Apparatus, system and method for preparing isotope-labeled carbon dioxide

Abstract

To provide an apparatus system and a method for preparing isotope-labeled carbon dioxide.SOLUTION: A preparation method includes vaporizing heavy oxygen water and then mixing the vaporized heavy oxygen water with carbon dioxide, catalyzing the mixture with a catalyst material, subjecting the heavy oxygen water and the carbon dioxide to oxygen substitution reaction, performing gas-liquid separation after reaction, and obtaining isotope-labeled carbon dioxide. An apparatus system has a simple structure, uses heavy oxygen water which is widely derived and inexpensive as an oxygen isotope source, achieves substitution oxygen-16 of general carbon dioxide with oxygen-18 of heavy oxygen water, obtains an oxygen-18 isotope-labeled carbon dioxide product, has a simple process, is green and has no contamination, has a high utilization rate of an oxygen isotope, has a mild separation purification condition, and has good economy benefits and prospective application.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present invention relates to the technical field of carbon dioxide preparation, and specifically to an apparatus system and method for preparing isotope-labeled carbon dioxide. [Background technology]

[0002] Under the trend toward "carbon peaking and carbon neutrality," scientific research related to the capture, conversion, and utilization of carbon dioxide has become a recognized research hotspot. In the carbon dioxide conversion reaction process, isotope tracing tests are an important tool for investigating CO2 conversion routes and reaction mechanisms, and oxygen-isotope-labeled carbon dioxide is the primary material for isotope testing. However, the preparation, separation, and purification processes of oxygen-isotope-labeled carbon dioxide are complicated, and the cost is extremely high, limiting the use of oxygen-isotope-labeled carbon dioxide in related research fields.

[0003] CN114436260A discloses an apparatus and method for preparing oxygen-isotope-labeled carbon monoxide and carbon dioxide, which involves heating oxygen-isotope-labeled oxalic acid in a reactor to decompose it, yielding oxygen-isotope-labeled CO2, CO, and HO. The oxygen-isotope-labeled CO2, CO, and HO are then collected at different temperatures using a recovery bolt and a refrigeration device. This method features a simple and efficient preparation process and product separation and purification process, a high oxygen isotope utilization rate, and a carbon dioxide product with an O-18 abundance of over 95%. However, this method relies on oxygen-isotope-labeled oxalic acid as the isotope source, which is expensive and requires harsh separation and purification conditions, requiring a refrigeration temperature of -100°C or below.

[0004] Therefore, the development of a simple, green, efficient, and low-cost apparatus system and method for preparing oxygen-18 isotope-labeled carbon dioxide is of great significance to meet the needs for its use in related research fields. Summary of the Invention [Problem to be solved by the invention]

[0005] The present invention aims to provide an apparatus system and method for preparing isotope-labeled carbon dioxide, which has a wide range of raw material sources, low cost, mild preparation conditions, a simple process, and good economic benefits and application prospects. [Means for solving the problem]

[0006] In order to achieve the object of the present invention, the present invention provides the following technical solutions.

[0007] In a first aspect, the present invention provides an apparatus system for preparing isotope-labeled carbon dioxide, the apparatus system comprising a preparation unit, a heavy oxygen water feedstock storage device, a carbon dioxide feedstock storage device, a product storage device, and a heavy oxygen water recovery and storage device; The preparation unit includes a heating vaporizer, an oxygen substitution reaction device provided with a catalytic material, and a gas-liquid separator, which are connected in series; The inlets of the heating vaporizer are respectively connected to a heavy oxygen water raw material storage device and a carbon dioxide raw material storage device; The gas-liquid separator has a gas-phase outlet connected to a product storage device, and a liquid-phase outlet connected to a heavy oxygen water recovery and storage device.

[0008] The apparatus system of the present invention uses deuterated oxygen water, which has a simple structure, is widely available, and is inexpensive, as an oxygen isotope source. Through oxygen substitution, the oxygen-18 in deuterated oxygen water is substituted for the oxygen-16 in ordinary carbon dioxide, thereby obtaining an oxygen-18 isotope-labeled carbon dioxide product. The process is simple, green, and pollution-free, with a high oxygen isotope utilization rate and mild separation and purification conditions, and has good economic benefits and application prospects.

[0009] Preferably, the equipment system comprises at least one preparation unit.

[0010] The equipment system of the present invention can flexibly configure the preparation units according to the purity requirements of the products, which is convenient to configure and can meet the needs of different products.

[0011] Preferably, when the equipment system includes two or more preparation units, the inlet of the heating vaporizer of the subsequent preparation unit is connected to the heavy oxygen water raw material storage device and the gas phase outlet of the gas-liquid separator of the previous preparation unit along the flow direction of the material in the equipment system.

[0012] Preferably, when the equipment system includes two or more preparation units, a heat exchange device is further provided between two adjacent preparation units; According to the flow direction of the material in the equipment system, the heat medium inlet of the heat exchanger is connected to the outlet of the oxygen substitution reaction device of the subsequent preparation unit; The refrigerant inlet of the heat exchanger is connected to the gas phase outlet of the gas-liquid separator of the previous preparation unit; The heat medium outlet of the heat exchanger is connected to the inlet of the gas-liquid separator of the subsequent preparation unit; The refrigerant outlet of the heat exchanger is connected to the inlet of the heating vaporizer of the subsequent preparation unit.

[0013] Preferably, the catalytic material comprises a combination of one or at least two of γ-Al2O3, CeO2, or anatase titanium dioxide. Typical combinations include, but are not limited to, a combination of γ-Al2O3 and CeO2, a combination of CeO2 and anatase titanium dioxide, a combination of γ-Al2O3 and anatase titanium dioxide, or a combination of γ-Al2O3, CeO2, and anatase titanium dioxide.

[0014] In a second aspect, the present invention provides a method for preparing isotope-labeled carbon dioxide using the apparatus system described in the first aspect.

[0015] Preferably, the preparation method comprises: Step (1) of vaporizing heavy oxygen water and then mixing it with carbon dioxide to obtain a mixed gas; The mixed gas obtained in step (1) is catalyzed by a catalyst material, and the heavy oxygen water and carbon dioxide are subjected to an oxygen substitution reaction, and the carbon dioxide 16 O in deoxygenated water 18 O is substituted to generate isotopically labeled carbon dioxide in deoxygenated water. 18 O 16 Step (2) in which O is substituted; and (3) liquefying the post-reaction heavy oxygen water and separating the post-reaction carbon dioxide into gas and liquid to obtain isotope-labeled carbon dioxide.

[0016] Preferably, the molar ratio of heavy oxygen water to carbon dioxide in step (1) is (2-5):1, and may be, for example, 2:1, 2.5:1, 3:1, 3.5:1, 4:1, 4.5:1, or 5:1, but is not limited to the recited values, and other unrecited values ​​within the range of values ​​also apply.

[0017] Preferably, the vaporization temperature in step (1) is 100 to 300°C, and may be, for example, 100°C, 120°C, 140°C, 150°C, 160°C, 180°C, 200°C, 220°C, 240°C, 250°C, 260°C, 280°C, or 300°C, but is not limited to the listed values, and other unlisted values ​​within the range of values ​​also apply.

[0018] Preferably, the volumetric space velocity of the oxygen substitution reaction described in step (2) is 5,000 to 100,000 h -1 For example, 5000h -1 , 10000h -1 , 15000h -1 , 20000h -1 , 30000h -1 , 40000h -1 , 500000h -1 , 60000h -1 , 70000h -1 , 80000h -1 , 90000h -1 or 100000h -1However, the present invention is not limited to the numerical values ​​listed above, and other unlisted numerical values ​​within the numerical range also apply.

[0019] Preferably, the liquefaction temperature in step (3) is between -10°C and 20°C, and may be, for example, -10°C, -5°C, 0°C, 5°C, 10°C, 15°C or 20°C, but is not limited to the listed values, and other unlisted values ​​within the range of values ​​also apply. [Effects of the Invention]

[0020] Compared with the prior art, the present invention has the following beneficial effects:

[0021] The apparatus system of the present invention uses deuterated oxygen water, which has a simple structure, is widely available, and is inexpensive, as an oxygen isotope source. Through oxygen substitution, the oxygen-18 in deuterated oxygen water is substituted for the oxygen-16 in ordinary carbon dioxide, thereby obtaining an oxygen-18 isotope-labeled carbon dioxide product. The process is simple, green, and pollution-free, with a high oxygen isotope utilization rate and mild separation and purification conditions, and has good economic benefits and application prospects. [Brief explanation of the drawings]

[0022] [Figure 1] FIG. 1 is a diagram showing an apparatus system for preparing isotope-labeled carbon dioxide according to Example 1. DETAILED DESCRIPTION OF THE INVENTION

[0023] The following will further illustrate the technical solutions of the present invention through specific embodiments. Those skilled in the art will appreciate that the above examples are merely intended to help understand the present invention and should not be construed as limiting the present invention in any way.

[0024] Example 1 This embodiment provides an equipment system for preparing isotope-labeled carbon dioxide, as shown in Figure 1. The equipment system includes a first-stage preparation unit, a second-stage preparation unit, a third-stage preparation unit, a heavy oxygen water raw material storage device 1, a carbon dioxide raw material storage device 2, a product storage device 15, a heavy oxygen water recovery and storage device 16, a heat exchanger 9, and a heat exchanger 13.

[0025] The first-stage preparation unit includes a first-stage heating vaporizer 3, a first-stage oxygen substitution reaction apparatus 4, and a first-stage gas-liquid separator 6, which are connected in sequence.

[0026] The two-stage preparation unit includes a two-stage heating vaporizer 7, a two-stage oxygen displacement reaction apparatus 8, and a two-stage gas-liquid separator 10, and the two-stage heating vaporizer 7 and the two-stage oxygen displacement reaction apparatus 8 are connected to each other.

[0027] The three-stage preparation unit includes a three-stage heating vaporizer 11, a three-stage oxygen substitution reaction apparatus 12, and a three-stage gas-liquid separator 14, and the three-stage heating vaporizer 11 and the three-stage oxygen substitution reaction apparatus 12 are connected to each other.

[0028] The first-stage oxygen displacement reactor 4, the second-stage oxygen displacement reactor 8 and the third-stage oxygen displacement reactor 12 are all provided with a catalyst material 5 which is γ-Al 2 O 3 .

[0029] The heavy oxygen water raw material storage device 1 is connected to a first-stage heating vaporizer 3, a second-stage heating vaporizer 7, and a third-stage heating vaporizer 11, respectively.

[0030] The carbon dioxide raw material storage device 2 and the first-stage heating vaporization device 3 are connected together.

[0031] The refrigerant inlet of the heat exchanger 9 is connected to the gas phase outlet of the first-stage gas-liquid separator 6. The heat medium inlet of the heat exchanger 9 is connected to the two-stage oxygen substitution reactor 8. The heat medium outlet of the heat exchanger 9 is connected to the two-stage gas-liquid separator 10. The refrigerant outlet of the heat exchanger 9 is connected to the two-stage heating vaporizer 7.

[0032] The refrigerant inlet of the heat exchanger 13 is connected to the gas phase outlet of the two-stage gas-liquid separation device 10. The heat medium inlet of the heat exchanger 13 is connected to the three-stage oxygen substitution reaction device 12. The heat medium outlet of the heat exchanger 13 is connected to the three-stage gas-liquid separation device 14. The refrigerant outlet of the heat exchanger 13 is connected to the three-stage heating vaporization device 11.

[0033] The product storage device 15 is connected to the vapor phase outlet of the three-stage vapor-liquid separator 14 .

[0034] The heavy oxygen water recovery and storage device 16 is connected to the liquid phase outlets of the first stage gas-liquid separator 6, the second stage gas-liquid separator 10 and the third stage gas-liquid separator 14, respectively.

[0035] Example 2 This embodiment provides an apparatus system for preparing isotope-labeled carbon dioxide, which includes a first-stage preparation unit, a second-stage preparation unit, a heavy oxygen water raw material storage device 1, a carbon dioxide raw material storage device 2, a product storage device 15, a heavy oxygen water recovery and storage device 16, and a heat exchange device 9.

[0036] The first-stage preparation unit includes a first-stage heating vaporizer 3, a first-stage oxygen substitution reaction apparatus 4, and a first-stage gas-liquid separator 6, which are connected in sequence.

[0037] The two-stage preparation unit includes a two-stage heating vaporizer 7, a two-stage oxygen displacement reaction apparatus 8, and a two-stage gas-liquid separator 10, and the two-stage heating vaporizer 7 and the two-stage oxygen displacement reaction apparatus 8 are connected to each other.

[0038] In both the first-stage oxygen displacement reactor 4 and the second-stage oxygen displacement reactor 8, a catalyst material 5 made of γ-Al 2 O 3 is provided.

[0039] The heavy oxygen water raw material storage device 1 is connected to the first-stage heating vaporizer 3 and the second-stage heating vaporizer 7, respectively.

[0040] The carbon dioxide raw material storage device 2 and the first-stage heating vaporization device 3 are connected together.

[0041] The refrigerant inlet of the heat exchanger 9 is connected to the gas phase outlet of the first-stage gas-liquid separator 6. The heat medium inlet of the heat exchanger 9 is connected to the two-stage oxygen substitution reactor 8. The heat medium outlet of the heat exchanger 9 is connected to the two-stage gas-liquid separator 10. The refrigerant outlet of the heat exchanger 9 is connected to the two-stage heating vaporizer 7.

[0042] The product storage device 15 is connected to the vapor phase outlet of the two-stage vapor-liquid separator 10 .

[0043] The heavy oxygen water recovery and storage device 16 is connected to the liquid phase outlets of the first-stage gas-liquid separator 6 and the second-stage gas-liquid separator 10, respectively.

[0044] Usage example 1 This use example provides a method for preparing isotope-labeled carbon dioxide, which uses the device system according to Example 1 and includes the following steps:

[0045] (1) Deoxygenated water (H2 18 The gaseous heavy oxygen water and the carbon dioxide are mixed in a molar ratio of 3:1, and the temperature of the mixed gas at the outlet of the first-stage heated vaporizer 3 is 120°C.

[0046] (2) Mixed gas H2 18 O and CO were introduced into the first-stage oxygen substitution reactor 4 (the reaction temperature of the first-stage oxygen substitution reactor 4 was 110°C, and the volumetric space velocity was 10,000 h -1 Under the action of the catalytic material γ-Al2O3, H2 18 O is decomposed and reacts with CO2 adsorbed on the material to replace oxygen. 16 O is H2 18 In O 18 O is replaced by oxygen-18 isotope-labeled carbon dioxide (C 18 O 16 O, C 18 O 18O) and H2 18 In O 18 O 16 O is replaced by H2 16 O was produced.

[0047] (3) The gas that has undergone the oxygen substitution reaction is cooled in the gas-liquid separator 6 (the cooling temperature is −3° C.), and the separated liquid water (H 18 O and H2 16 O) into the heavy oxygen water recovery and storage device 16, and separated gaseous carbon dioxide (C 16 O 16 O, C 18 O 16 O, C 18 O 18 0) was heated to 80°C in the heat exchanger 9.

[0048] (4) The gas phase carbon dioxide (C 16 O 16 O, C 18 O 16 O, C 18 O 18 The oxygen-containing water and the heavy oxygen water further pass through a two-stage preparation unit and a three-stage preparation unit, respectively, and undergo the vaporization, oxygen substitution reaction, and gas-liquid separation processes similar to steps (1) to (3), and the resulting isotope-labeled carbon dioxide product enters product storage device 15.

[0049] In this embodiment, C in CO at the gas phase outlet of the first-stage gas-liquid separator 6 18 O 18 The ratio of O to CO2 at the gas phase outlet of the two-stage gas-liquid separator 10 is 52%. 18 O 18 The ratio of O to CO2 at the gas phase outlet of the three-stage gas-liquid separator 14 is 84%. 18 O 18 The proportion of O is 98%.

[0050] Usage example 2 This use example provides a method for preparing isotope-labeled carbon dioxide, which uses the device system according to Example 1 and includes the following steps:

[0051] (1) Deoxygenated water (H2 18 The gaseous heavy oxygen water and the carbon dioxide are mixed in a molar ratio of 2:1, and the temperature of the mixed gas at the outlet of the first-stage heated vaporizer 3 is 100°C.

[0052] (2) Mixed gas H2 18 O and CO were introduced into the first-stage oxygen substitution reactor 4 (the reaction temperature of the first-stage oxygen substitution reactor 4 was 110°C and the volumetric space velocity was 5000 h -1 Under the action of the catalytic material γ-Al2O3, H2 18 O is decomposed and reacts with CO2 adsorbed on the material to replace oxygen. 16 O is H2 18 In O 18 O is replaced by oxygen-18 isotope-labeled carbon dioxide (C 18 O 16 O, C 18 O 18 O) and H2 18 In O 18 O 16 O is replaced by H2 16 O was produced.

[0053] (3) The gas that has undergone the oxygen substitution reaction is cooled in the gas-liquid separator 6 (the cooling temperature is −10° C.), and the separated liquid water (H 18 O and H2 16 O) into the heavy oxygen water recovery and storage device 16, and separated gaseous carbon dioxide (C 16 O 16 O, C 18 O 16 O, C 18 O 18 0) was heated to 80°C in the heat exchanger 9.

[0054] (4) The gas phase carbon dioxide (C 16 O 16 O, C 18 O 16 O, C18 O 18 The oxygen-containing water and the heavy oxygen water further pass through a two-stage preparation unit and a three-stage preparation unit, respectively, and undergo the vaporization, oxygen substitution reaction, and gas-liquid separation processes similar to steps (1) to (3), and the resulting isotope-labeled carbon dioxide product enters product storage device 15.

[0055] In this embodiment, C in CO at the gas phase outlet of the first-stage gas-liquid separator 6 18 O 18 The ratio of O to CO2 at the gas phase outlet of the two-stage gas-liquid separator 10 is 45%. 18 O 18 The ratio of O was 72%, and the C in CO2 at the gas phase outlet of the three-stage gas-liquid separator 14 18 O 18 The proportion of O is 88%.

[0056] Usage example 3 This use example provides a method for preparing isotope-labeled carbon dioxide, which uses the device system according to Example 1 and includes the following steps:

[0057] (1) Deoxygenated water (H2 18 The gaseous heavy oxygen water and the carbon dioxide are mixed in a molar ratio of 5:1 between the heavy oxygen water and the carbon dioxide, and the temperature of the mixed gas at the outlet of the first-stage heated vaporizer 3 is 300°C.

[0058] (2) Mixed gas H2 18 O and CO were introduced into the first-stage oxygen substitution reactor 4 (the reaction temperature of the first-stage oxygen substitution reactor 4 was 110°C, and the volumetric space velocity was 100,000 h -1 Under the action of the catalytic material γ-Al2O3, H2 18 O is decomposed and reacts with CO2 adsorbed on the material to replace oxygen. 16 O is H2 18 In O 18 O is replaced by oxygen-18 isotope-labeled carbon dioxide (C 18 O16 O, C 18 O 18 O) and H2 18 In O 18 O 16 O is replaced by H2 16 O was produced.

[0059] (3) The gas that has undergone the oxygen substitution reaction is cooled in the gas-liquid separator 6 (the cooling temperature is 20°C), and the separated liquid water (H 18 O and H2 16 O) into the heavy oxygen water recovery and storage device 16, and separated gaseous carbon dioxide (C 16 O 16 O, C 18 O 16 O, C 18 O 18 0) was heated to 80°C in the heat exchanger 9.

[0060] (4) The gas phase carbon dioxide (C 16 O 16 O, C 18 O 16 O, C 18 O 18 The oxygen-containing water and the heavy oxygen water further pass through a two-stage preparation unit and a three-stage preparation unit, respectively, and undergo the vaporization, oxygen substitution reaction, and gas-liquid separation processes similar to steps (1) to (3), and the resulting isotope-labeled carbon dioxide product enters product storage device 15.

[0061] In this embodiment, C in CO at the gas phase outlet of the first-stage gas-liquid separator 6 18 O 18 The ratio of O to CO2 at the gas phase outlet of the two-stage gas-liquid separator 10 is 64%. 18 O 18 The ratio of O to CO2 at the gas phase outlet of the three-stage gas-liquid separator 14 is 87%. 18 O 18 The O ratio is 99%.

[0062] Usage example 4 This example provides a method for preparing isotope-labeled carbon dioxide. The method is the same as in Example 1, except that the molar ratios of heavy oxygen water to carbon dioxide in the first-stage heated vaporizer 3, the second-stage heated vaporizer 7, and the third-stage heated vaporizer 8 are 2:1, 3:1, and 4:1, respectively.

[0063] In this example, the C in CO2 at the gas phase outlet of the first-stage gas-liquid separator 6 18 O 18 The ratio of O is 40%, and the C in CO2 at the gas phase outlet of the two-stage gas-liquid separator 10 18 O 18 The ratio of O is 75%, and the C in CO2 at the gas phase outlet of the three-stage gas-liquid separator 14 18 O 18 The proportion of O is 96%.

[0064] Usage example 5 This example provides a method for preparing isotope-labeled carbon dioxide. The method uses the apparatus system of Example 1, but the catalyst materials in the first-stage oxygen substitution reactor 4, the second-stage oxygen substitution reactor 8, and the third-stage oxygen substitution reactor 12 are replaced with CeO2 in equal amounts compared to Example 1.

[0065] In this example, the C in CO2 at the gas phase outlet of the first-stage gas-liquid separator 6 18 O 18 The ratio of O to CO2 at the gas phase outlet of the two-stage gas-liquid separator 10 is 50%. 18 O 18 The ratio of O to CO2 at the gas phase outlet of the three-stage gas-liquid separator 14 is 82%. 18 O 18 The proportion of O is 95%.

[0066] Usage example 6 This example provides a method for preparing isotope-labeled carbon dioxide. The method uses the apparatus system of Example 1, but the catalyst materials in the first-stage oxygen substitution reactor 4, the second-stage oxygen substitution reactor 8, and the third-stage oxygen substitution reactor 12 are replaced with anatase titanium dioxide in equal amounts compared to Example 1.

[0067] In this example, the C in CO2 at the gas phase outlet of the first-stage gas-liquid separator 6 18 O 18 The ratio of O to CO2 at the gas phase outlet of the two-stage gas-liquid separator 10 is 48%. 18 O 18 The ratio of O was 78%, and the C in CO2 at the gas phase outlet of the three-stage gas-liquid separator 14 18 O 18 The proportion of O is 90%.

[0068] Comparative use case 1 This example provides a method for preparing isotope-labeled carbon dioxide. The method uses the apparatus system of Example 1, but unlike Example 1, the first-stage oxygen substitution reactor 4, the second-stage oxygen substitution reactor 8, and the third-stage oxygen substitution reactor 12 do not include catalytic materials.

[0069] In this comparative example, the oxygen substitution reaction device does not contain a catalyst material, so the oxygen substitution reaction between heavy oxygen water and CO2 cannot occur, and the oxygen in CO2 is not substituted with O-18. [Table 1]

[0070] As can be seen from Table 1, the apparatus system and method according to the present invention can realize the preparation of isotope-labeled carbon dioxide by oxygen substitution with deuterated water, and the C 18 The O2 concentration reaches 72% or more, and after three-stage oxygen substitution, the concentration can be increased to 88% or more, resulting in high reaction efficiency, high preparation purity, and high utilization rate of the heavy oxygen water, the reaction raw material. After the reaction, the heavy oxygen water can be collected in a storage device and reused.

[0071] In summary, the apparatus system of the present invention uses heavy oxygen water, which has a simple structure, is widely available, and is inexpensive, as an oxygen isotope source, and through oxygen substitution, replaces the oxygen-16 in ordinary carbon dioxide with the oxygen-18 from heavy oxygen water to obtain an oxygen-18 isotope-labeled carbon dioxide product. The process is simple, green, and pollution-free, with a high oxygen isotope utilization rate and mild separation and purification conditions, and has good economic benefits and application prospects.

[0072] The applicant declares that the above is only a specific embodiment of the present invention, and the protection scope of the present invention is not limited thereto. It should be understood that any changes or substitutions that can be easily thought up by those skilled in the art within the technical scope disclosed in the present invention are all within the protection scope and disclosure scope of the present invention. [Explanation of symbols]

[0073] 1: Heavy oxygen water raw material storage device; 2: Carbon dioxide raw material storage device; 3: One-stage heating vaporization device; 4: One-stage oxygen substitution reaction device; 5: Catalyst material; 6: One-stage gas-liquid separation device; 7: Two-stage heating vaporization device; 8: Two-stage oxygen substitution reaction device; 9: Heat exchanger; 10: Two-stage gas-liquid separation device; 11: Three-stage heating vaporization device; 12: Three-stage oxygen substitution reaction device; 13: Heat exchanger; 14: Three-stage gas-liquid separation device; 15: Product storage device; 16: Heavy oxygen water recovery and storage device.

Claims

1. 1. An apparatus system for preparing isotope-labeled carbon dioxide, comprising: The equipment system includes a preparation unit, a heavy oxygen water raw material storage device, a carbon dioxide raw material storage device, a product storage device, and a heavy oxygen water recovery storage device; The preparation unit includes a heating vaporizer, an oxygen substitution reaction device provided with a catalytic material, and a gas-liquid separator, which are connected in series; The inlets of the heating vaporizer are respectively connected to a heavy oxygen water raw material storage device and a carbon dioxide raw material storage device; The gas-liquid separator has a gas-phase outlet connected to a product storage device, and a liquid-phase outlet connected to a heavy oxygen water recovery and storage device.

2. The equipment system of claim 1 , wherein the equipment system includes at least one preparation unit.

3. The equipment system according to claim 2, characterized in that when the equipment system includes two or more preparation units, the inlet of the heating vaporizer of the subsequent preparation unit is connected to the heavy oxygen water raw material storage device and the gas phase outlet of the gas-liquid separator of the previous preparation unit along the flow direction of the material within the equipment system.

4. When the equipment system includes two or more preparation units, a heat exchange device is further provided between two adjacent preparation units; According to the flow direction of the material in the equipment system, the heat medium inlet of the heat exchanger is connected to the outlet of the oxygen substitution reaction device of the subsequent preparation unit; The refrigerant inlet of the heat exchanger is connected to the gas phase outlet of the gas-liquid separator of the previous preparation unit; The heat medium outlet of the heat exchanger is connected to the inlet of the gas-liquid separator of the subsequent preparation unit; 3. The system according to claim 2, wherein the refrigerant outlet of the heat exchanger is connected to the inlet of a heating vaporizer of a subsequent preparation unit.

5. The catalytic material is γ-Al ２ O ３ , CeO ２ or anatase type titanium dioxide, or a combination of at least two of them.

6. 1. A method for preparing isotope-labeled carbon dioxide, comprising: The preparation method is characterized in that the preparation method uses the apparatus system according to any one of claims 1 to 5.

7. The preparation method comprises: Step (1) of vaporizing heavy oxygen water and then mixing it with carbon dioxide to obtain a mixed gas; The mixed gas obtained in step (1) is catalyzed with a catalyst material to cause an oxygen substitution reaction between heavy oxygen water and carbon dioxide, and １６ O in deoxygenated water １８ O to generate isotope-labeled carbon dioxide, １８ O １６ Step (2) of replacing with O; The method according to claim 6, further comprising the step (3) of liquefying the heavy oxygen water after the reaction and separating the heavy oxygen water from the carbon dioxide after the reaction into gas and liquid to obtain isotope-labeled carbon dioxide.

8. 8. The method according to claim 7, wherein the molar ratio of heavy oxygen water to carbon dioxide in step (1) is (2-5):

1.

9. The preparation method according to claim 7, characterized in that the temperature of vaporization in step (1) is 100-300°C.

10. The volumetric space velocity of the oxygen substitution reaction described in step (2) is 5,000 to 100,000 h －１ and The preparation method according to claim 7, characterized in that the temperature of liquefaction in step (3) is -10°C to 20°C.

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