Gas separation method and gas separation device

Abstract

The present invention aims to provide a gas separation method and a gas separation device that can stabilize the purity and recovery rate of separated rare gas while recycling exhaust gas from a rare gas using device. The gas separation method is characterized by introducing a rare gas separated by pressure adsorption as a first introduction gas and an impurity gas separated by pressure adsorption as a second introduction gas into a raw material gas, and controlling the flow rate of the first introduction gas and the flow rate of the second introduction gas according to the flow rate of each of the rare gas and the impurity gas in the exhaust gas from the rare gas using device (20). The gas separation device (1) includes an introduction pipe (L6) that introduces a rare gas in a separation gas container (6) into a raw material gas, an introduction pipe (L7) that introduces an impurity gas in a separation gas container (7) into the raw material gas, a flow meter (2) provided in a supply pipe (L1) that supplies the exhaust gas to the rare gas using device (20), and a calculation device (12) that is electrically connected to the flow meter (2), a flow rate controller (8), and a flow rate controller (9).

Description

Technical Field

[0001] This invention relates to a gas separation method and a gas separation apparatus. Background Technology

[0002] High-value-added gases such as krypton and xenon are used in industrial fields and equipment that generate plasma through high-frequency discharge. As a method for purifying these high-value-added gases, a gas separation method is known to separate a first gas component and a second gas component from a raw gas containing multiple gas components by pressure adsorption (Patent Document 1).

[0003] Patent document 1 proposes a scheme for separating and purifying krypton, xenon, etc. by combining equilibrium pressure swing adsorption (PSA) separation method and velocity pressure swing adsorption (PSA) separation method.

[0004] Patent Document 1: Japanese Patent Application Publication No. 2002-126435

[0005] Rare gases are high-value-added gases, therefore, from an economic perspective, the reuse of exhaust gases containing rare gases from rare gas utilization equipment is very important. However, the concentration of each gas component in the exhaust gas from rare gas utilization equipment can vary greatly depending on the operating conditions of the equipment.

[0006] Although Patent Document 1 combines different adsorption separation methods to achieve both the removal of components other than rare gases from the raw material gas (high purity of rare gases) and the removal of rare gases (high purity of components other than rare gases), the following problems will occur if the concentration of each component in the exhaust gas from the rare gas using equipment changes.

[0007] When the proportion of rare gas components in the exhaust gas decreases while the proportion of other gas components increases, the concentration of gas components to be adsorbed and removed by the adsorbent used for adsorption separation (which should remove other gas components) relatively increases. Therefore, the pressure inside the adsorption tower decreases, and it becomes insufficient to remove other gas components. As a result, the purity of the separated rare gas decreases.

[0008] When the proportion of rare gas components in the exhaust gas increases while the proportion of other gas components decreases, the concentration of rare gas components to be adsorbed and removed by the adsorbent used for adsorption separation of rare gas components relatively increases. Therefore, the pressure inside the adsorption tower decreases, and it becomes impossible to sufficiently remove rare gas components. As a result, the purity of the components other than rare gases after separation decreases, i.e., the recovery rate of rare gases decreases.

[0009] As a countermeasure to the aforementioned problems, a method of changing the separation conditions of the adsorption tower according to the changes in the composition of the discharged gas has been considered. However, the control of the separation conditions of the adsorption tower involves frequency conversion control of the compressor's discharge flow rate and changes in the switching time between the adsorption and regeneration processes. Furthermore, by changing the switching time, the time point or amount at which the mixed gas of each gas component discharged in the regeneration process of the adsorption tower returns to the feed gas, as is characteristic of Patent Document 1, changes. As a result, the composition of the feed gas changes further, leading to a very complex control burden.

[0010] As explained above, in conventional gas separation methods, it is difficult to consistently improve both the purity and recovery rate of the separated rare gases if the exhaust gas from the equipment is to be reused. Summary of the Invention

[0011] This invention provides a gas separation method and a gas separation device that can recycle the exhaust gas from rare gas-using equipment while steadily improving both the purity and recovery rate of the separated rare gas.

[0012] To address the aforementioned problems, the present invention provides the following gas separation method and gas separation apparatus.

[0013] [1] A gas separation method, comprising separating a first gas component and a second gas component from a raw material gas containing multiple gas components by pressure adsorption, characterized in that the first gas component after separation from the raw material gas is introduced into the raw material gas as a first inlet gas, and the second gas component after separation from the raw material gas is introduced into the raw material gas as a second inlet gas, wherein the flow rate V of the first inlet gas is controlled based on the flow rates of the first gas component and the second gas component in the exhaust gas discharged from the rare gas application device. R1 and the flow rate V of the second introduced gas R2 .

[0014] [2] According to the gas separation method described in [1], the following gas flow rates and S1 and the following gas flow rates and S2 are further controlled to specified values,

[0015] Gas flow rate and S1 are the flow rates V of the first gas component in the discharged gas. F1 With the flow rate V of the first introduced gas R1 The total value,

[0016] Gas flow rate and S2 are the flow rates V of the second gas component in the discharged gas. F2With the flow rate V of the second introduced gas R2 The total value.

[0017] [3] According to the gas separation method described in [1] or [2], wherein the first gas component is krypton or xenon.

[0018] [4] The gas separation method according to any one of [1] to [3], wherein the second gas component comprises at least one selected from hydrogen, nitrogen, oxygen, helium, neon and argon.

[0019] [5] According to the gas separation method described in [1], wherein,

[0020] The exhaust gas discharged from the rare gas application device also contains a third gas component.

[0021] After the first gas component separated from the raw material gas is introduced into the raw material gas as a first introducing gas, and the second gas component separated from the raw material gas is introduced into the raw material gas as a second introducing gas, the third gas component is removed from the raw material gas.

[0022] [6] According to the gas separation method described in [5], the third gas component is an organic compound.

[0023] [7] A gas separation apparatus includes: a separation section for separating a first gas component and a second gas component from a raw gas containing multiple gas components by pressure adsorption; a raw gas container for storing the raw gas; a first supply pipe for supplying exhaust gas discharged from a rare gas application device to the raw gas container; a second supply pipe for connecting the raw gas container and the separation section; a first separation gas container for storing the first gas component separated by the separation section; a second separation gas container for storing the second gas component separated by the separation section; a first inlet pipe for introducing the first gas component in the first separation gas container as a first inlet gas into the raw gas; a second inlet pipe for introducing the second gas component in the second separation gas container as a second inlet gas into the raw gas; a first flow controller disposed on the first inlet pipe; a second flow controller disposed on the second inlet pipe; a flow information acquisition device for acquiring information on the flow rates of the first gas component and the second gas component flowing in the first supply pipe; and a computing device electrically connected to the first flow controller, the second flow controller, and the flow information acquisition device, respectively.

[0024] [8] According to the gas separation apparatus of [7], wherein the flow information acquisition device comprises at least one selected from the following: a flow meter disposed on the first supply pipe; a concentration meter disposed on the first supply pipe for measuring the concentration of a first gas component; a concentration meter disposed on the first supply pipe for measuring the concentration of a second gas component; a receiver electrically receiving flow information of the first gas component discharged from the rare gas using device; and a receiver electrically receiving flow information of the second gas component used in the rare gas using device.

[0025] [9] According to the gas separation device of [7] or [8], a first concentration meter for measuring the concentration of a first gas component in the first inlet pipe is further provided in the first inlet pipe, and the first concentration meter is also electrically connected to the computing device.

[0026]

[10] The gas separation device according to any one of [7] to [9], wherein a second concentration meter for measuring the concentration of a second gas component in the second inlet pipe is further provided in the second inlet pipe, and the second concentration meter is also electrically connected to the computing device.

[0027]

[11] The gas separation device according to any one of [7] to

[10] , wherein the first gas component is krypton or xenon.

[0028]

[12] The gas separation apparatus according to any one of [7] to

[11] , wherein the second gas component comprises at least one selected from hydrogen, nitrogen, oxygen, helium, neon and argon.

[0029]

[13] According to the gas separation device of [9], the exhaust gas discharged from the rare gas using device further contains a third gas component.

[0030] A third gas removal device for removing third gas components is further provided downstream of the first concentration meter in the first supply pipe.

[0031] The first inlet pipe and the second inlet pipe are connected to the first supply pipe between the first concentration meter and the third gas removal device.

[0032]

[14] According to the gas separation device of

[13] , the third gas component is an organic compound.

[0033] According to the present invention, the purity and recovery rate of the separated rare gas can be steadily improved while reusing the exhaust gas from the rare gas utilization equipment. Attached Figure Description

[0034] Figure 1 This is a schematic diagram illustrating the gas separation apparatus and the rare gas usage equipment using rare gases according to the first embodiment.

[0035] Figure 2 For illustrative purposes Figure 1 A schematic diagram of the separation section of a gas separation device.

[0036] Figure 3 This is a schematic diagram illustrating the gas separation apparatus and the rare gas usage device using rare gases according to the second embodiment. Detailed Implementation

[0037] The following is a reference to the appendix. Figure 1 One embodiment will be described in detail below. For ease of understanding, the parts that are features are sometimes enlarged in the drawings used in the following description for convenience, and the size ratios of each component are not limited to the actual dimensions.

[0038] In this specification, the "~" indicating a numerical range means that the values ​​before and after it are included as the lower limit and upper limit.

[0039] First Implementation Method

[0040] <Gas Separation Device>

[0041] The following is for reference Figure 1 , 2 The gas separation apparatus involved in this embodiment will be described.

[0042] Figure 1 This is a schematic diagram showing the gas separation device 1 and the rare gas usage device 20 that uses rare gases according to this embodiment. Figure 2 This is a schematic diagram illustrating the structure of the separation section 5.

[0043] Gas separation device 1 is a device that separates a first gas component and a second gas component from a raw material gas by pressure adsorption. The raw material gas includes the exhaust gas discharged from the rare gas application device 20.

[0044] The gas separation device 1 includes: a first supply pipe L1, a flow meter 2, a concentration meter 13, a raw material gas container 3, a supply source 15 for a first gas component, a second supply pipe L2, a compressor 4, a separation section 5, a return pipe L3, a first separation pipe L4, a second separation pipe L5, a first separated gas container 6, a first inlet pipe L6, a second separated gas container 7, a second inlet pipe L7, a first flow controller 8, a second flow controller 9, a first outlet pipe L8, a second outlet pipe L9, a third flow controller 10, a fourth flow controller 11, a processing unit 12, and a receiver 14.

[0045] The rare gas utilization device 20 is connected to the second end of the first outlet pipe L8 of the gas separation device 1. A first gas component separated by the gas separation device 1 flows within the first outlet pipe L8. Additionally, the rare gas utilization device 20 is connected to a third supply pipe L11, the first end of which is connected to a second gas component supply device (not shown). The second gas component flows within the third supply pipe L11. Therefore, the rare gas utilization device 20 can utilize both the first gas component separated by the gas separation device 1 and the second gas component supplied by the second gas component supply device (not shown).

[0046] The rare gas utilization device 20 can be electrically connected to the computing device 12 described below. In addition, the rare gas utilization device 20 can send the flow rates of the first gas component and the second gas component used and discharged in the rare gas utilization device as electrical signals to the computing device 12.

[0047] Rare gas usage equipment 20 is not particularly limited to any equipment that uses rare gases. Examples include: apparatus for manufacturing semiconductor integrated devices, inspection equipment, and equipment for manufacturing display devices such as liquid crystal panels.

[0048] The exhaust gas from the rare gas application device 20 contains a first gas component that is the target for purification, and a second gas component that is the target for removal. Examples of the first gas component include high-value-added gases such as krypton and xenon. Examples of the second gas component include hydrogen, nitrogen, oxygen, helium, neon, and argon.

[0049] The first end of the first supply pipe L1 is connected to the rare gas using device 20, and the second end of the first supply pipe L1 is connected to the raw material gas container 3. The first supply pipe L1 supplies the exhaust gas discharged from the rare gas using device 20 to the raw material gas container 3.

[0050] A flow meter 2 is installed in the first supply pipe L1. The flow meter 2 measures the flow rate of the rare gas discharged from the rare gas application device 20 flowing within the first supply pipe L1. The flow meter 2 is only required to measure the flow rate V of the first gas component in the discharged gas. F1 The flow rate V of the second gas component F2 The sum of V F0 It needs to be able to transmit the flow rate value as an electrical signal. For example, a mass flow meter, Coriolis flow meter, or volumetric flow meter can be used. The flow meter 2 is electrically connected to the processing unit 12, thus enabling it to transmit the flow rate V... F0 The measured value is sent to the processing unit 12. The flow meter 2 can also measure V. F1 and V F2 .

[0051] The gas separation apparatus of this embodiment includes a flow information acquisition device for acquiring information about the flow rates of a first gas component and a second gas component flowing through a first supply pipe L1. In the gas separation apparatus 1, for example, a concentration meter 13 is provided in the first supply pipe L1. The concentration meter 13 is capable of measuring the concentration of the first gas component, the concentration of the second gas component, or both, in the discharged gas. The concentration meter 13 only needs to be able to measure the concentration of the first gas component, the second gas component, or both, and be able to transmit the concentration value as an electrical signal. For example, an ultrasonic concentration meter or a mass spectrometer can be used as the concentration meter 13. The concentration meter 13 can transmit the concentration values ​​of the first gas component, the second gas component, or both as electrical signals to the processing unit 12.

[0052] As long as the traffic information acquisition device can acquire V F1 and V F2 As information, there is no particular limitation on the specific manner in which it is used. In another embodiment, for example, the flow information acquisition device may be configured to include at least one of the following: a flow meter installed in the first supply pipe L1; a concentration meter installed in the first supply pipe L1 for measuring the concentration of a first gas component; a concentration meter installed in the first supply pipe L1 for measuring the concentration of a second gas component; a receiver electrically receiving flow information of the first gas component discharged from the rare gas usage device 20 from the rare gas usage device 20; and a receiver electrically receiving flow information of the second gas component used in the rare gas usage device 20 from the rare gas usage device 20.

[0053] For example, in the gas separation device 1, the receiver 14 is capable of electrically receiving flow rate information of the first gas component discharged from the rare gas utilization device 20. Furthermore, the receiver 14 is also a receiver that electrically receives flow rate information of the second gas component used in the rare gas utilization device 20.

[0054] The configuration of the traffic information acquisition device is not limited to the examples above.

[0055] The raw material gas container 3 stores the raw material gas to be supplied to the separation unit 5. The second ends of the first supply pipe L1, the second ends of the return pipe L3, the second ends of the first inlet pipe L6, and the second inlet pipe L7 are connected to the raw material gas container 3. Therefore, the raw material gas container 3 contains a mixture of gases supplied from the first supply pipe L1, the return pipe L3, the first inlet pipe L6, and the second inlet pipe L7, and this mixed gas is stored as the raw material gas. A replenishment pipe L12 for supplementing the first gas component into the gas separation device 1 can be connected to the raw material gas container 3. The replenishment pipe L12 is connected to a supply source 15 for the first gas component. The supply source 15 for the first gas component is, for example, a container for storing the first gas component.

[0056] The first end of the second supply pipe L2 is connected to the raw material gas container 3, and the second end of the second supply pipe L2 is connected to the primary side of the separation section 5. A compressor 4 is installed on the second supply pipe L2. The second supply pipe L2 compresses the raw material gas in the raw material gas container 3 and supplies it to the primary side of the separation section 5. The compressor 4 can be a general compressor used in pressure adsorption gas separation methods and is not particularly limited. Among them, the compressor 4 is preferably an oil-free type that will not contaminate the raw material gas supplied to the separation section 5 and a highly airtight type that prevents air intake or raw material gas leakage. For example, a diaphragm compressor can be used.

[0057] Separation section 5 separates the first gas component and the second gas component from the raw material gas using pressure adsorption. For example... Figure 2 As shown, the separation section 5 includes a first adsorption tower 53A and a second adsorption tower 53B. Furthermore, the second ends of branches of the second supply pipe L2 are connected to the first adsorption tower 53A and the second adsorption tower 53B, respectively. Supply valves 51A and 51B are respectively provided at the second ends of the branches of the second supply pipe L2.

[0058] The first adsorption tower 53A contains a first adsorbent (not shown) that adsorbs the second gas component in the feed gas. The first adsorbent need only be able to adsorb the second gas component and can be appropriately selected based on the second gas component. For example, when the second gas component is nitrogen, Na-A type zeolite, carbon molecular sieve, mesoporous silica, or metal-organic structure (MOF) are preferred as the first adsorbent.

[0059] The first adsorption tower 53A removes the second gas component from the raw material gas and discharges the first gas component to the secondary side of the separation section 5. The secondary side of the first adsorption tower 53A is connected to the first end of the first separation pipe L4. The first adsorption tower 53A discharges the separated first gas component into the first separation pipe L4.

[0060] The first separation pipe L4 connects the first adsorption tower 53A of the separation section 5 to the first separation gas container 6. The first separation gas container 6 stores the first gas component separated by the first adsorption tower 53A of the separation section 5. The first end of the first inlet pipe L6 and the first end of the first outlet pipe L8 are connected to the first separation gas container 6.

[0061] The second adsorption tower 53B contains a second adsorbent (not shown) that adsorbs the first gaseous component in the feed gas. The second adsorbent need only be able to adsorb the first gaseous component and can be appropriately selected based on that component. For example, if the first gaseous component is xenon, activated carbon, CaA-type zeolite, Na-X-type zeolite, Ca-X-type zeolite, Li-X-type zeolite, or metal-organic structures (MOFs) are preferred as the second adsorbent.

[0062] The second adsorption tower 53B removes the first gas component from the feed gas and discharges the second gas component to the secondary side of the separation section 5. The secondary side of the second adsorption tower 53B is connected to the first end of the second separation pipe L5. The second adsorption tower 53B discharges the separated second gas component into the second separation pipe L5.

[0063] The second separation pipe L5 connects the separation section 5 and the second separation gas container 7. The second separation gas container 7 stores the second gas component separated by the separation section 5. The first end of the second inlet pipe L7 and the first end of the second outlet pipe L9 are connected to the second separation gas container 7.

[0064] The primary sides of the first adsorption tower 53A and the second adsorption tower 53B are respectively connected to the first ends of branches of the reflux pipe L3. Pressure relief valves 52A and 52B are respectively installed at the first ends of the branches of the reflux pipe L3. The reflux pipe L3 supplies a mixed gas containing the second gas component adsorbed on the first adsorbent discharged from the first adsorption tower 53A and the first gas component adsorbed on the second adsorbent discharged from the second adsorption tower 53B to the raw material gas container 3. In this way, the reflux pipe L3 refluxes the mixed gas containing the first and second gas components discharged from the primary side of the separation section 5 back to the raw material gas container 3.

[0065] The secondary sides of the first adsorption tower 53A and the second adsorption tower 53B are connected to regeneration pipes 57A and 57B, respectively. Regeneration valves 56A and 56B are respectively installed on regeneration pipes 57A and 57B. Regeneration pipes 57A and 57B supply regeneration gas for regenerating each adsorbent to the first adsorption tower 53A and the second adsorption tower 53B, respectively.

[0066] Pressure gauges 54A and 54B are respectively installed in the first adsorption tower 53A and the second adsorption tower 53B. Pressure gauges 54A and 54B measure the pressure inside each adsorption tower 53A and 53B.

[0067] The separation unit 5, like a typical pressure adsorption gas separation device, may further include a pressure equalization pipe equipped with a pressure equalization valve.

[0068] The separation unit 5 can be used to separate the first gas component and the second gas component by pressure adsorption, or it can be separated by multiple adsorption towers filled with a second adsorbent that adsorbs the first gas component in the raw material gas.

[0069] like Figure 1 As shown, the second end of the first inlet pipe L6 is connected to the raw material gas container 3. Therefore, the first inlet pipe L6 can introduce the first gas component in the first separation gas container 6 as the first inlet gas into the raw material gas. The connection of the second end of the first inlet pipe L6 is not limited to the raw material gas container 3. In another embodiment, the second end of the first inlet pipe L6 may also be connected, for example, to the second supply pipe L2 connected to the primary side of the separation section 5 and the primary side of the compressor 4.

[0070] The second end of the second inlet pipe L7 is connected to the raw material gas container 3. Therefore, the second inlet pipe L7 can introduce the second gas component in the second separation gas container 7 as the second inlet gas into the raw material gas. The connection of the second end of the second inlet pipe L7 is not limited to the raw material gas container 3. In another embodiment, the second end of the second inlet pipe L7 may also be connected, for example, to the second supply pipe L2 connected to the primary side of the separation section 5 and the primary side of the compressor 4.

[0071] A first flow controller 8 is installed on the first inlet pipe L6. The first flow controller 8 regulates and controls the flow rate V of the first inlet gas from the first separating gas container 6 according to the instructions of the arithmetic unit 12 electrically connected to it. R1 .

[0072] A second flow controller 9 is installed on the second inlet pipe L7. The second flow controller 9 regulates and controls the flow rate V of the second inlet gas from the second separation gas container 7 according to the instructions of the arithmetic unit 12 electrically connected to it. R2 .

[0073] The first flow controller 8 and the second flow controller 9 only need to be able to control the flow rate according to the indication of the electrical signal. For example, a mass flow controller can be used.

[0074] The arithmetic unit 12 is electrically connected to the first flow controller 8, the second flow controller 9, the flow meter 2, and the concentration meter 13, respectively. The arithmetic unit 12 calculates the flow rate V of the first gas component in the discharged gas. R1 The flow rate V of the second gas component R2 The flow rate V of the first gas component in the discharged gas is determined and indicated to the first flow controller 8 and the second flow controller 9 respectively. R1 The flow rate V of the second gas component R2 It is calculated based on the flow rate of the exhaust gas from the rare gas using device 20, which is transmitted as an electrical signal from the flow meter 2, and the concentration of the first gas component or the second gas component in the exhaust gas, which is transmitted as an electrical signal from the concentration meter 13.

[0075] As long as the flow meter 2 can measure the flow rates of the first gas component and the second gas component in the discharged gas, it can also determine the flow rate based on the respective flow rate values ​​and indicate the first flow controller 8 and the second flow controller 9 respectively.

[0076] In addition, as long as the computing device 12 is electrically connected to the rare gas usage device 20, it can send the flow rates of the first gas component and the second gas component in the discharged gas as electrical signals from the rare gas usage device 20. The computing device 12 can also determine each flow rate based on these flow rates and give instructions to the first flow controller 8 and the second flow controller 9 respectively.

[0077] The arithmetic unit 12 determines the amount of the first gas component introduced based on the first inlet pipe L6 and the amount of the second gas component introduced based on the second inlet pipe L7, and instructs the first flow controller 8 and the second flow controller 9 to keep the flow rate and composition of the exhaust gas introduced into the raw material gas container 3 and the mixture of the first inlet gas and the second inlet gas constant.

[0078] A first concentration meter (not shown) is installed in the first inlet pipe L6 to measure the concentration of a first gas component within the first inlet pipe L6. When the first concentration meter is electrically connected to the processing unit 12, the processing unit 12 can calculate the flow rate V of the first inlet gas based on the concentration of the first gas component within the first inlet pipe L6. R1 The instruction is given to the first flow controller 8. As a result, the composition of the raw material gas can be controlled more reliably and precisely, further stabilizing and improving the purity and recovery rate of the separated gas components.

[0079] A second concentration meter (not shown) is installed in the second inlet pipe L7 to measure the concentration of the second gas component within the second inlet pipe L7. When the second concentration meter is electrically connected to the processing unit 12, the processing unit 12 can, based on the concentration of the second gas component within the second inlet pipe L7, determine the flow rate V of the second inlet gas flowing through the second inlet pipe L7. R2 The instruction is given to the second flow controller 9. As a result, the composition of the feed gas can be controlled more reliably and precisely, further stabilizing and improving the purity and recovery rate of the separated gas components.

[0080] The first outlet pipe L8 outlets the first gas component separated by the separator 5 to the rare gas application device 20. A third flow controller 10 is installed on the first outlet pipe L8. The third flow controller 10 regulates and controls the flow rate V of the first gas component flowing through the first outlet pipe L8. 01 .

[0081] A fourth flow controller 11 is installed in the second outlet pipe L9. The fourth flow controller 11 regulates and controls the flow rate V of the second gas component flowing in the second outlet pipe L9. 02 The connection object at the second end of the second outgoing pipe L9 is not particularly limited.

[0082] (Effects)

[0083] The gas separation device 1 described above includes a computing unit 12 that is electrically connected to the first flow controller 8, the second flow controller 9, the flow meter 2, and the concentration meter 13, respectively. Therefore, the gas separation device 1 can calculate the flow rate V of the first gas component in the exhaust gas discharged from the rare gas application device 20 based on the flow rate value measured by the flow meter 2 and the concentration value measured by the concentration meter 13. F1 Flow rate V of the second gas component F2 To control the flow rate V of the first gas component flowing through the first inlet pipe L6. R1 and the flow rate V of the second gas component flowing in the second inlet pipe R2 .

[0084] Therefore, according to the gas separation device 1 of this embodiment, even if the concentration of the second gas component in the exhaust gas of the rare gas using equipment increases, the flow rate V can be calculated by the calculation device 12. R1 and traffic V R2 The control aims to make the concentration of the first gas component in the raw material gas relatively high, so that the purity of the first gas component after separation is not easily reduced.

[0085] On the other hand, according to the gas separation device 1, even if the concentration of the first gas component in the exhaust gas of the rare gas using equipment increases, the calculation device 12 can control the concentration of the first gas component in the raw material gas to relatively decrease. As a result, even without changing the operating conditions of the pressure adsorption separation unit, the rare gas separation energy of the separation unit can be stabilized, a certain gas separation energy can be obtained, and the recovery rate of the first gas component can be increased.

[0086] Therefore, the gas separation device 1 according to this embodiment can recycle the exhaust gas from the rare gas usage equipment while steadily improving both the purity and recovery rate of the separated rare gas.

[0087] <Gas Separation Methods>

[0088] The following is for reference Figure 1 and Figure 2 The gas separation method according to this embodiment will be explained. In the gas separation method according to this embodiment, a separation unit 5 is used to separate a first gas component and a second gas component from a raw material gas containing multiple gas components by pressure adsorption.

[0089] In the following description, the embodiments of the present invention will be described using the case where the first gas component is xenon (Xe) and the second gas component is nitrogen (N2) as an example, but the present invention is not limited to this example.

[0090] Here, the following description will begin with the adsorption process performed using the first adsorption tower 53A.

[0091] First, in the adsorption process of the first adsorption tower 53A, the exhaust gas from the rare gas application device 20 is supplied to the raw material gas container 3. The flow rate V of the xenon in the exhaust gas is... F1 and nitrogen flow rate V F2 The flow meter 2 measures the flow and sends the measured value to the computing device 12. The raw material gas is drawn from the raw material gas container 3 through the second supply pipe L2 and pressurized to the specified pressure by the compressor 4.

[0092] The feed gas, pressurized by compressor 4, flows into the first adsorption tower 53A through supply valve 51A. Compared to nitrogen, the Na-A type zeolite filling the first adsorption tower 53A is less adsorbent of xenon. Therefore, nitrogen, an easily adsorbed component in the feed gas flowing into the first adsorption tower 53A, will preferentially adsorb onto the Na-A type zeolite. Xenon, a difficult-to-adsorb component, will be separated, and the separated xenon will be stored in the first separated gas container 6 from the secondary side of adsorption tower 53A via the first separation pipe L4 and separation valve 55A.

[0093] During this process, the second adsorption tower 53B undergoes a regeneration process. The xenon adsorbed in the second adsorption tower 53B is returned to the raw material gas container 3 via the reflux pipe L3 and the pressure relief valve 52B.

[0094] When switching between the adsorption and regeneration processes, similar to conventional pressure adsorption separation processes, pressure equalization operations using pressure equalization piping with equalization valves and cleaning and regeneration operations using regeneration piping 57B with regeneration valve 56B can be performed.

[0095] In the regeneration process of the second adsorption tower 53B, the pressure inside the tower is reduced, causing the xenon that has separated from the activated carbon filling the second adsorption tower 53B to be discharged. Therefore, the mixed gas discharged from the primary side of the separation section 5 in the regeneration process is reused via the gas separation device 1 instead of being discarded. Specifically, the mixed gas released to the return pipe L3 is returned to the raw material gas container 3 located on the primary side of the compressor 4, where it is mixed with the raw material gas for reuse.

[0096] Before the nitrogen adsorption capacity of the Na-A type zeolite in the first adsorption tower 53A reaches saturation and before the nitrogen flows out from the secondary side of the first adsorption tower 53A, the supply valves 51A and 51B, the separation valves 55A and 55B, and the pressure relief valves 52A and 52B are opened and closed to switch the process of adsorption towers 53A and 53B. That is, the first adsorption tower 53A is switched to the regeneration process, and the second adsorption tower 53B is switched to the adsorption process.

[0097] The adsorption process of the second adsorption tower 53B is described.

[0098] The feed gas, pressurized by compressor 4, flows into the second adsorption tower 53B through supply valve 51B. Compared to xenon, the activated carbon filled in the second adsorption tower 53B is less adsorbent of nitrogen. Therefore, xenon, an easily adsorbed component in the feed gas flowing into the second adsorption tower 53B, will preferentially adsorb onto the activated carbon, while nitrogen, a difficult-to-adsorb component, will be separated. The separated nitrogen will be stored in the second separated gas container 7 from the secondary side of the second adsorption tower 53B via the second separation pipe L5 and separation valve 55B.

[0099] During this process, the first adsorption tower 53A undergoes a regeneration process. The nitrogen adsorbed in the first adsorption tower 53A flows back to the raw material gas container 3 through the reflux pipe L3 and the pressure relief valve 52A.

[0100] When switching between the adsorption and regeneration processes, similar to conventional pressure adsorption separation processes, pressure equalization operations using pressure equalization piping with equalization valves and cleaning and regeneration operations using regeneration piping 57A with regeneration valve 56A can be performed.

[0101] In the regeneration process of the first adsorption tower 53A, the nitrogen released from the Na-A type zeolite is released by reducing the pressure inside the tower. Furthermore, xenon inside the first adsorption tower 53A is also discharged. Therefore, the mixed gas discharged from the primary side of the separation section 5 during the regeneration process is reused via the gas separation device 1 instead of being discarded. Specifically, the mixed gas released to the return pipe L3 is returned to the raw material gas container 3 located on the primary side of the compressor 4, where it is mixed with the raw material gas for reuse.

[0102] In the gas separation method of this embodiment, xenon, which is a first gas component and is separated from the raw material gas by the first adsorption tower 53A of the separation unit 5, is introduced into the raw material gas as a first introducer gas. Furthermore, nitrogen, which is a second gas component and is separated from the raw material gas by the second adsorption tower 53B of the separation unit 5, is introduced into the raw material gas as a second introducer gas.

[0103] Xenon, separated by separation unit 5, flows from the first separated gas container 6 through the first inlet pipe L6 and is introduced into the raw material gas container 3 as the first inlet gas. Nitrogen, separated by separation unit 5, flows from the second separated gas container 7 through the second inlet pipe L7 and is introduced into the raw material gas container 3 as the second inlet gas.

[0104] In the gas separation method according to this embodiment, the flow rate V of the first gas component (xenon) in the exhaust gas discharged from the rare gas using device 20 is used as the basis for the separation method. F1 To control the flow rate V of the first introduced gas R1 Specifically, based on the flow rate V of the first gaseous component (xenon) in the exhaust gas... F1 The flow rate V of the first introduced gas is determined by the arithmetic unit 12. R1 The flow rate V is controlled by a first flow controller 8 electrically connected to the computing device 12. R1 Regulation and control.

[0105] Furthermore, based on the flow rate V of the second gas component (nitrogen) in the exhaust gas discharged from the rare gas using device 20... F2 To control the flow rate V of the second introduced gas R2 Specifically, based on the flow rate V of the second gaseous component (nitrogen) in the exhaust gas. F2 The flow rate V of the second introduced gas is determined by the arithmetic unit 12. R2 The flow rate V is controlled by a second flow controller 9 electrically connected to the computing device 12. R2 Regulation and control.

[0106] (Effects)

[0107] As described above, the gas separation method provided in this embodiment is characterized by the fact that, based on the flow rate V of the first gas component (xenon) in the exhaust gas discharged from the rare gas using device 20... F1 The flow rate V of the second gas component (nitrogen) F2 To control the flow rate V of the first introduced gas respectively. R1 The flow rate V of the second introduced gas R2 .

[0108] Therefore, according to the gas separation method of this embodiment, even if the composition of the exhaust gas from the rare gas application device 20 changes, the flow rate V of the first introduced gas can be maintained. R1 The flow rate V of the second introduced gas R2 The adjustment is made so that the ratio of xenon to nitrogen in the raw material gas supplied to the separation unit 5 does not change. Therefore, according to the gas separation method of this embodiment, at least the following effects (1) and (2) are obtained.

[0109] (1) When the ratio of xenon in the exhaust gas of the rare gas using device 20 decreases and the ratio of nitrogen increases, it is possible to control the flow rate V of the first introduced gas to achieve this. R1 Increase, and increase the flow rate V of the second introduced gas. R2 The concentration of nitrogen to be removed in the first adsorption tower 53A is reduced to suppress fluctuations. Therefore, the nitrogen removal performance of the first adsorption tower 53A can be stabilized and maintained at a high level, nitrogen can be removed sufficiently, and the purity of the separated xenon can be maintained and improved steadily.

[0110] (2) When the ratio of xenon to nitrogen in the exhaust gas of the rare gas using device 20 increases and the ratio of nitrogen decreases, the flow rate V of the first introduced gas can be controlled to achieve this. R1 Reduce, and increase the flow rate V of the second introduced gas. R2 The amount of xenon increases to suppress fluctuations in the concentration of xenon that should be removed in the second adsorption tower 53B. Therefore, the xenon removal performance in the second adsorption tower 53B can be stabilized and maintained at a high level, ensuring sufficient removal of xenon and maintaining a stable and high purity of the separated nitrogen. The separated nitrogen is not reused, thus reducing the amount of unusable xenon. As a result, the xenon recovery rate remains stable and high.

[0111] Because the effects of (1) and (2) can be obtained, the composition of the raw material gas can be stably maintained even if the composition of the exhaust gas from the rare gas utilization device 20 changes. Therefore, it is not necessary to change the operating conditions of the separation unit 5 according to the changes in the composition of the exhaust gas. In addition, assuming that the concentration of the rare gas (first gas component) in the exhaust gas of the rare gas utilization device 20 changes within the range of 0 to 100% by volume, the flow rate V of the first introduced gas can be controlled by the calculation device 12. R1 The flow rate V of the second introduced gas R2 Because of the control, the purity and recovery rate of rare gases can be steadily improved.

[0112] The gas separation method described in this embodiment preferably further controls the gas flow rate and S1 and the gas flow rate and S2 described below to predetermined values ​​respectively. For example, by using the arithmetic device 12 to control the gas flow rate and S1 and the gas flow rate and S2 to predetermined values, the following effect (3) can be further obtained.

[0113] Gas flow rate and S1 are the xenon flow rates V in the exhaust gas. F1 With the flow rate V of the first introduced gas R1 The total value,

[0114] Gas flow rate and S2 are the flow rates of nitrogen in the exhaust gas, V. F2 With the flow rate V of the second introduced gas R2 The total value.

[0115] (3) Since the separated xenon can be introduced into the raw material gas as the first inlet gas and nitrogen as the second inlet gas, the gas separation device can be operated according to the rapid changes in the composition and flow rate of the exhaust gas of the rare gas utilization device 20. Therefore, it is not necessary to drastically change the separation conditions of the separation section 5 according to the changes in the exhaust gas of the rare gas utilization device 20.

[0116] According to the gas separation method using the gas separation device 1 disclosed in this embodiment, in addition to the effects of (1) to (3) mentioned above, the effects of (4) and (5) mentioned below can also be obtained.

[0117] (4) The gas separation device 1 has a first inlet pipe L6 and a second inlet pipe L7, so it can cope with the sudden start-up and stop-up of the rare gas use equipment 20.

[0118] In this embodiment, the xenon flow rate V in the first outlet pipe L8 can be adjusted and controlled by the third flow controller 10 and the fourth flow controller 11. 01 Nitrogen flow rate V in the second outlet pipe L9 02Therefore, as long as the operation of the rare gas application device 20 is stopped, the xenon flow rate V will be reduced. 01 and nitrogen flow rate V 02 Both are 0, so even if the rare gas usage device 20 is not in operation, the gas separation device 1 can be operated by using the first inlet pipe L6 and the second inlet pipe L7 as bypass paths.

[0119] In conventional gas separation apparatuses, when starting the apparatus from a stopped state, a preparation period is required for the supply of the raw material gas before the desired performance is achieved and high-purity rare gas is prepared. In contrast, in the gas separation apparatus 1 of this embodiment, it is assumed that even if the rare gas utilization device 20 suddenly stops and becomes unused, the gas separation apparatus 1 can continue operating without stopping, continuously producing high-purity rare gas. Therefore, with the gas separation apparatus 1, the supply of rare gas can be immediately resumed in conjunction with the restoration of the rare gas utilization device 20. As a result, the start-up time of the gas separation apparatus 1 required for preparing high-purity rare gas is eliminated.

[0120] (5) The gas separation device 1 is equipped with a raw material gas container 3, a first separation gas container 6, a second separation gas container 7, a first inlet pipe L6 and a second inlet pipe L7. Therefore, it does not require the raw material gas required in a general gas separation device during the period from starting from a stopped state to obtaining the specified performance and preparing high-purity rare gas, and can economically utilize precious rare gas.

[0121] In the absence of a gas separation device with a raw material gas container 3, a first separated gas container 6, a second separated gas container 7, a first inlet pipe L6, and a second inlet pipe L7, the rare gas separated from the raw material gas until the specified separation performance is achieved during the preparation period for preparing high-purity rare gas must be discarded.

[0122] In contrast, when the gas separation device 1 of this embodiment is started from a stopped state, the rare gas separated from the raw material gas until the specified separation performance is achieved can be returned to the raw material gas container 3 for recycling via the first inlet pipe L6. Therefore, the valuable rare gas is not wasted, which is economically advantageous. Furthermore, there is no need to supply exhaust gas to the rare gas utilization device 20 during startup operation.

[0123] Second Implementation Method

[0124] The following is for reference Figure 3 The gas separation apparatus and gas separation method involved in this embodiment will be described.

[0125] Figure 3 This is a schematic diagram showing the gas separation apparatus 100 and the rare gas usage device 20 that uses rare gases according to this embodiment.

[0126] The gas separation device 100 of this embodiment differs from the gas separation device 1 of the first embodiment in the following aspects:

[0127] First difference: The gas separation device 100 of this embodiment has a third gas component removal device that is not present in the gas separation device 1 of the first embodiment described above.

[0128] The second difference is that, in contrast to the gas separation device 1 of the first embodiment described above, where the second ends of the first inlet pipe L6 and the second inlet pipe L7 are connected to the raw material gas container 3, in the gas separation device 100 of this embodiment, they are connected to the first supply pipe L1.

[0129] These points will be explained in detail below.

[0130] Regarding the first point of difference:

[0131] In the gas separation apparatus 100 of this embodiment, the third gas component, which is a trace component, contained in the exhaust gas discharged from the rare gas usage device 20 is removed by the third gas component removal device 103 described above.

[0132] The third gaseous component refers to components other than the first and second gaseous components described above. Organic compounds can be cited as examples of the third gaseous component.

[0133] The organic compound in question is not particularly limited to any organic compound that is discharged from a rare gas usage device and mixed into the raw material gas. Examples include: chain or cyclic hydrocarbon compounds, alcohols, carbonyl compounds, organofluorine compounds, etc.

[0134] Examples of chain or cyclic hydrocarbon compounds include chain or cyclic hydrocarbon compounds with 1 to 15 carbon atoms, such as methane, ethane, propane, n-butane, isobutane, n-pentane, isopentane, neopentane, hexane, heptane, octane, nonane, decane, undecane, dodecane, tridecane, tetradecane, pentadecane, cyclopropane, cyclobutane, cyclopentane, benzene, naphthalene, etc.

[0135] Examples of such organofluorine compounds include fluoromethane, difluoromethane, trifluoromethane, trichlorofluoromethane, chlorofluorocarbons, tetrafluoromethane, dichlorodifluoromethane, dichlorodifluoromethane, tetrachlorodifluoroethane, dichlorofluoroethane, dichlorodifluoroethane, dichlorodifluoroethane, difluoroethane, and other fluorocarbon compounds.

[0136] In this embodiment, the third gas component is preferably a hydrocarbon compound or an organic fluorine compound, such as a chain or cyclic hydrocarbon compound.

[0137] The aforementioned third gas component removal device 103 is located on the secondary side of the concentration meter 13 and is installed in the first supply pipe L1 located on the primary side of the raw material gas container 3. Therefore, the exhaust gas discharged from the rare gas application device 20 flows through the flow meter 2 and the concentration meter 13 in the first supply pipe L1 and is introduced into the third gas component removal device 103. The third gas component removal device 103 is not particularly limited as long as it can remove the aforementioned third gas component; for example, an adsorption removal device can be used. When the third gas component is a hydrocarbon compound or an organic fluorine compound, the third gas component removal device 103 preferably uses an activated carbon adsorption removal tower.

[0138] Regarding the second point of difference:

[0139] The second end of the first inlet pipe L6, which allows the first gas component stored in the first separating gas container 6 to flow through the first flow controller 8, is connected to the first supply pipe L1. More specifically, the second end of the first inlet pipe L6 is connected to the first supply pipe L1 located between the concentration meter 13 and the third gas component removal device 103.

[0140] The second end of the second inlet pipe L7, which allows the second gas component stored in the second separation gas container 7 to flow through the second flow controller 9, is connected to the first supply pipe L1. More specifically, the second end of the second inlet pipe L7 is connected to the first supply pipe L1 located between the concentration meter 13 and the third gas component removal device 103.

[0141] In the gas separation device 100 of this embodiment, the configuration involved in the above-mentioned differences 1 and 2 is provided. Therefore, the exhaust gas after the third gas component is removed by the third gas component removal device 103 is stored in the raw material gas container 3.

[0142] The first gas component stored in the first separated gas container 6 flows through the first flow controller 8 into the first inlet pipe L6 and merges with the exhaust gas flowing through the first supply pipe L1, and is then introduced into the third gas component removal device 103.

[0143] The second gas component stored in the second separate gas container 7 flows through the second flow controller 9 into the second inlet pipe L7 and merges with the exhaust gas flowing through the first supply pipe L1, and is then introduced into the third gas component removal device 103.

[0144] (Effects)

[0145] In addition to the effects of the gas separation apparatus 100 and gas separation method of the first embodiment described above, the following effects can also be obtained according to the gas separation apparatus 1 and gas separation method of this embodiment.

[0146] • Even if the conditions of the raw gas (flow rate, composition) change, it can more stably remove the third gas component as a trace component.

[0147] The feed gas conditions (flow rate, concentration of rare gases) vary depending on the operating conditions of the equipment using the rare gases. Adsorbents used for trace component removal (pretreatment adsorbents, typically activated carbon, etc.) not only adsorb trace components but also strongly adsorb rare gases (especially xenon). Therefore, their temperature rises or falls due to the heat of adsorption, depending on changes in the rare gas concentration (e.g., from 0% to 100%). For example, when the rare gas concentration changes from 0% to 100%, the adsorbent temperature can be expected to exceed 100°C. The adsorption performance of the adsorbent is greatly affected by temperature; therefore, this temperature change can affect the degree to which the intended trace components are adequately adsorbed.

[0148] In contrast, according to the gas separation device 100 and gas separation method of the second embodiment, the flow rate V of the first introduced gas is adjusted. R1 The flow rate V of the second introduced gas R2 Subsequently, the first gas component is drawn from the first inlet pipe L6 and the second gas component is drawn from the second inlet pipe L7 into the first supply pipe L1. Therefore, even if the composition of the exhaust gas of the rare gas use device 20 changes, the concentration of the first gas component (rare gas) in the raw material gas introduced into the third gas component removal device 103 will not change.

[0149] Therefore, the temperature of the adsorbent in the third gas component removal device 103 is not easily changed, and the variation in adsorption performance is small. As a result, trace impurities can be stably removed by the third gas component removal device 103.

[0150] • Because the separated and purified first gas component (rare gas) and second gas component (N2, etc.) are mixed into the exhaust gas supplied from the first supply pipe L1, the concentration of impurity components contained in the exhaust gas is further reduced. Since the concentration of impurities to be removed is reduced, the adsorbent capacity of the third gas component removal device described above can be maintained.

[0151] The above describes several embodiments of the present invention, but the present invention is not limited to the specific embodiments described. Furthermore, the present invention can be modified by adding, omitting, or substituting features within the scope of the spirit of the invention as described in the claims.

[0152] In this embodiment, although Figure 1 The present invention discloses a flow information acquisition device having a flow meter 2 and a concentration meter 13 (a first concentration meter for measuring the concentration of a first gas component and a second concentration meter for measuring the concentration of a second gas component), but is not limited to this embodiment. For example, a rare gas application device 20 has a flow rate V capable of separately measuring the first gas component. F1 Flow rate V of the second gas component F2 If the processing unit 12 is equipped with a receiver that electrically receives this information, then that receiver can become a flow rate information acquisition device. Additionally, the rare gas application device 20 is equipped with a flow rate V capable of measuring the composition of the first gas. F1 Or the flow rate V of the second gas component F2 In the case of the device, the flow rate V of the first gas component can be received by the electrical input of the flow meter 2 and the arithmetic unit 12. F1 Or the flow rate V of the second gas component F2 The receiver of the information is used to form a traffic information acquisition device.

[0153] If the flow meter 2 is required to measure the flow rate of the first gas component and the flow rate of the second gas component in the mixed gas respectively, the flow meter 2 can be used as the flow information acquisition device.

[0154] Example

[0155] The present invention will be specifically described below using examples, but the present invention is not limited to the following description.

[0156] <Example 1>

[0157] Construct Figure 1 The gas separation device 1 shown. The gas separation device 1 used in Example 1 includes... Figure 2 Separation section 5 is shown.

[0158] The detailed configuration of the gas separation device used in Example 1 is described below.

[0159] • Compressor 4: Set the ejection flow rate to 26 L / min at 0°C and 1 atm.

[0160] • First adsorption tower 53A: An adsorption tower with an inner diameter of 154 mm and a length of 650 mm, filled with 8.8 kg of Na-A type zeolite.

[0161] • Second adsorption tower 53B: An adsorption tower with an inner diameter of 108 mm and a length of 650 mm, filled with 2.7 kg of activated carbon.

[0162] First, using a mixture of gases of the following composition 1, which is envisioned as the exhaust gas of a rare gas application device, xenon is separated from the raw material gas as the first gas component, and nitrogen is separated as the second gas component.

[0163] • Composition 1: A mixture of Xe and N2 (Xe concentration: 33% by volume, N2 concentration: 67% by volume)

[0164] • Flow rate of exhaust gas from component 1: 1.5 NL / min

[0165] Here, during the separation of the raw material gas using the exhaust gas of component 1, the introduction of the first inlet gas (Xe) into the raw material gas via the first inlet pipe L6 and the introduction of the second inlet gas (N2) into the raw material gas via the second inlet pipe L7 are not performed. Furthermore, the supply flow rate V of Xe to the rare gas utilization device 20 is... 01 Controlled at 0.5 NL / min,

[0166] The flow rate V of N2 02 Controlled at 1.0 NL / min.

[0167] The separation results of the raw material gas using the exhaust gas of component 1 in Example 1 are shown below.

[0168] • Xe purity in first outlet pipe L8: 99.993% by volume

[0169] • N2 concentration as an impurity in the first outlet pipe L8: 70 ppm (by volume)

[0170] • N2 purity in the second outlet pipe L9: 99.988% by volume

[0171] • Xe concentration as an impurity in the second outlet pipe L9: 120 ppm (by volume)

[0172] • Xe recovery rate: 99.98%.

[0173] Next, the composition of the exhaust gas mixture from the device intended to use rare gases was changed from composition 1 to composition 2. This was an experiment conducted to change the composition of the intended exhaust gas. The compressor's ejection flow rate, the switching time of the adsorption process, and the regeneration process were set to the same values.

[0174] • Composition 2: A mixture of Xe and N2 (Xe concentration: 50% by volume, N2 concentration: 50% by volume)

[0175] • Flow rate of exhaust gas from component 2: 1.0 NL / min

[0176] When separating the feed gas using the exhaust gas of component 2, the flow rates of Xe and N2 in the exhaust gas are controlled to such that the flow rate V of the first inlet gas (Xe) introduced through the first inlet pipe L6 is equal to the flow rate V of the first inlet gas (Xe). R1 To achieve 0 NL / min, and to make the flow rate V of the second inlet gas (N2) introduced through the second inlet pipe L7... R2 The flow rate becomes 0.5 NL / min. Furthermore, the supply flow rate V of Xe to the rare gas utilization device 20 is... 01 Control the flow rate to 0.5 NL / min, and increase the flow rate V of N2. 02 The speed is controlled at 0.5 NL / min.

[0177] In Example 1, the separation results of the feed gas using the exhaust gas of composition 2 are shown below. As shown below, even if the composition of the feed gas is changed from composition 1 to composition 2, the Xe recovery rate can be improved while maintaining the high purity of Xe.

[0178] • Xe purity in first outlet pipe L8: 99.993% by volume

[0179] • N2 concentration as an impurity in the first outlet pipe L8: 70 ppm (by volume)

[0180] • N2 purity in the second outlet pipe L9: 99.988% by volume

[0181] • Xe concentration as an impurity in the second outlet pipe L9: 120 ppm (by volume)

[0182] • Xe recovery rate: 99.99%

[0183] Next, the composition of the gas mixture discharged from the device intended for use with rare gases is changed to the following composition 3. The compressor's discharge flow rate, the switching time of the adsorption process, and the regeneration process are set to the same value.

[0184] • Composition 3: A mixture of Xe and N2 (Xe concentration: 1% by volume, N2 concentration: 99% by volume)

[0185] • Flow rate of exhaust gas from component 3: 1.0 NL / min

[0186] When separating the feed gas using the exhaust gas of component 3, the flow rates of Xe and N2 in the exhaust gas are controlled to ensure that the flow rate V of the first inlet gas (Xe) introduced through the first inlet pipe L6 is equal to the flow rate V of the first inlet gas (Xe). R1The flow rate becomes 0.49 NL / min, and the flow rate V of the second inlet gas (N2) introduced through the second inlet pipe L7 is increased. R2 The flow rate becomes 0.01 NL / min. Furthermore, the supply flow rate V of Xe to the rare gas utilization device 20 is... 01 Controlled to 0.01 NL / min, the flow rate V of N2 is... 02 The control rate is 0.99 NL / min.

[0187] The separation results of the feed gas using the exhaust gas of composition 3 are shown below. As shown below, even if the composition of the feed gas is changed from composition 2 to composition 3, the high purity and high recovery rate of Xe can be maintained.

[0188] • Xe purity in the first outgoing pipe L8: 99.993% by volume

[0189] • N2 concentration as an impurity in the first outlet pipe L8: 70 ppm (by volume)

[0190] • N2 purity in the second outlet pipe L9: 99.988% by volume

[0191] • Xe concentration as an impurity in the second outlet pipe L9: 120 ppm (by volume)

[0192] • Xe recovery rate: 98.8%

[0193] <Comparative Example 1>

[0194] In Comparative Example 1, the separation device was assembled in the same manner as in Example 1, except that it did not have the arithmetic device 12, the first inlet pipe L6, and the second inlet pipe L7.

[0195] Using the following mixture of gases, which is also used in Example 1 as the exhaust gas of a rare gas application device, xenon (Xe) is separated from the raw material gas as the first gas component and nitrogen (N2) is separated as the second gas component.

[0196] In Comparative Example 1, during the separation of the exhaust gas of Component 1, the supply flow rate V of Xe to the rare gas utilization device 20 is also increased. 01 Control the flow rate to 0.5 NL / min, and increase the flow rate V of N2. 02 Controlled at 1.0 NL / min.

[0197] • Composition 1: A mixture of Xe and N2 (Xe concentration: 33% by volume, N2 concentration: 67% by volume)

[0198] • Flow rate of the feed gas for component 1: 1.5 NL / min

[0199] The separation results of the feed gas using the exhaust gas of Component 1 in Comparative Example 1 are shown below. The separation results of the feed gas using the exhaust gas of Component 1 in Comparative Example 1 are consistent with the separation results of the feed gas of Component 1 in Example 1, in which the first introductory gas (Xe) and the second introductory gas (N2) were not introduced into the feed gas.

[0200] • Xe purity in the first outgoing pipe L8: 99.993% by volume

[0201] • N2 concentration as an impurity in the first outlet pipe L8: 70 ppm (by volume)

[0202] • N2 purity in the second outlet pipe L9: 99.988% by volume

[0203] • Xe concentration as an impurity in the second outlet pipe L9: 120 ppm (by volume)

[0204] • Xe recovery rate: 99.98%

[0205] Next, using the mixture of the following components 2, which is also intended to be the exhaust gas of a rare gas utilization device used in Example 1, xenon (Xe) is separated from the raw gas as the first gas component, and nitrogen (N2) is separated as the second gas component. In Comparative Example 1, when separating the exhaust gas of component 2, the supply flow rate V of Xe to the rare gas utilization device 20 is also increased. 01 Control the flow rate to 0.5 NL / min, and increase the flow rate V of N2. 02 The flow rate is controlled at 0.5 NL / min. The switching time for the compressor's discharge flow rate, adsorption process, and regeneration process is set to the same value.

[0206] • Composition 2: A mixture of Xe and N2 (Xe concentration: 50% by volume, N2 concentration: 50% by volume)

[0207] • Flow rate of feed gas for component 2: 1.0 NL / min

[0208] The separation results of the raw material gas using the exhaust gas of Component 2 in Comparative Example 1 are shown below.

[0209] • Xe purity in the first outgoing pipe L8: 99.9990% by volume

[0210] • N2 concentration as an impurity in the first outlet pipe L8: 10 ppm (volume)

[0211] • N2 purity in the second outlet pipe L9: 99.6770% by volume

[0212] • Xe concentration as an impurity in the second outlet pipe L9: 3230 ppm (volume)

[0213] • Xe recovery rate: 99.68%

[0214] In Comparative Example 1, if the separation of the feed gas using the exhaust gas of Component 2 continues, the feed gas in the feed gas container 3 will become insufficient, and the ejection flow rate of the compressor 4 will decrease. As a result, the pressure of the adsorption tower in the adsorption process will decrease.

[0215] Next, using the mixture of the following components 3, which is also intended to be the exhaust gas of a rare gas utilization device used in Example 1, xenon (Xe) is separated from the raw gas as the first gas component, and nitrogen (N2) is separated as the second gas component. In Comparative Example 1, when separating the exhaust gas of component 3, the supply flow rate V of Xe to the rare gas utilization device 20 is also... 01 Controlled to 0.01 NL / min, the flow rate V of N2 is... 02 The control rate is 0.99 NL / min.

[0216] • Composition 3: A mixture of Xe and N2 (Xe concentration: 1% by volume, N2 concentration: 99% by volume)

[0217] • Flow rate of feed gas in component 3: 1.0 NL / min

[0218] The separation results of the raw material gas using the exhaust gas of Component 3 in Comparative Example 1 are shown below.

[0219] • Xe purity in first outlet pipe L8: 99.148% by volume

[0220] • N2 concentration as an impurity in the first outlet pipe L8: 8520 ppm (by volume)

[0221] • N2 purity in the second outlet pipe L9: 99.6770% by volume

[0222] • Xe concentration as an impurity in the second outlet pipe L9: 100 ppm per volume

[0223] • Xe recovery rate: 99.01%

[0224] Here, similar to component 2 of Comparative Example 1, if the separation of the raw material gas continues, the raw material gas in the raw material gas container 3 will become insufficient, and the ejection flow rate of the compressor 4 will decrease. As a result, the pressure of the adsorption tower in the adsorption process will decrease.

[0225] In Comparative Example 1, as the composition of the exhaust gas changes sequentially from composition 1 to composition 2 and then to composition 3, the Xe recovery rate decreases. Furthermore, the purity of Xe within the first outlet pipe L8 also varies, causing the separation performance to become unstable due to changes in the composition of the exhaust gas.

[0226] <Example 2>

[0227] Construct Figure 3 The gas separation device 100 shown. The gas separation device 1 used in Example 2 includes... Figure 2 Separation section 5 is shown.

[0228] The gas separation device used in Example 2 is configured as follows.

[0229] • Compressor 4: Set the ejection flow rate to 26 L / min at 0°C and 1 atm.

[0230] • First adsorption tower 53A: An adsorption tower with an inner diameter of 108 mm and a length of 650 mm, filled with 2.7 kg of activated carbon.

[0231] • Second adsorption tower 53B: An adsorption tower with an inner diameter of 154 mm and a length of 650 mm, filled with 8.8 kg of Na-A type zeolite.

[0232] • Third gas component removal device 103: Adsorption removal tower using activated carbon

[0233] First, using a mixture of gases with the following composition 4, which is intended to be the exhaust gas of a rare gas utilization device, xenon is separated from the raw gas as the first gas component, nitrogen is separated as the second gas component, and n-butane (n-C4H) is separated. 10 ( ) as the third gas component.

[0234] • Composition 4: Xe and N2 and n-butane (n-C4H) 10 A mixture of gases (Xe concentration: 1 vol%, N2 concentration: 99 vol%, n-butane (n-C4H)) 10 : 100 ppm (by volume)

[0235] • Flow rate of exhaust gas from component 4: 1.0 NL / min

[0236] Here, when separating the raw material gas using the exhaust gas of component 4, the flow rates of Xe and N2 in the exhaust gas are controlled to ensure that the flow rate V of the first inlet gas (Xe) introduced through the first inlet pipe L6 is equal to that of the first inlet gas (Xe). R1 The flow rate of the second inlet gas (N2) introduced through the second inlet pipe L7 is 0.49 NL / min, and the flow rate V is also increased.R2 The flow rate becomes 0.01 NL / min. Additionally, the supply flow rate V of Xe to the rare gas utilization device 20 is... 01 Controlled to 0.01 NL / min, the flow rate V of N2 is... 02 The control rate is 0.99 NL / min.

[0237] The separation results of the raw material gas using the exhaust gas of component 4 in Example 2 are shown below.

[0238] • Xe purity in the first outgoing pipe L8: 99.993%

[0239] • N2 concentration as an impurity in the first outlet pipe L8: 70 ppm (by volume)

[0240] • n-Butane (n-C4H) as an impurity in the first outgoing pipe L8 10 Concentration: less than 1 ppm (volume)

[0241] • N2 purity in the second outlet pipe L9: 99.988% by volume

[0242] • Xe concentration as an impurity in the second outlet pipe L9: 120 ppm (by volume)

[0243] • Xe recovery rate: 98.8%

[0244] In addition, the temperature of the third gas component removal device 103 is 25°C.

[0245] Next, the composition of the gas mixture emanating from the device intended for use with rare gases is changed from composition 4 to composition 5. The compressor's ejection flow rate, the switching time of the adsorption process, and the regeneration process are set to the same value.

[0246] • Composition 5: Xe and N2 and n-butane (n-C4H) 10 A mixture of gases (Xe concentration: 50 vol%, N2 concentration: 50 vol%, n-butane (n-C4H)) 10 : 100 ppm (by volume)

[0247] • Flow rate of exhaust gas from component 5: 1.0 NL / min

[0248] When separating the feed gas using the exhaust gas of component 5, the flow rates of Xe and N2 in the exhaust gas are controlled to ensure that the flow rate V of the first inlet gas (Xe) introduced through the first inlet pipe L6 is equal to the flow rate V of the first inlet gas (Xe). R1 To achieve 0 NL / min, and to make the flow rate V of the second inlet gas (N2) introduced through the second inlet pipe L7... R2The flow rate becomes 0.5 NL / min. Additionally, the supply flow rate V of Xe to the rare gas utilization device 20 is... 01 Control the flow rate to 0.5 NL / min, and increase the flow rate V of N2. 02 The speed is controlled at 0.5 NL / min.

[0249] In Example 2, the separation results of the feed gas using the exhaust gas of composition 5 are shown below. As shown below, even if the composition of the feed gas is changed from composition 4 to composition 5, the Xe recovery rate can be improved while maintaining the high purity of Xe.

[0250] • Xe purity in the first outgoing pipe L8: 99.993% by volume

[0251] • N2 concentration as an impurity in the first outlet pipe L8: 70 ppm (by volume)

[0252] • n-Butane (n-C4H) as an impurity in the first outgoing pipe L8 10 Less than 1 ppm by volume

[0253] • N2 purity in the second outlet pipe L9: 99.988% by volume

[0254] • Xe concentration as an impurity in the second outlet pipe L9: 120 ppm (by volume)

[0255] • Xe recovery rate: 99.99%

[0256] In addition, the temperature of the third gas component removal device 103 is 25°C.

[0257] <Comparative Example 2>

[0258] In Comparative Example 2, the separation device was assembled in the same manner as in Example 2, except that it did not have the arithmetic device 12, the first inlet pipe L6, and the second inlet pipe L7.

[0259] Using the mixture of the following five components of the exhaust gas from the rare gas application device, which is also used in Example 2, xenon (Xe) is separated from the raw material gas as the first gas component, nitrogen (N2) is separated as the second gas component, and n-butane (n-C4H) is separated. 10 ( ) as the third gas component.

[0260] In Comparative Example 2, during the separation of the exhaust gas of Component 5, the supply flow rate V of Xe to the rare gas utilization device 20 is also increased. 01 Control the flow rate to 0.5 NL / min, and increase the flow rate V of N2. 02 The speed is controlled at 0.5 NL / min.

[0261] • Composition 5: Xe and N2 and n-butane (n-C4H) 10 A mixture of gases (Xe concentration: 50 vol%, N2 concentration: 50 vol%, n-butane (n-C4H)) 10 : 100 ppm (by volume)

[0262] • Flow rate of exhaust gas from component 5: 1.0 NL / min

[0263] The separation results of the feed gas using the exhaust gas of composition 5 in Comparative Example 2 are shown below.

[0264] • Xe purity in the first outgoing pipe L8: 99.9990% by volume

[0265] • N2 concentration as an impurity in the first outlet pipe L8: 10 ppm (volume)

[0266] • n-Butane (n-C4H) as an impurity in the first outgoing pipe L8 10 Concentration: 3.5 ppm (by volume)

[0267] • Xe concentration as an impurity in the second outlet pipe L9: 3230 ppm (volume)

[0268] • N2 purity in the second outlet pipe L9: 99.6770% by volume

[0269] • Xe recovery rate: 99.68%

[0270] In addition, the temperature of the third gas component removal device 103 is 67°C.

[0271] In Comparative Example 2, the temperature of the third gas component removal device 103 increased, causing n-butane (n-C4H) to be removed. 10 Removal of n-butane (n-C4H) becomes difficult. 10 The concentration increases.

[0272] Explanation of reference numerals in the attached figures

[0273] 1, 100: Gas separation device

[0274] 2: Flow meter

[0275] 3: Raw material gas container

[0276] 4: Compressor

[0277] 5: Separation section

[0278] 6: First gas separation container

[0279] 7: Second gas separation container

[0280] 8: First Flow Controller

[0281] 9: Second Flow Controller

[0282] 10: Third Flow Controller

[0283] 11: Fourth Flow Controller

[0284] 12: Computing device

[0285] 13: Concentration meter

[0286] 14: Receiver

[0287] 15: Supply source of the first gas component

[0288] 20: Gas usage equipment

[0289] 51A, 51B: Supply valves

[0290] 52A, 52B: Pressure relief valves

[0291] 53A, 53B: Adsorption towers

[0292] 54A, 54B: Pressure gauges

[0293] 55A, 55B: Separation valve

[0294] 56A, 56B: Regeneration valves

[0295] 57A, 57B: Regenerated Piping

[0296] L1: First supply piping

[0297] L2: Second supply piping

[0298] L3: Return piping

[0299] L4: First disconnect piping

[0300] L5: Second split piping

[0301] L6: First inlet piping

[0302] L7: Second inlet piping

[0303] L8: First Outgoing Piping

[0304] L9: Second Outlet Piping

[0305] L11: Third Supply Piping

[0306] L12: Supplies

[0307] 103: Third gas component removal device

Claims

1. A gas separation method, comprising using a gas separation device to separate a first gas component and a second gas component, which are rare gas components, from a raw gas containing multiple gas components, characterized in that, The gas separation device includes: The separation section includes an adsorption tower, and separates the first gas component and the second gas component from a feed gas containing multiple gas components by pressure adsorption. A raw material gas container for storing the raw material gas; The first supply piping supplies the exhaust gas containing the first gas component and the second gas component from the rare gas using equipment to the raw material gas container; The second supply piping connects the raw material gas container to the separation unit; A first gas separation container stores the first gas component separated by the separation section; The second gas separation container stores the second gas component separated by the separation section; The first inlet pipe introduces the first gas component in the first separated gas container as the first inlet gas into the raw material gas container; The second inlet pipe introduces the second gas component in the second separated gas container as the second inlet gas into the raw material gas container; A first flow controller is installed in the first inlet pipe; A second flow controller is installed in the second inlet pipe; A flow information acquisition device is used to acquire information on the flow rates of the first gas component and the second gas component flowing in the first supply pipe; as well as The processing unit is electrically connected to the first flow controller, the second flow controller, and the flow information acquisition device, respectively, and is configured to adjust the flow rate V of the first introduced gas. R1 and the flow rate V of the second introduced gas R2 Each of them, The traffic information acquisition device includes: A flow meter is installed in the first supply piping; and A concentration meter, installed in the first supply pipe, measures the concentration of at least one of the first gas component and the second gas component in the discharged gas. The gas separation method includes an introduction step, wherein the first gas component separated from the raw material gas is introduced into the raw material gas container as a first introduction gas, and the second gas component separated from the raw material gas is introduced into the raw material gas container as a second introduction gas. Based on the flow rates of the first gas component and the second gas component in the discharged gas obtained by the flow information acquisition device, the following gas flow rates S1 and S2 are controlled to predetermined values ​​respectively. Gas flow rate and S1 are the flow rates V of the first gas component in the discharged gas. F1 With the flow rate V of the first introduced gas R1 The total value, Gas flow rate and S2 are the flow rates V of the second gas component in the discharged gas. F2 With the flow rate V of the second introduced gas R2 The total value.

2. The gas separation method according to claim 1, wherein, The first gas component is krypton or xenon.

3. The gas separation method according to claim 1, wherein, The second gaseous component contains at least one selected from hydrogen, nitrogen, oxygen, helium, neon, and argon.

4. The gas separation method according to claim 1, wherein, The exhaust gas discharged from the rare gas application device also contains a third gas component. After the first gas component separated from the raw material gas is introduced into the raw material gas container as the first inlet gas, and the second gas component separated from the raw material gas is introduced into the raw material gas container as the second inlet gas, the third gas component is removed from the raw material gas.

5. The gas separation method according to claim 4, wherein, The third gas component is an organic compound.

6. A gas separation device, comprising: The separation section includes an adsorption tower, and separates a first gas component and a second gas component from a feed gas containing multiple gas components by pressure adsorption. A raw material gas container for storing the raw material gas; The first supply piping supplies the exhaust gas containing the first gas component and the second gas component from the rare gas using equipment to the raw material gas container; The second supply piping connects the raw material gas container to the separation unit; A first gas separation container stores the first gas component separated by the separation section; The second gas separation container stores the second gas component separated by the separation section; The first inlet pipe introduces the first gas component in the first separated gas container as the first inlet gas into the raw material gas container; The second inlet pipe introduces the second gas component in the second separated gas container as the second inlet gas into the raw material gas container; A first flow controller is installed in the first inlet pipe; A second flow controller is installed in the second inlet pipe; A flow information acquisition device is used to acquire information on the flow rates of the first gas component and the second gas component flowing in the first supply pipe; as well as The processing unit is electrically connected to the first flow controller, the second flow controller, and the flow information acquisition device, respectively, and is configured to adjust the flow rate V of the first introduced gas. R1 and the flow rate V of the second introduced gas R2 Each of them, Among them, when: The flow meter installed in the first supply piping is denoted as A. The concentration meter installed in the first supply pipe and used to measure the concentration of the first gas component is denoted as B. When the concentration meter installed in the first supply pipe and used to measure the concentration of the second gas component is recorded as C, The traffic information acquisition device is composed of at least one of the following groups: A and B, A and C, and A and B and C; Wherein, based on the respective flow rates of the first gas component and the second gas component in the discharged gas obtained by the flow information acquisition device, The first flow controller controls the flow rate V of the first introduced gas introduced from the first separated gas container into the raw material gas container through the first introduced pipe. R1 This causes the flow rate V of the first gas component in the exhaust gas discharged from the rare gas using the device to increase. F1 The flow rate V of the first introduced gas introduced from the first separated gas container into the raw material gas container through the first introduced pipe R1 The gas flow rate and S1 are constant values, and The second flow controller controls the flow rate V of the second inlet gas introduced from the second separated gas container into the raw material gas container through the second inlet pipe. R2 This causes the flow rate V of the second gas component in the exhaust gas discharged from the rare gas using the device to increase. F2 The flow rate V of the second introduced gas introduced from the second separated gas container into the raw material gas container through the second introduced pipe R2 The gas flow rate and S2 are constant values.

7. The gas separation device according to claim 6, wherein, A first concentration meter for measuring the concentration of a first gas component within the first inlet pipe is further provided in the first inlet pipe, and the first concentration meter is also electrically connected to the computing device.

8. The gas separation device according to claim 6, wherein, A second concentration meter for measuring the concentration of a second gas component within the second inlet pipe is further provided in the second inlet pipe, and the second concentration meter is also electrically connected to the computing device.

9. The gas separation device according to claim 6, wherein, The first gas component is krypton or xenon.

10. The gas separation device according to claim 6, wherein, The second gaseous component contains at least one selected from hydrogen, nitrogen, oxygen, helium, neon, and argon.

11. The gas separation device according to claim 7, wherein, The exhaust gas discharged from the rare gas application device also contains a third gas component. The gas separation device includes a concentration meter installed in the first supply pipe. A third gas removal device for removing third gas components is further provided downstream of the first concentration meter in the first supply pipe. The first inlet pipe and the second inlet pipe are connected to the first supply pipe between the first concentration meter and the third gas removal device.

12. The gas separation device according to claim 11, wherein, The third gas component is an organic compound.

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