for each distillation column (first distillation column 1 to nth distillation column n).
- One reboiler 21 is provided for each distillation column.
- the reboiler 21 is provided on a circulation line 37 having both ends connected to different positions at the bottom of each distillation column.
- the reboiler 21 has a function of vaporizing the liquid that has descended in the distillation column by heat exchange and raising the inside of the distillation column again.
- the reboiler 21 may be configured to be provided once every several columns for each distillation column (first distillation column 1 to nth distillation column n).
- the raw material supply line 30 is a route for introducing a stable isotope as a raw material into the intermediate portion of the first distillation column (one distillation column) 1 in the distillation column group.
- the middle part of the distillation column means a position other than the top and bottom of the distillation column.
- the position (height) at which the raw material is introduced into the first distillation column 1 is not limited to the intermediate portion, but is close to the stable isotope concentration of the raw material in the steady state of the first distillation column 1. It is preferable to have.
- the raw material supply line 30 may be provided with a valve 30a.
- one end of the raw material supply line 30 does not necessarily have to be connected to the first distillation column 1, and when there is another distillation column on the primary side of the distillation column that supplies the raw material, one end of the raw material supply line 30 is It will be connected to the second distillation column 2 and subsequent distillation columns.
- the stable isotope used as a raw material is preferably a stable isotope with a high purity of 99.999% or more.
- the connection point in the first distillation column 1 of the isotope-impaired fluid extraction line 32 differs depending on the target stable isotope molecule, and may be a column top or a column bottom.
- the concentration of the target stable isotope molecule is lower than the natural abundance ratio from the first distillation column (one distillation column) 1 in the distillation column group.
- the gas or isotope-damaged liquid is withdrawn and introduced into the isotope exchange reactor 22.
- the isotope regeneration fluid return line 33 resupplyes the isotope regeneration gas or the isotope regeneration liquid regenerated by the isotope exchange reactor 22 and further purified by the isotope regeneration fluid purifier 23 to the first distillation column 1. do.
- the connection point in the first distillation column 1 of the isotope regeneration fluid return line 33 is connected above the raw material supply line 30 when the target stable isotope molecule is a component having a low vapor pressure, for example. Is preferable.
- the target stable isotope molecule is a component having a high vapor pressure
- the isotope regeneration fluid return line 33 does not necessarily have to be connected to the same distillation column as the raw material supply line 30, and the raw material supply line 30 is connected to the second distillation column 2 and subsequent distillation columns. May be connected to the distillation column on the primary side of the distillation column to which the isotope regeneration fluid return line 33 is connected to the raw material supply line 30.
- the isotope exchange reaction raw material supply line 34 has the same stable isotope atom as the isotope-damaged gas or isotope-damaged liquid, and is nontoxic and has no environmental load or has a very small environmental load, or isotope-damaged gas or This is a line for supplying a substance having a smaller environmental load than an isotope-depleted liquid to the isotope exchange reactor 22. It was
- the isotope-damaged gas or isotope-damaged liquid introduced from the first distillation column 1 by the isotope-depleted fluid extraction line 32 is supplied to the isotope-exchange reactor 22 by the isotope-exchange reaction raw material supply line 34.
- a stable isotope introduced from the first distillation tower 1 and another substance having the same stable isotope atom are subjected to an isotope exchange reaction.
- the isotope exchange reactor 22 is used to bring the concentration of stable isotope molecules in the isotope-damaged gas or isotope-damaged liquid closer to the natural abundance ratio by the isotope-depleted gas or isotope-depleted solution.
- the liquid is regenerated to produce an isotope regenerating gas or an isotope regenerating liquid.
- Examples of the isotope exchange reaction in the isotope exchange reactor 22 include a catalytic heating reaction, a discharge reaction, an ion exchange method, and a photochemical reaction.
- the inside of the isotope exchange reactor 22 can be filled with a substance (not shown) that causes an isotope exchange reaction with an isotope-damaged gas or an isotope-damaged liquid.
- the isotope exchange reaction raw material supply line 34 may be omitted.
- the isotope regeneration fluid purifier 23 purifies the isotope regeneration gas or isotope regeneration liquid generated by the isotope exchange reactor 22 to stabilize the isotope regeneration gas or isotope regeneration liquid as a raw material. Separates into isotope molecules and other substances.
- the method for purifying the isotope regeneration gas or the isotope regeneration liquid in the isotope regeneration fluid purifier 23 is not particularly limited, and examples thereof include solidification purification, adsorption, membrane separation, and distillation.
- a part of the reflux liquid near the top of each distillation column in which the concentration of stable isotope molecules having a high vapor pressure is increased is passed through the path 39 to the tower of the front column. Supplied to the bottom.
- the driving force for the flow of the reflux liquid at this time is the head pressure of the reflux liquid.
- a compressor may be used as a driving force for the flow of the reflux liquid. When a compressor is used, it is also possible to compress the gas at the top of the tower and supply it to the front tower.
- the reflux liquid supplied to the bottom of the front tower is vaporized by the reboiler 21 together with the reflux liquid in the tower, and is returned to the bottom of the tower.
- the product derivation line 31 is a route for deriving the concentrated stable isotope component from the nth distillation column n as a product.
- One end of the product lead-out line 31 is connected to a position near the bottom of the nth distillation column (another distillation column) n located on the secondary side of the first distillation column (one distillation column) 1. ing.
- the product derived from the distillation column by the product extraction line 31 is a stable isotope component concentrated to a high concentration (for example, 99.9 atomic% or more).
- a distillation column serving as a recovery unit may be located in front of the column for supplying the raw material.
- the isotope-impaired fluid extraction line 32 is connected to the end of the distillation column whose one end side is the recovery unit.
- the column for collecting products does not necessarily have to be the final column (nth distillation column n), and may be a distillation column located in the middle of the distillation column group.
- an isotope-impaired gas or an isotope-impaired liquid cannot be reused as a raw material as it is because the concentration of the target stable isotope is lower than the natural abundance ratio. If the isotope-damaged gas or isotope-damaged solution can be regenerated so that the concentration of the desired stable isotope in the isotope-depleted gas or isotope-depleted solution approaches the natural abundance ratio, the regenerated "isotope” It becomes possible to reuse "regenerated gas” or "isotope regenerated liquid" as a raw material.
- An isotope exchange reaction is a reaction in which an atom (or atomic group) in a molecule (or ion) is replaced with an isotope (or an atomic group containing an isotope) in another molecule (or ion).
- the atom (or atomic group) to be replaced is X
- the labeled atom (or atomic group) is marked with *
- the molecule (or ion) involved in the exchange is represented by A or B
- isotope exchange is performed.
- the reaction generally has a relationship represented by the following formula (1).
- An intermediate substance eg, ABX 2
- AX corresponds to an isotope-depleted gas or an isotope-depleted liquid having a concentration of X * smaller than the natural abundance ratio
- BX * is a substance containing X * of the natural abundance ratio. If it corresponds to, the concentration of X * in AX * after the isotope exchange reaction will be close to the natural abundance ratio. Furthermore, when the mixing ratio of BX * to AX is sufficiently large, the concentration of X * in AX * becomes a value substantially equal to the natural abundance ratio.
- the isotope regeneration gas or the isotope regeneration liquid in which the concentration of the target stable isotope is regenerated to be close to the natural abundance is re-supplied to the distillation column as a raw material. It will be possible to do.
- the substance discharged to the outside of the system corresponds to BX. Therefore, the substance corresponding to BX * used in the isotope exchange reaction can be non-toxic and has no environmental load, has an extremely small environmental load, or has a smaller environmental load than AX, and isotopes. It is possible to suppress the environmental impact of the impaired gas or isotope-impaired liquid.
- NO gas whose concentration of 15 N discharged from the distillation column is lower than the natural abundance ratio and general N 2 gas are used. It is conceivable to carry out an isotope exchange reaction. In this case, the NO gas having a concentration of 15 N almost equal to the natural abundance ratio is re-supplied to the distillation column. Further, in this case, a large amount of N 2 gas is discharged, but since N 2 is a substance existing in the air, the influence on the environment is small.
- the present invention is an isotope-damaged gas or a stable isotope in an isotope-damaged solution by subjecting an isotope-damaged gas or an isotope-damaged solution to an isotope exchange reaction with another substance having the same stable isotope atom.
- the isotope-damaged gas or isotope-damaged liquid is regenerated so that the concentration of the molecule approaches the natural abundance ratio, and the isotope-regenerated gas or isotope-regenerated liquid obtained thereby is re-supplied to the distillation unit as a raw material. This makes it possible to reduce the emission of isotope-impaired gas or isotope-impaired liquid, which is toxic, flammable, or has an environmental load due to being discharged into the atmosphere.
- the present invention is also very useful for the purpose of concentrating stable isotopes using a substance whose supply is uncertain due to a small amount of distribution in the market and a high rarity value.
- most of the raw materials supplied are raw materials that are regenerated and resupplied so that the concentration of the target stable isotope molecule is close to the natural abundance ratio. For this reason, the amount of raw materials that need to be newly supplied is almost the same as the amount extracted as a product, so even if some of the loss due to by-products generated by the isotope exchange reaction is taken into consideration, the raw materials used. This is because the total amount of the used amount can be significantly reduced.
- the stable isotope enrichment method of the present embodiment (hereinafter, may be simply referred to as “concentration method”) will be described.
- concentration method the method of concentrating the stable isotope using the stable isotope concentrator 100 of the present embodiment described above will be described with reference to FIG. 1 in the same manner as described above.
- the enrichment method of the present embodiment is a method of enriching a stable isotope containing a stable isotope atom by distillation. That is, in the enrichment method of the present embodiment, a stable isotope concentrator 100 was used, and a plurality of distillation towers were extracted from the first distillation tower (one distillation tower) 1 in the group of distillation towers connected in cascade. A method in which an isotope-damaged gas or isotope-damaged liquid in which the concentration of the target stable isotope molecule is lower than the natural abundance ratio is subjected to an isotope exchange reaction with another substance having the same stable isotope atom as the stable isotope. be.
- the isotope-damaged gas or the isotope-damaged liquid is regenerated so that the concentration of the stable isotope molecule in the isotope-damaged gas or the isotope-damaged liquid approaches the natural abundance ratio. It includes a resupply step of producing a body regenerated gas or an isotope regenerated liquid and resupplying the isotope regenerated gas or the isotope regenerated liquid to the first distillation column 1.
- the raw material (stable isotope) is supplied into the first distillation column 1 in a gas or liquid state from the raw material supply line 30.
- a cold heat source is supplied to the condenser 20
- the stable isotope is cooled and liquefied, and the liquid is stored in the bottom of each distillation column.
- a heating source is supplied to the reboiler 21.
- the isotope-damaged gas or isotope-damaged liquid extracted from the first distillation tower 1 has the same stable isotope atom.
- Isotope regeneration by regenerating the isotope-damaged gas or isotope-damaged liquid extracted from the first distillation tower 1 so that the isotope exchange reaction with other substances causes the concentration of stable isotope molecules to approach the natural abundance ratio. It comprises a resupply step of producing a gas or an isotope regenerated liquid and resupplying the isotope regenerated gas or the isotope regenerated liquid to the first distillation column 1.
- the amount of raw materials used can be reduced while reducing the environmental load in the stable isotope enrichment process. Therefore, high-purity stable isotopes containing stable isotope molecules at the desired concentration are good. It is possible to obtain efficiently at low cost while maintaining the process environment.
- the isotope-damaged gas or the isotope-damaged liquid is used so that the concentration of the target stable isotope in the isotope-damaged gas or the isotope-damaged liquid approaches the natural abundance ratio.
- the regenerated "isotope regenerating gas" or “isotope regenerating liquid” can be reused as a raw material.
- any one of a catalytic heating reaction, a discharge reaction, an ion exchange reaction, or a photochemical reaction can be adopted as the isotope exchange reaction.
- the above-mentioned condenser 20 and reboiler 21 are not indispensable configurations for each distillation column, and are provided when the gas rise is sufficient due to the pressure difference between the front and rear distillation columns, the pump, the blower, and the like. It does not have to be.
- the connection positions of the path 38 and the path 39 with respect to the distillation column may be reversed, and a part of the reflux liquid near the top of the column may be supplied to the bottom of the next column via the path 38.
- a part of the steam at the bottom of the tower may be supplied to the top of the front tower via the path 39.
- the stable isotope concentrator 100 of the present embodiment is an isotope-depleted gas or an isotope-depleted gas extracted from the first distillation tower 1 in which the concentration of the target stable isotope molecule is lower than the natural abundance ratio.
- the isotope exchange reactor 22 for regenerating the isotope-damaged gas or the isotope-damaged liquid and producing the isotope-regenerated gas or the isotope-regenerated liquid.
- the stable isotope concentrator 100 of the present embodiment is provided with the isotope exchange reactor 22 to provide a toxic or flammable substance, or an isotope-depleted gas containing a substance that causes an environmental load in the atmosphere. The amount of isotope-damaged liquid discharged can be reduced, and these substances can be reused as raw materials.
- the stable isotope enrichment method of the present embodiment stabilizes an isotope-damaged gas or an isotope-damaged liquid in which the concentration of the target stable isotope molecule is lower than the natural abundance ratio, which is extracted from one distillation column.
- concentration of the stable isotope molecule in the isotope-damaged gas or the isotope-damaged liquid becomes the same as the natural abundance ratio.
- the step of performing the isotope exchange reaction it is possible to reduce the amount of raw materials used while reducing the environmental load in the stable isotope enrichment process as described above. Therefore, it is possible to efficiently obtain a high-purity stable isotope containing a stable isotope molecule having a target concentration at a low cost while maintaining a good process environment.
- the stable isotope enrichment apparatus and the stable isotope enrichment method of the present invention will be described in more detail by showing examples, but the present invention is not limited to the following examples, and the gist thereof is changed. It can be changed as appropriate to the extent that it does not.
- Example 1 15 N 18 O was concentrated using the stable isotope concentrator 200 of nitric oxide having the configuration according to the present invention shown in FIG.
- the stable isotope concentrator 200 used in Example 1 basically has the same configuration as the stable isotope concentrator 100 shown in FIG. 1, but the distillation column group is composed of six distillation columns. It differs in that.
- the first distillation column 1 to the sixth distillation column 6 are distillation columns in which a regular packing is filled.
- the isotope ratio composition of the raw material nitric oxide supplied to the first distillation column 1 is shown in Table 1 below. Further, the isotope exchange reactor 22 was supplied with a gas in which oxygen and nitrogen were mixed in a volume ratio of 1: 1. The isotope ratio composition of the supplied oxygen and nitrogen is shown in Tables 2 and 3 below. Further, in Example 1, the product of 15 N 18 O was extracted from the bottom of the sixth distillation column 6, and some by-products were extracted from the bottom of the third distillation column 3.
- the isotope exchange reactor 22 a photochemical reaction by irradiation with ultraviolet light was used.
- the isotope ratio composition of nitric oxide before and after the flow direction of the isotope exchange reactor 22 is shown in Table 5 below.
- nitric oxide and other substances were separated by using an adsorption method and a distillation method.
- the nitric oxide stable isotope concentrator 200 comprises an isotope scrambler 24.
- the isotope scrambler 24 is a device for generating isotope scrambling, which is an exchange reaction in which atoms are randomly rearranged.
- one end of the isotope enrichment gas extraction line 40 is connected to the bottom portion of the fourth distillation column 4, and the other end is connected to the isotope scrambler 24.
- Part or all of nitric oxide was withdrawn from the fourth distillation column 4 and fed to the isotope scrambler 24.
- the nitric oxide that had undergone the isotope exchange reaction in the isotope scrambler 24 was returned to the top portion of the fifth distillation column 5 by the isotope concentrated gas return line 41.
- Liquefied methane was used as the cold source of the condenser 20, and liquefied methane was supplied to each condenser from the liquefied methane supply line 42.
- An electric heater was used as the heat source of the reboiler 21.
- the abundance ratio of stable isotope molecules of the 15 N 18 O product delivered from the sixth distillation column 6, which is the final stage, at the time of stabilization of the entire concentrator is as shown in Tables 6 and 7 below.
- the total amount of heat exchange required for the capacitor 20 and the reboiler 21 was 160 kW.
- Comparative Example 1 In Comparative Example 1, 15 N 18 O was concentrated using the stable isotope concentrator 300 of nitric oxide shown in FIG.
- the stable isotope concentrator 300 shown in FIG. 3 is not provided with the isotope exchange reactor 22, the isotope regeneration fluid purifier 23, and the lines before and after the isotope exchange reactor 22, and the stable isotope according to the present invention shown in FIG. It is different from the body concentrator 200.
- the distillation column group is composed of six distillation columns, and the first distillation column 1 to the sixth distillation column 6 are inside. It is a distillation column filled with regular filling.
- the isotope ratio composition of the raw material nitric oxide supplied to the first distillation column 1 is as shown in Table 1 above. Further, in Comparative Example 1, the product of 15 N 18 O was extracted from the bottom of the sixth distillation column 6, and some by-products were extracted from the bottom of the third distillation column 3.
- the stable isotope enricher 300 shown in FIG. 3 includes an isotope scrambler 24 similar to the stable isotope enricher 200 shown in FIG. Further, in the stable isotope concentrator 300, one end of the isotope enrichment gas extraction line 40 is connected to the bottom portion of the fourth distillation column 4, and the other end is connected to the isotope scrambler 24. .. Part or all of nitric oxide was withdrawn from the fourth distillation column 4 and fed to the isotope scrambler 24. The nitric oxide subjected to the isotope exchange reaction in the isotope scrambler 24 was returned to the top portion of the fifth distillation column 5 by the isotope enriched gas return line 41.
- Liquefied methane was used as the cold source of the condenser 20, and liquefied methane was supplied to each condenser from the liquefied methane supply line 42.
- An electric heater was used as the heat source of the reboiler 21.
- the abundance ratios of stable isotope molecules of the 15 N 18 O product delivered from the sixth distillation column 6, which is the final stage, at the time of stabilization of the entire concentrator are as shown in Tables 9 and 10 below. ..
- the total amount of heat exchange required for the capacitor 20 and the reboiler 21 was 160 kW.
- Example 1 since the total amount of the product is 17 NL / hr out of the raw material 20 Nm 3 / hr, the flow rate of nitric oxide is almost the same as that of the raw material discharged from the top of the first tower. Needed to be processed. In the ammonia catalytic reduction method, it is necessary to add more than the same amount of ammonia as nitric oxide, and the amount of toxic gas handled increases, so the manufacturing cost increases with the implementation of safety measures. On the other hand, in Example 1, the added gas is oxygen and nitrogen, and most of the exhaust gas is oxygen and nitrogen separated by the isotope regeneration fluid purifier 23. Therefore, it is not necessary to perform abatement treatment, and it can be manufactured at low cost. In addition, the amount of nitric oxide newly required as a raw material could be reduced to 1/10. Moreover, the heat exchange amount, the product concentration, and the product amount required in each of Example 1 and Comparative Example 1 were almost the same.
- Example 2 13 CF 4 was enriched using a stable isotope enricher 400 for carbon tetrafluoride having the configuration according to the present invention as shown in FIG.
- the stable isotope concentrator 400 used in Example 2 is different from the stable isotope concentrator 100 in that the distillation column group is composed of 14 distillation columns.
- the first distillation column 1 to the 14th distillation column 14 is a distillation column in which a regular packing is filled.
- the isotope ratio composition of the raw material carbon tetrafluoride supplied to the first distillation column 1 is as shown in Table 11 below.
- the isotope exchange reactor 22 was filled with a carbon catalyst carrying palladium.
- the metal to be supported on the carbon carrier for example, zinc, nickel, cesium, cobalt, vanadium, calcium, manganese, magnesium, tungsten, titanium, platinum, copper or the like can be used in addition to the above-mentioned palladium. ..
- the carrier of the catalyst in addition to the above carbon, for example, aluminum phosphate, alumina, a complex of alumina and zirconium oxide, or the like can be used.
- the amount of the catalyst charged in the isotope exchange reactor 22 is about 30 kg, and the isotope ratio composition of carbon in the carbon carrier is as shown in Table 12 below. Further, in Example 2, the product of 13 CF 4 was extracted from the bottom of the 14th distillation column 14.
- the isotope ratio composition of carbon tetrafluoride before and after the flow direction of the isotope exchange reactor 22 is as shown in Table 14 below.
- carbon tetrafluoride and other substances were separated by using a distillation method. Liquefied carbon tetrafluoride was used as the cold source of the capacitor 20, and liquefied carbon tetrafluoride was supplied to each capacitor from the liquefied carbon tetrafluoride supply line 42A.
- Gas tetrafluoride was used as the heat source of the reboiler 21, and gas tetrafluoride was supplied to each reboiler 21 from the gas tetrafluoride supply line 43.
- the abundance ratio of stable isotope molecules of the 3 CF 4 product delivered from the 14th distillation column 14, which is the final stage, at the time of stabilization of the entire concentrator is as shown in Tables 15 and 16 below.
- the total amount of heat exchange required for the capacitor 20 and the reboiler 21 was 1180 kW.
- the isotope ratio composition of the raw material carbon tetrafluoride supplied to the first distillation column 1 is as shown in Table 11 above. Further, in Comparative Example 2, the product of 13 CF 4 was extracted from the bottom of the 14th distillation column 14.
- Liquefied carbon tetrafluoride was used as the cold source of the capacitor 20, and liquefied carbon tetrafluoride was supplied to each capacitor from the liquefied carbon tetrafluoride supply line 42A.
- Gas tetrafluoride was used as the heat source of the reboiler 21, and gas tetrafluoride was supplied to each reboiler 21 from the gas tetrafluoride supply line 43.
- the abundance ratio of stable isotope molecules of the 13 CF4 product delivered from the 14th distillation column 14 which is the final stage, at the time of stabilization of the entire concentrator is as shown in Tables 18 and 19 below.
- the total amount of heat exchange required for the capacitor 20 and the reboiler 21 was 1170 kW.
- Comparative Example 2 In Comparative Example 2, about 680 tons of carbon tetrafluoride is emitted into the atmosphere annually, which is equivalent to about 5 million tons of CO 2 emissions, which has a great impact on the environment. Therefore, in the case of Comparative Example 2, it is necessary to convert it into a substance having a small impact on the environment and discharge it, and this cost is also added. On the other hand, in Example 2, although some emissions of CO 2 and the like generated as by-products in the isotope exchange reactor 22 are observed, the emissions are very small compared to the CO 2 conversion in Comparative Example 2. ..
- the above results are not limited to the stable isotope molecules in Examples 1 and 2, and are the same when the present invention is applied to other stable isotope molecules. That is, for example, by applying the present invention to the enrichment of stable isotopes such as CO, CH 4 , CF 4 , CHF 3 , NH 3 , NF 3 , BF 3 , etc., a substance having toxicity or flammability, or in the atmosphere It is possible to reduce the amount of exhaust gas or effluent that causes an environmental load when discharged to. In addition, when a substance with an uncertain supply is used as a raw material, the amount used can be reduced.
- stable isotope molecules such as CO, CH 4 , CF 4 , CHF 3 , NH 3 , NF 3 , BF 3 , etc.
- the stable isotope concentrating device and the stable isotope concentrating method of the present invention it is possible to reduce the emission of toxic or flammable substances or substances that cause an environmental load in the atmosphere, and the amount of raw materials used can be reduced. Can be reduced. Therefore, in the present invention, for example, in addition to stable isotopes used as tracers in the fields of natural science and medical science, stable isotopes used in drug discovery and organic synthesis, and infrared rays using differences in spectroscopic properties. It is extremely useful in providing stable isotopes used in Raman spectroscopy.
- isotope enriched gas extraction line 41 isotope Concentrated gas return line 42 . Liquefied methane supply line 42A . Liquefied tetrafluorocarbon supply line 43 . Gas tetrafluorocarbon supply line
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Abstract
Description
特許文献2が開示する技術を用いて炭素安定同位体を濃縮した場合においても、上述した特許文献1の場合と同様、第1の蒸留塔の塔頂から、13COの濃度が天然存在比よりも減少したCOガスが系外に大量に放出される(以下、安定同位体濃縮装置から排出される、目的とする安定同位体の濃度が天然存在比よりも減少した排ガスまたは排液を、「同位体減損ガス」または「同位体減損液」と称することがある。)。この場合、一酸化炭素は可燃性かつ毒性を有するから、そのまま大気に放出することはできず、除害処理を実施する必要がある。
除害処理の工業的な方法としては、例えば、フレアスタックによる方法や、触媒反応による酸化処理を用いた方法等が挙げられる。
上述したいずれの方法も、一酸化炭素を酸化することによって二酸化炭素に変換する。結果的に大量の二酸化炭素を大気中に放出することになり、環境負荷を伴う。
なお、四フッ化炭素の場合、可燃性や毒性は無いことから、除害処理を実施する必要は無いものの、四フッ化炭素の地球温暖化係数は約7400と非常に大きいため、環境への負荷はより大きいものになるという問題もある。地球温暖化計数は、数ある環境負荷を示す指標のうちの一つである。
例えば、窒素の安定同位体を濃縮する方法としては、一酸化窒素蒸留が挙げられる。この方法は、窒素の同位体と同時に酸素の同位体が得られる利便性の高い方法である。非特許文献1に記載されているように、米国において、95%以上の高濃度の酸素と、窒素との重成分を併産するプラントが存在していたことが知られている。しかしながら、一酸化窒素は窒素酸化物として酸性雨や光化学スモッグを引き起こす原因とされており、毒性を有する。このため、一酸化炭素と同様、大気中に直接放出することはできないことから、アンモニア接触還元法等による除害処理が必要となる。
(1)蒸留によって安定同位体原子を含む安定同位体を濃縮する安定同位体濃縮装置であって、
複数の蒸留塔がカスケード接続された蒸留塔群と、
前記蒸留塔群のうち、一の蒸留塔に原料を供給する原料供給ラインと、
前記蒸留塔群のうち、前記一の蒸留塔よりも二次側に位置する他の蒸留塔から製品を導出する製品導出ラインと、
前記蒸留塔群のうちの前記一の蒸留塔もしくは前記一の蒸留塔よりも一次側に位置する他の蒸留塔から、目的とする安定同位体分子の濃度が天然存在比よりも低下した、同位体減損ガスまたは同位体減損液を抜き出す同位体減損流体抜出ラインと、
前記同位体減損流体抜出ラインによって導入される前記同位体減損ガスまたは前記同位体減損液を、前記安定同位体と同じ安定同位体原子を有する他の物質と同位体交換反応させることにより、前記同位体減損ガスまたは前記同位体減損液中における前記安定同位体分子の濃度を天然存在比に近づけるように、前記同位体減損ガスまたは前記同位体減損液を再生し、同位体再生ガスまたは同位体再生液を生成する同位体交換反応器と、
前記同位体交換反応器で再生された前記同位体再生ガスまたは前記同位体再生液を前記一の蒸留塔に再供給する同位体再生流体返送ラインとを備えることを特徴とする安定同位体濃縮装置である。
複数の蒸留塔がカスケード接続された蒸留塔群のうちの一の蒸留塔もしくは前記一の蒸留塔よりも一次側に位置する他の蒸留塔から抜き出した、目的とする安定同位体分子の濃度が天然存在比よりも低下した同位体減損ガスまたは同位体減損液を、前記安定同位体と同じ安定同位体原子を有する他の物質と同位体交換反応させることにより、前記同位体減損ガスまたは前記同位体減損液中における前記安定同位体分子の濃度を天然存在比に近づけることで同位体再生ガスまたは同位体再生液を生成し、前記一の蒸留塔に前記同位体再生ガスまたは前記同位体再生液を再供給する再供給工程を含むことを特徴とする安定同位体濃縮方法。
本発明の安定同位体濃縮装置によれば、上記同位体交換反応器を備えるため、毒性や可燃性を有する物質、または大気中において環境負荷を生じさせる物質を含んだ同位体減損ガスまたは同位体減損液の排出量を低減でき、かつこれらの物質を原料として再利用することが可能になる。
したがって、安定同位体の濃縮プロセスにおける環境負荷を低減しながら、原料の使用量を低減することができるので、目的とする濃度の安定同位体分子を含む高純度の安定同位体を、良好なプロセス環境を維持しながら、低コストで効率的に得ることが可能になる。
本発明の安定同位体濃縮方法は、上記同位体交換反応を行う再供給工程を具備するため、安定同位体の濃縮プロセスにおける環境負荷を低減しながら、原料の使用量を低減することができる。このため、目的とする濃度の安定同位体分子を含む高純度の安定同位体を、良好なプロセス環境を維持しながら、低コストで効率的に得ることが可能になる。
なお、以下の説明で用いる図面は、特徴をわかりやすくするため、便宜上、特徴となる部分を拡大あるいは簡略化して示している場合がある。また、以下の説明において例示される材料等は一例であって、本発明はそれらに限定されるものではなく、その要旨を変更しない範囲で適宜変更して実施することが可能である。
「同位体再生ガス」または「同位体再生液」とは、上記「同位体減損ガス」または「同位体減損液」が、同位体交換反応によって再使用可能な原料として再生されたガスまたは液化ガスのことを意味する。
以下、本実施形態の安定同位体濃縮装置について詳述する。
図1は、本実施形態の安定同位体濃縮装置100の主要部を示す系統図である。
本実施形態の安定同位体濃縮装置100は、蒸留によって安定同位体原子を含む安定同位体を濃縮する。安定同位体濃縮装置100は、複数の蒸留塔がカスケード接続された蒸留塔群と、原料供給ライン30と、製品導出ライン31と、同位体減損流体抜出ライン32と、同位体交換反応器22と、同位体再生流体精製器23と、同位体再生流体返送ライン33とを備え、概略構成される。
また、図示例の安定同位体濃縮装置100は、さらに、複数のコンデンサ20と、複数のリボイラ21と、同位体交換反応原料供給ライン34と、同位体交換反応器排流体ライン35を備える。
また、本実施形態の安定同位体濃縮装置100は、例えば、以下の(1)~(3)に示すようなケースに適用することが好ましい。
(1)原料となる物質が毒性や可燃性を有するか、または原料となる物質が大気中に排出されることで環境負荷が生じるおそれがある場合。
(2)原料となる毒性を有する物質を除害処理することで変換された物質が、大気中に排出されたときに環境負荷を生じさせるおそれがある場合。
(3)市場供給量が少ないか、または希少価値がある等、供給不安に繋がる物質が原料である場合。
NH3、NF3、BF3等を例示できる。
以下の説明においては、蒸留塔群の上流側末端からn番目の蒸留塔を第nの蒸留塔という。
図1に示す例では、第1の蒸留塔1~第nの蒸留塔nのうち、原料である安定同位体分子が供給される第1の蒸留塔1と、第nの蒸留塔nのみとを図示している。
第1の蒸留塔1~第nの蒸留塔nは、冷却された安定同位体分子を低温または極低温で蒸留することで、塔頂側に蒸気圧の高い安定同位体分子を濃縮し、塔底側に蒸気圧の低い安定同位体分子を濃縮するように構成される。
これに対して、例えば、原料として製品の純度に近い安定同位体を用い、1本の蒸留塔で製品濃度まで濃縮できる場合には、nは1(すなわち、1本の蒸留塔)とすることができる。この場合、原料を供給する塔と製品を採取する塔は同一となる。
なお、コンデンサ20は、各蒸留塔(第1の蒸留塔1~第nの蒸留塔n)に対して、数塔おきに1つ設けられた構成であってもよい。
なお、リボイラ21は、各蒸留塔(第1の蒸留塔1~第nの蒸留塔n)に対して、数塔おきに1つ設けられた構成であってもよい。
蒸留塔の中間部とは、蒸留塔の塔頂部および塔底部以外の位置を意味する。
なお、第1の蒸留塔1に原料を導入する位置(高さ)は、中間部に限定されるものではなく、第1の蒸留塔1の定常状態における原料の安定同位体濃度に近い位置であることが好ましい。
また、原料供給ライン30には、図1に示すように、バルブ30aが設けられていてもよい。
なお、必ずしも原料供給ライン30の一端が第1の蒸留塔1に接続されている必要はなく、原料を供給する蒸留塔の一次側に他の蒸留塔がある場合、原料供給ライン30の一端は第2の蒸留塔2以降の蒸留塔に接続されることになる。
同位体再生流体精製器23における同位体再生ガスまたは同位体再生液の精製方法としては、特に限定されないが、例えば、固化精製、吸着、膜分離、または蒸留等の方法が例示できる。
なお、還流液の流れの推進力として圧縮機を用いてもよい。圧縮機を用いた場合には、塔頂のガスを圧縮して前塔に供給することも可能である。
前塔の塔底に供給された還流液は、その塔内の還流液とともにリボイラ21で気化され、その塔の塔底に還流される。
一般的に、同位体減損ガスまたは同位体減損液は、目的とする安定同位体の濃度が天然存在比よりも低下しているため、そのまま原料として再利用することはできない。同位体減損ガスまたは同位体減損液中における、目的とする安定同位体の濃度が天然存在比に近づけるように同位体減損ガスまたは同位体減損液を再生することができれば、再生された「同位体再生ガス」または「同位体再生液」を原料として再利用することが可能になる。
ここで、入れ替わる原子(または原子団)をXとし、標識された原子(または原子団)に*印を付与し、交換に関与する分子(またはイオン)をAまたはBで表すと、同位体交換反応は一般に下記式(1)で表される関係となる。左辺から右辺への反応の間に、中間体となる物質(例えば、ABX2)が存在してもよい。
AX+BX*→AX*+BX ・・・・・(1)
次に、本実施形態の安定同位体濃縮方法(以下、単に「濃縮方法」と称することがある。)について説明する。
なお、本実施形態においては、上述した本実施形態の安定同位体濃縮装置100を用いて安定同位体を濃縮する方法について、上記と同様、図1を参照しながら説明する。
そして、本実施形態の濃縮方法は、同位体減損ガスまたは同位体減損液中における安定同位体分子の濃度が天然存在比に近づけるように、同位体減損ガスまたは同位体減損液を再生して同位体再生ガスまたは同位体再生液を生成し、第1の蒸留塔1に同位体再生ガスまたは同位体再生液を再供給する再供給工程を含む。
この際、例えば、コンデンサ20に冷熱源を供給し、安定同位体を冷却して液化させて、液体を各蒸留塔の底部に溜める。
リボイラ21の運転に必要な液量が各蒸留塔の底部にたまった後、リボイラ21に加熱源を供給する。
そして、各蒸留塔が安定状態であることを確認した後、第1の蒸留塔1に原料供給ライン30から原料(安定同位体)の連続導入を開始し、安定同位体濃縮装置100の濃縮運転を開始する。
すなわち、安定同位体濃縮装置100の起動が完了した後、第nの蒸留塔nから製品導出ライン31によって製品を導出する。
これにより、安定同位体の濃縮プロセスにおける環境負荷を低減しながら、原料の使用量を低減することができるので、目的とする濃度の安定同位体分子を含む高純度の安定同位体を、良好なプロセス環境を維持しながら、低コストで効率的に得ることが可能になる。
以上、実施形態により本発明に係る安定同位体濃縮装置および安定同位体濃縮方法の一例を説明したが、本発明は上記実施形態に限定されるものではない。上記実施形態における各構成およびそれらの組み合わせ等は一例であり、本発明の趣旨を逸脱しない範囲内で、構成の付加、省略、置換、およびその他の変更が可能である。
以上説明したように、本実施形態の安定同位体濃縮装置100は、第1の蒸留塔1から抜き出した、目的とする安定同位体分子の濃度が天然存在比よりも低下した同位体減損ガスまたは同位体減損液を、同じ安定同位体原子を有する他の物質と同位体交換反応させることにより、同位体減損ガスまたは同位体減損液中における安定同位体分子の濃度が天然存在比に近づけるように、同位体減損ガスまたは同位体減損液を再生し、同位体再生ガスまたは同位体再生液を生成する同位体交換反応器22を備える。
本実施形態の安定同位体濃縮装置100は、上記同位体交換反応器22を備えることで、毒性や可燃性を有する物質、または大気中において環境負荷を生じさせる物質を含んだ同位体減損ガスまたは同位体減損液の排出量を低減でき、かつこれらの物質を原料として再利用することが可能になる。
したがって、安定同位体の濃縮プロセスにおける環境負荷を低減しながら、原料の使用量を低減することができるので、目的とする濃度の安定同位体分子を含む高純度の安定同位体を、良好なプロセス環境を維持しながら、低コストで効率的に得ることが可能になる。
本発明によれば、上記同位体交換反応を行う工程を具備することにより、上記同様、安定同位体の濃縮プロセスにおける環境負荷を低減しながら、原料の使用量を低減することができる。このため、目的とする濃度の安定同位体分子を含む高純度の安定同位体を、良好なプロセス環境を維持しながら、低コストで効率的に得ることが可能になる。
実施例1においては、図2に示す、本発明に係る構成を備える一酸化窒素の安定同位体濃縮装置200を用いて、15N18Oの濃縮を行った。実施例1で用いた安定同位体濃縮装置200は、基本的には、図1に示した安定同位体濃縮装置100と同様の構成を有するが、蒸留塔群が6本の蒸留塔から構成される点で異なる。第1の蒸留塔1~第6の蒸留塔6は、内部に規則充填物が充填された蒸留塔である。
また、同位体交換反応器22には、酸素と窒素とを体積比で1対1に混合したガスを供給した。供給した酸素と窒素との同位体比組成を下記表2および3に示す。
また、実施例1では、15N18Oの製品を、第6の蒸留塔6の塔底より抜き出し、一部の副製品を、第3の蒸留塔3の塔底より抜き出した。
(1)原料一酸化窒素流量
(2)15N18O製品一酸化窒素抜出流量
(3)第1の蒸留塔1から同位体交換反応器22に供給する一酸化窒素の流量
(4)同位体交換反応原料供給ライン34から供給される酸素と窒素の混合ガスの流量
(5)同位体再生流体精製器23から第1の蒸留塔1の中間部に返送される一酸化窒素の流量
(6)副製品の流量
同位体交換反応器22の流れ方向の前後における一酸化窒素の同位体比組成を、下記表5に示す。
また、同位体再生流体精製器23においては、吸着法および蒸留法を利用して、一酸化窒素と、それ以外の物質とに分離した。
一酸化窒素の安定同位体濃縮装置200は、同位体スクランブラ24を備える。この同位体スクランブラ24は、原子をランダムに組み替える交換反応である、同位体スクランブリングを発生させる装置である。
また、安定同位体濃縮装置200では、同位体濃縮ガス抜出ライン40が、一端が第4の蒸留塔4の塔底部分に接続され、他端が同位体スクランブラ24に接続されている。一酸化窒素の一部または全部を第4の蒸留塔4から抜き出し、同位体スクランブラ24に供給した。
同位体スクランブラ24において同位体交換反応を経た一酸化窒素は、同位体濃縮ガス返送ライン41によって第5の蒸留塔5の塔頂部分に返送された。
コンデンサ20の寒冷源には液化メタンを用いており、液化メタン供給ライン42より各コンデンサに液化メタンが供給された。
リボイラ21の熱源には電気ヒータを用いた。
濃縮装置全体の安定時における、最終段である第6の蒸留塔6から送出される15N18O製品の安定同位体分子の存在割合は、下記表6および7に示すとおりであった。
また、コンデンサ20とリボイラ21で必要な熱交換量の総量は160kWであった。
比較例1においては、図3に示す一酸化窒素の安定同位体濃縮装置300を用いて、15N18Oの濃縮を行った。図3に示す安定同位体濃縮装置300は、同位体交換反応器22、同位体再生流体精製器23、およびその前後のラインを備えていない点で、図2に示した本発明に係る安定同位体濃縮装置200とは異なる。
また、安定同位体濃縮装置300は、安定同位体濃縮装置200と同様、蒸留塔群が6本の蒸留塔から構成されおり、第1の蒸留塔1~第6の蒸留塔6は、内部に規則充填物が充填された蒸留塔である。
また、比較例1では、15N18Oの製品を、第6の蒸留塔6の塔底より抜き出し、また、一部の副製品を、第3の蒸留塔3の塔底より抜き出した。
(1)原料一酸化窒素流量
(2)15N18O製品一酸化窒素抜出流量
(3)副製品の流量
また、安定同位体濃縮装置300においても、同位体濃縮ガス抜出ライン40が、一端が第4の蒸留塔4の塔底部分に接続され、他端が同位体スクランブラ24に接続されている。一酸化窒素の一部または全部を第4の蒸留塔4から抜き出し、同位体スクランブラ24に供給した。
同位体スクランブラ24において同位体交換反応が実施された一酸化窒素は、同位体濃縮ガス返送ライン41によって第5の蒸留塔5の塔頂部分に返送された。
コンデンサ20の寒冷源には液化メタンを用いており、液化メタン供給ライン42より各コンデンサに液化メタンが供給された。
リボイラ21の熱源には電気ヒータを用いた。
そして、濃縮装置全体の安定時における、最終段である第6の蒸留塔6から送出される15N18O製品の安定同位体分子の存在割合は、下記表9および10に示すとおりであった。
また、コンデンサ20とリボイラ21で必要な熱交換量の総量は160kWであった。
一方、実施例1においては、添加ガスは酸素と窒素とであり、排ガスの大半も同位体再生流体精製器23で分離される酸素および窒素である。そのため、除害処理を行う必要がなく、低コストで製造することができた。また、原料として新たに必要な一酸化窒素の量も10分の1に低減することができた。
また、実施例1および比較例1の各々において必要な熱交換量、製品濃度、製品量は、ほぼ同等であった。
実施例2においては、図4に示すような、本発明に係る構成を備える四フッ化炭素の安定同位体濃縮装置400を用いて、13CF4の濃縮を行った。実施例2で用いた安定同位体濃縮装置400は、蒸留塔群が14本の蒸留塔で構成されている点が安定同位体濃縮装置100と異なる。おり、第1の蒸留塔1~第14の蒸留塔14は、内部に規則充填物が充填された蒸留塔である。
同位体交換反応器22には、パラジウムを担持したカーボン触媒を充填した。
なお、カーボン担体に担持させる金属としては、上記パラジウムの他、例えば、亜鉛、ニッケル、セシウム、コバルト、バナジウム、カルシウム、マンガン、マグネシウム、タングステン、チタン、白金、または銅等を用いることも可能である。
また、触媒の担体としては、上記カーボンの他、例えば、リン酸アルミニウム、アルミナ、アルミナと酸化ジルコニウムの複合体等を用いることも可能である。
同位体交換反応器22に充填した触媒の量は約30kgであり、カーボン担体中の炭素の同位体比組成は下記表12に示すとおりである。
また、実施例2では、13CF4の製品を、第14の蒸留塔14の塔底より抜き出した。
(1)原料四フッ化炭素流量
(2)13CF4製品四フッ化炭素抜出流量
(3)第1の蒸留塔1から同位体交換反応器22に供給する四フッ化炭素の流量
(4)同位体再生流体精製器23から第1の蒸留塔1の中間部に返送される四フッ化炭素の流量
同位体交換反応器22の流れ方向の前後における四フッ化炭素の同位体比組成は、下記表14に示すとおりであった。
また、同位体再生流体精製器23においては、蒸留法を利用して、四フッ化炭素とそれ以外の物質とに分離した。
コンデンサ20の寒冷源には液化四フッ化炭素を用いており、液化四フッ化炭素供給ライン42Aより各コンデンサに液化四フッ化炭素を供給した。
リボイラ21の熱源にはガス四フッ化炭素を用い、ガス四フッ化炭素供給ライン43より各リボイラ21にガス四フッ化炭素を供給した。
濃縮装置全体の安定時における、最終段である第14の蒸留塔14から送出された3CF4製品の安定同位体分子の存在割合は、下記表15および16に示すとおりであった。
また、コンデンサ20とリボイラ21で必要な熱交換量の総量は1180kWであった。
比較例2においては、図5に示す四フッ化炭素の安定同位体濃縮装置500を用いて、13CF4の濃縮を行った。
図5に示す安定同位体濃縮装置500は、同位体交換反応器22、同位体再生流体精製器23、およびその前後のラインを備えていない点で、図4に示した本発明に係る安定同位体濃縮装置400とは異なる。
また、安定同位体濃縮装置500は、安定同位体濃縮装置400と同様、蒸留塔群が14本の蒸留塔から構成されおり、第1の蒸留塔1~第14の蒸留塔14は、内部に規則充填物が充填された蒸留塔である。
また、比較例2においても、13CF4の製品を、第14の蒸留塔14の塔底より抜き出した。
(1)原料四フッ化炭素流量
(2)13CF4製品四フッ化炭素抜出流量
リボイラ21の熱源にはガス四フッ化炭素を用い、ガス四フッ化炭素供給ライン43より各リボイラ21にガス四フッ化炭素を供給した。
濃縮装置全体の安定時における、最終段である第14の蒸留塔14から送出された13CF4製品の安定同位体分子の存在割合は、下記表18および19に示すとおりであった。
また、コンデンサ20とリボイラ21で必要な熱交換量の総量は1170kWであった。
これに対して、実施例2においては、原料として必要な四フッ化炭素は年間約38トンであり、原料の使用量を大きく低減することができ、十分に供給可能な原料の量であった。
一方、実施例2では、同位体交換反応器22において副生成物として発生したCO2等の排出が一部みられるものの、その排出量は、比較例2におけるCO2換算に対して非常に小さい。
したがって、本発明は、例えば、自然科学や医療分野におけるトレーサとして使用される安定同位体の他、創薬・有機合成で使用される安定同位体、分光学的性質の差異を利用した赤外・ラマン分光法で使用される安定同位体を提供するのに極めて有用である。
1,2,3,4,5,6~14,(n)…蒸留塔(第1の蒸留塔1~第nの蒸留塔n;蒸留塔群)
20…コンデンサ
21…リボイラ
22…同位体交換反応器
23…同位体再生流体精製器
24…同位体スクランブラ
30…原料供給ライン
30a…バルブ
31…製品導出ライン
32…同位体減損流体抜出ライン
33…同位体再生流体返送ライン
34…同位体交換反応原料供給ライン
35…同位体交換反応器排流体ライン
36,37…循環ライン
38,39…経路
40…同位体濃縮ガス抜出ライン
41…同位体濃縮ガス返送ライン
42…液化メタン供給ライン
42A…液化四フッ化炭素供給ライン
43…ガス四フッ化炭素供給ライン
Claims (4)
- 蒸留によって安定同位体原子を含む安定同位体を濃縮する安定同位体濃縮装置であって、
複数の蒸留塔がカスケード接続された蒸留塔群と、
前記蒸留塔群のうち、一の蒸留塔に原料を供給する原料供給ラインと、
前記蒸留塔群のうち、前記一の蒸留塔よりも二次側に位置する他の蒸留塔から製品を導出する製品導出ラインと、
前記蒸留塔群のうちの前記一の蒸留塔もしくは前記一の蒸留塔よりも一次側に位置する他の蒸留塔から、目的とする安定同位体分子の濃度が天然存在比よりも低下した同位体減損ガスまたは同位体減損液を抜き出す同位体減損流体抜出ラインと、
前記同位体減損流体抜出ラインによって導入される前記同位体減損ガスまたは前記同位体減損液を、前記安定同位体と同じ安定同位体原子を有する他の物質と同位体交換反応させることにより、前記同位体減損ガスまたは前記同位体減損液中における前記安定同位体分子の濃度を天然存在比に近づけるように、前記同位体減損ガスまたは前記同位体減損液を再生し、同位体再生ガスまたは同位体再生液を生成する同位体交換反応器と、
前記同位体交換反応器で再生された前記同位体再生ガスまたは前記同位体再生液を前記一の蒸留塔に再供給する同位体再生流体返送ラインと、
を備えることを特徴とする安定同位体濃縮装置。 - 前記同位体交換反応器における前記同位体交換反応が、触媒加熱反応、放電反応、イオン交換反応、または光化学反応の何れかであることを特徴とする請求項1に記載の安定同位体濃縮装置。
- 蒸留によって安定同位体原子を含む安定同位体を濃縮する安定同位体濃縮方法であって、
複数の蒸留塔がカスケード接続された蒸留塔群のうちの一の蒸留塔もしくは前記一の蒸留塔よりも一次側に位置する他の蒸留塔から抜き出した、目的とする安定同位体分子の濃度が天然存在比よりも低下した同位体減損ガスまたは同位体減損液を、前記安定同位体と同じ安定同位体原子を有する他の物質と同位体交換反応させることにより、前記同位体減損ガスまたは前記同位体減損液中における前記安定同位体分子の濃度を天然存在比に近づけるように、前記同位体減損ガスまたは前記同位体減損液を再生して同位体再生ガスまたは同位体再生液を生成し、前記一の蒸留塔に前記同位体再生ガスまたは前記同位体再生液を再供給する再供給工程を含むことを特徴とする安定同位体濃縮方法。 - 前記同位体交換反応が、触媒加熱反応、放電反応、イオン交換反応、または光化学反応の何れかであることを特徴とする請求項3に記載の安定同位体濃縮方法。
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Citations (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2000027509A1 (fr) * | 1998-11-09 | 2000-05-18 | Nippon Sanso Corporation | Procede et dispositif d'enrichissement en composant lourd d'isotopes d'oxygene |
JP4309162B2 (ja) | 2002-12-04 | 2009-08-05 | パナソニックエコシステムズ株式会社 | 一酸化炭素除去ユニット、一酸化炭素除去方法、空気清浄装置および一酸化炭素除去触媒組成物 |
JP4327287B2 (ja) | 1999-01-29 | 2009-09-09 | 大陽日酸株式会社 | 重酸素水の製造方法および装置 |
CN201493052U (zh) * | 2009-08-13 | 2010-06-02 | 上海化工研究院 | 一种间歇生产超轻水的同位素分离装置 |
JP2018164884A (ja) | 2017-03-28 | 2018-10-25 | 大陽日酸株式会社 | 一酸化炭素安定同位体濃縮装置および一酸化炭素安定同位体濃縮方法 |
JP2019513556A (ja) * | 2016-04-08 | 2019-05-30 | アクツィオネルノエ オブシチェストヴォ “ラディエヴィ インスティテュート イメニ ヴェーゲー フローピナ” | 酸素18を富化した水を得る方法、およびその製造のための設備 |
-
2020
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2021
- 2021-12-08 CN CN202180086833.2A patent/CN116670070A/zh active Pending
- 2021-12-08 US US18/258,788 patent/US20240082786A1/en active Pending
- 2021-12-08 EP EP21910311.6A patent/EP4268942A1/en active Pending
- 2021-12-08 WO PCT/JP2021/045097 patent/WO2022138162A1/ja active Application Filing
Patent Citations (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2000027509A1 (fr) * | 1998-11-09 | 2000-05-18 | Nippon Sanso Corporation | Procede et dispositif d'enrichissement en composant lourd d'isotopes d'oxygene |
JP4327287B2 (ja) | 1999-01-29 | 2009-09-09 | 大陽日酸株式会社 | 重酸素水の製造方法および装置 |
JP4309162B2 (ja) | 2002-12-04 | 2009-08-05 | パナソニックエコシステムズ株式会社 | 一酸化炭素除去ユニット、一酸化炭素除去方法、空気清浄装置および一酸化炭素除去触媒組成物 |
CN201493052U (zh) * | 2009-08-13 | 2010-06-02 | 上海化工研究院 | 一种间歇生产超轻水的同位素分离装置 |
JP2019513556A (ja) * | 2016-04-08 | 2019-05-30 | アクツィオネルノエ オブシチェストヴォ “ラディエヴィ インスティテュート イメニ ヴェーゲー フローピナ” | 酸素18を富化した水を得る方法、およびその製造のための設備 |
JP2018164884A (ja) | 2017-03-28 | 2018-10-25 | 大陽日酸株式会社 | 一酸化炭素安定同位体濃縮装置および一酸化炭素安定同位体濃縮方法 |
Non-Patent Citations (2)
Title |
---|
"Gas Diorama 2020", 2020, GAS REVIEW CO., LTD, pages: 88 |
SHOHEI ISOMURAYASUHIKO TONOOKAHAYATO KAETSU: "Separation of Nitrogen and Oxygen Isotopes by Nitric Oxide Low Temperature Distillation", JAPAN RADIOISOTOPE ASSOCIATION, vol. 36, no. 2, 15 February 1987 (1987-02-15), pages 57 - 63 |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20220282913A1 (en) * | 2021-03-05 | 2022-09-08 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Purification of carbon monoxide by cryogenic distillation |
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