Integrated apparatus and method for gas super purification

Abstract

This invention provides an integrated device and method for gas ultrapurification, comprising: an integrated sealed cavity; an adsorption system disposed inside the integrated sealed cavity, the adsorption system being filled with at least one adsorbent; a temperature control system disposed inside the integrated sealed cavity, including independent refrigerant circulation loops and hot medium circulation loops, for temperature control of the adsorption system; and a gas pipeline system including a raw material inlet, a displacement gas inlet, a product gas outlet, and a desorption gas outlet, each interface being connected to the integrated sealed cavity; the temperature control system controls the temperature of the adsorption system, enabling the sequential execution of a series of processes within the integrated gas ultrapurification device under the condition of an inert gas flow: preheating and activation of the adsorbent, low-temperature adsorption purification of the gas, high-temperature desorption regeneration, and cooling of the adsorbent for later use. The method of this invention is simple, easy to operate, and has broad industrial application prospects.

Description

Technical Field

[0001] This invention relates to the field of gas purification technology, and in particular to an integrated device and method for gas ultrapurification. Background Technology

[0002] As high-end industrial manufacturing, electronics and semiconductors, new energy, and precision chemicals continue to demand increasingly stringent requirements for gas purity and adsorbent activity, the demand for ultra-high purity gases (with impurity content below ppb or even ppt) is growing. Meanwhile, the activity state of the adsorbents, catalysts, and other materials used for purification directly determines the effectiveness and stability of gas purification.

[0003] In traditional technologies, gas ultrapurification and adsorbent activation / regeneration are typically separated. Gas purification relies on a separate purification tower, while adsorbent activation or regeneration requires transfer to a dedicated activation furnace. This "separate" processing mode requires two independent sets of equipment, increasing equipment investment and operational complexity. It also easily generates secondary pollution at pipeline connections, affecting gas purity. Furthermore, adsorbent activation requires removal from the purification equipment and transfer to the activation furnace. The transfer and secondary loading processes can easily cause adsorbent performance degradation and a decrease in adsorption capacity. Moreover, when the activated adsorbent is returned to the purification equipment, it can easily introduce external impurities, leading to fluctuations in gas purity. In addition, traditional devices often use single temperature field control, which cannot achieve the wide-range, high-precision temperature switching required for adsorption purification and desorption activation. This can easily lead to incomplete adsorption or insufficient desorption, wasted energy, and an inability to achieve continuous ultrapure gas supply. Based on this, the present invention provides an integrated device and method for gas ultrapurification, solving the problem that existing technologies cannot simultaneously achieve high-purity gas preparation and adsorbent activation. Summary of the Invention

[0004] This invention provides an integrated device and method for gas ultrapurification, aiming to solve the technical problem that existing technologies cannot simultaneously achieve high-purity gas preparation and adsorbent activation.

[0005] To achieve the above objectives, the present invention provides an integrated device for gas ultrapurification, comprising: an integrated sealed cavity.

[0006] The adsorption system is located inside the integrated sealed cavity, and the adsorption system is filled with at least one adsorbent.

[0007] The temperature control system is located inside the integrated sealed cavity and includes independent refrigerant circulation loops and heat transfer loops for temperature control of the adsorption system.

[0008] The gas pipeline system includes a raw material inlet, a displacement gas inlet, a product gas outlet, and a desorption gas outlet, each of which is connected to the integrated sealed cavity.

[0009] The temperature control system controls the temperature of the adsorption system, so that under the condition of introducing inert gas, the integrated gas ultrapurification device sequentially performs the following processes: preheating and activation of the adsorbent, low-temperature adsorption and purification of the gas, high-temperature desorption and regeneration, and cooling of the adsorbent for later use.

[0010] According to an embodiment of this application, the temperature control system controls the temperature of the adsorption system within a range of -80 to 350°C.

[0011] The refrigerant circulation loop is used to control the temperature of the adsorption system to -80~25℃.

[0012] The heat medium circulation loop is used to control the temperature of the adsorption system to 150~350℃.

[0013] According to an embodiment of this application, the adsorption system has a modular and replaceable structure.

[0014] The adsorbent includes one or more of molecular sieves, activated alumina, activated carbon, and metal-organic frameworks (MOFs).

[0015] According to an embodiment of this application, the integrated sealed cavity is made of a corrosion-resistant, low-desorption material.

[0016] The inner wall of the integrated sealed cavity is electrochemically polished, with a surface roughness Ra<10μm.

[0017] The gas pipeline system uses EP-grade stainless steel pipelines.

[0018] According to an embodiment of this application, the displacement gas inlet is used to introduce inert gas.

[0019] The inert gas is used for purging activation and impurity replacement.

[0020] The inert gas includes at least one of argon and nitrogen.

[0021] In the gas pipeline system, both the raw material inlet and the replacement gas inlet are equipped with filter components and one-way valves.

[0022] Both the product gas outlet and the analytical gas outlet are equipped with isolation valves.

[0023] The present invention also provides a method for gas ultrapurification, employing the aforementioned integrated gas ultrapurification device, comprising the following steps: S1: Start the heat medium circulation loop to heat the adsorption system to the first temperature, and at the same time, introduce inert gas from the displacement gas inlet for purging and activation.

[0024] S2: Switch to the refrigerant circulation loop, cool the adsorption system to the second temperature, then introduce raw material gas from the raw material inlet for low-temperature adsorption and purification, and obtain ultrapure gas from the product gas outlet. S3: When adsorption reaches saturation or the purity of the product gas falls below a set threshold, stop the supply of raw material gas. Switch to the heat medium circulation loop, heat the adsorption system to the third temperature, and introduce inert gas from the displacement gas inlet to discharge the desorbed impurity gas from the desorbed gas outlet.

[0025] S4: After the analysis is completed, switch back to the refrigerant circulation loop to cool the adsorption system to the second temperature and enter the next cycle.

[0026] According to an embodiment of this application, the first temperature is 180~350°C.

[0027] The second temperature is -80~-30℃.

[0028] The third temperature is 150~300℃.

[0029] According to the embodiments of this application, the analysis in step S3 and the activation in step S1 are combined. That is, after the impurities are analyzed at high temperature, the high temperature is maintained and the inert gas is switched to purge to complete the deep activation of the adsorbent.

[0030] The purging activation time is 1-3 hours.

[0031] According to an embodiment of this application, the volume ratio of water in the desorbed impurity gas is less than 100 ppb.

[0032] The concentration of impurities at the product gas outlet is monitored in real time by online mass spectrometry to determine the adsorption saturation state.

[0033] According to embodiments of this application, the method is used for gas ultrapurification in the fields of electronic semiconductors, precision chemicals, new energy, or scientific research experiments.

[0034] The feed gas includes electronic-grade arsine or silane.

[0035] The electronic-grade arsine has a purity of 99.999%, and impurities include H2O ≤ 5 ppm and O2 ≤ 3 ppm.

[0036] The silane contains >50 ppb of B and >50 ppb of P impurities.

[0037] The purity of the product gas is ppb or ppt.

[0038] Compared with the prior art, the beneficial effects of the present invention are: The aforementioned integrated device and method for gas ultrapurification integrates the adsorption system, temperature control system, and gas pipeline system into a single sealed cavity, and configures independent refrigerant and heat circulation loops. This enables continuous execution of processes such as adsorbent preheating and activation, low-temperature gas adsorption and purification, high-temperature desorption and regeneration, and cooling for later use within the same device. Compared to traditional technologies where adsorbent activation and gas purification are separated into independent devices and require multiple material transfers or disassemblies, this invention significantly simplifies the process flow, avoids the risk of secondary pollution and heat loss during material transfer, effectively reduces equipment footprint and energy costs, and improves the overall energy efficiency of gas ultrapurification operations. Furthermore, this invention employs a variable temperature control strategy to preheat and activate the adsorbent in situ under an inert gas atmosphere, ensuring that the adsorbent reaches its optimal activity state before use. Subsequently, precise temperature control achieves low-temperature deep adsorption and purification of the gas, effectively removing trace impurities from the raw gas. After adsorption saturation, high-temperature desorption and regeneration achieve efficient desorption and activity recovery of the adsorbent, which is then controlled and cooled to a ready-to-use state. This integrated closed-loop process not only ensures the high purity output of the product gas, but also significantly extends the service life of the adsorbent through in-situ activation-regeneration cycle, solving the technical bottleneck of the difficulty in simultaneously achieving high-purity gas preparation and adsorbent activation in existing technologies.

[0039] The apparatus and method of the present invention are simple, easy to operate, and capable of continuous production, and have broad prospects for industrial application. Attached Figure Description

[0040] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on the structures shown in these drawings without creative effort.

[0041] Figure 1 This is a structural diagram of the integrated gas ultrapurification device in Embodiment 1 of the present invention; Figure 2 This is a process flow diagram of the gas ultrapurification method in Embodiment 1 of the present invention; Figure 3 This is a process implementation diagram of the integrated gas ultrapurification device in Embodiment 1 of the present invention.

[0042] The attached figures are labeled as follows: 1. Integrated sealed cavity; 2. Adsorption system; 3. Temperature control system; 4. Refrigerant circulation loop; 5. Heat transfer fluid circulation loop; 6. Raw material gas inlet; 7. Replacement gas inlet; 8. Product gas outlet; 9. Desorption gas outlet; 10. Adsorbent replacement port; 11. Inlet pipe of refrigerant circulation loop; 12. Outlet pipe of refrigerant circulation loop; 13. Weight outlet pipe of refrigerant circulation loop; 14. Inlet pipe of heat transfer fluid circulation loop; 15. Outlet pipe of heat transfer fluid circulation loop; 16. Exhaust pipe of heat transfer fluid circulation loop; 17. Inner coil temperature measuring interface; 18. Inner cylinder temperature measuring interface; 19. Jacket temperature measuring interface.

[0043] The realization of the objective, functional characteristics and advantages of the present invention will be further explained in conjunction with the embodiments and with reference to the accompanying drawings. Detailed Implementation

[0044] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only a part of the embodiments of the present invention, and not all of them. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0045] The technical solutions of the various embodiments of the present invention can be combined with each other, but this must be based on the ability of those skilled in the art to implement them. When the combination of technical solutions is contradictory or cannot be implemented, it should be considered that such combination of technical solutions does not exist and is not within the scope of protection claimed by the present invention.

[0046] To achieve the above objectives, the present invention provides an integrated device for gas ultrapurification, comprising: an integrated sealed cavity.

[0047] The adsorption system is located inside the integrated sealed cavity, and the adsorption system is filled with at least one adsorbent.

[0048] The temperature control system is located inside the integrated sealed cavity and includes independent refrigerant circulation loops and heat transfer loops for temperature control of the adsorption system.

[0049] The gas pipeline system includes a raw material inlet, a displacement gas inlet, a product gas outlet, and a desorption gas outlet, each of which is connected to the integrated sealed cavity.

[0050] The temperature control system controls the temperature of the adsorption system, so that under the condition of introducing inert gas, the integrated gas ultrapurification device sequentially performs the following processes: preheating and activation of the adsorbent, low-temperature adsorption and purification of the gas, high-temperature desorption and regeneration, and cooling of the adsorbent for later use.

[0051] In some embodiments, see Figure 1 An integrated gas ultrapurification device is provided, specifically including an integrated sealed cavity 1, an adsorption system 2, a temperature control system 3, and a gas pipeline system. The integrated sealed cavity 1 serves as the supporting foundation of the entire device and is made of a corrosion-resistant and low-desorption material, which can effectively prevent the cavity material itself from contaminating the gas, while reducing the desorption of impurities on the material surface and ensuring the gas purification effect.

[0052] In some embodiments, to further reduce the risk of impurity adsorption and desorption, the inner wall of the integrated sealed cavity 1 is electrochemically polished, and the surface roughness Ra after the treatment is 1~10μm, which significantly improves the smoothness of the inner wall and reduces the sites for impurity adhesion.

[0053] In some embodiments, the adsorption system 2 is disposed inside the integrated sealed cavity 1, and is filled with at least one adsorbent. The adsorbent can be flexibly selected according to the type of raw gas and the type of impurities to achieve efficient adsorption of trace impurities in the raw gas. At the same time, the adsorption system 2 adopts a modular replaceable structure. When the activity of the adsorbent decreases to the point that it can no longer meet the purification requirements, the adsorption module can be quickly disassembled and replaced without disassembling the entire device, thereby improving the convenience of operation and reducing maintenance costs.

[0054] In some embodiments, the temperature control system 3 is disposed inside the integrated sealed cavity 1 and is the core component for realizing adsorbent activation, gas adsorption purification, desorption regeneration, and cooling. It includes independent refrigerant circulation loop 03 and hot refrigerant circulation loop 04, which can achieve precise temperature control of the adsorption system 2 to meet the temperature requirements of different processes. Specifically, the refrigerant circulation loop 03 is used to control the temperature of the adsorption system 2 at -80~25℃, which is suitable for the low-temperature gas adsorption purification and adsorbent cooling and standby processes; the hot refrigerant circulation loop 04 is used to control the temperature of the adsorption system 2 at 150~350℃, which is suitable for the adsorbent preheating activation and high-temperature desorption regeneration processes.

[0055] To achieve accurate temperature monitoring, in some embodiments, the integrated sealed cavity 1 is also equipped with an interface 101 for measuring the temperature of the inner coil, an interface 102 for measuring the temperature of the inner cylinder, and an interface 103 for measuring the temperature of the jacket. This allows for real-time monitoring of the temperature at different locations inside the cavity, facilitating adjustment of the temperature control system 3. Furthermore, the refrigerant circulation loop 03 is equipped with an inlet pipe 031, an outlet pipe 032, and a gravity outlet pipe 033. The heat transfer fluid circulation loop 04 is equipped with an inlet pipe 041, an outlet pipe 042, and an exhaust pipe 043, ensuring smooth circulation of the refrigerant and heat transfer fluid and system safety.

[0056] In some embodiments, the gas pipeline system is used to transport raw material gas, displacement gas, product gas, and desorption gas. It includes a raw material gas inlet 05, a displacement gas inlet 06, a product gas outlet 07, and a desorption gas outlet 08. Each inlet is connected to the integrated sealed cavity 1 to ensure orderly gas flow within the device. To ensure the cleanliness of the pipeline transport process, the gas pipeline system uses EP-grade stainless steel pipes, which effectively reduces the desorption of impurities from the inner wall of the pipes and avoids secondary contamination. Simultaneously, both the raw material gas inlet 05 and the displacement gas inlet 06 are equipped with filter components and one-way valves. The filter components pre-treat the raw material gas and displacement gas entering the device, removing large particulate impurities, while the one-way valves prevent gas backflow and ensure system stability. Both the product gas outlet 07 and the desorption gas outlet 08 are equipped with isolation valves, allowing flexible control of gas output and discharge according to process requirements. Furthermore, the integrated sealed cavity 1 is also equipped with an adsorbent replacement port 09 for easy replacement of the adsorption module.

[0057] The aforementioned integrated gas ultrapurification device integrates the adsorption system, temperature control system, and gas pipeline system into a single sealed cavity, and is equipped with independent refrigerant and heat circulation loops. This allows for the continuous execution of processes such as adsorbent preheating and activation, low-temperature gas adsorption and purification, high-temperature desorption and regeneration, and cooling for later use within the same device. Compared to traditional technologies where adsorbent activation and gas purification are handled in separate equipment and require multiple material transfers or disassemblies, this invention significantly simplifies the process flow, avoids the risk of secondary contamination and heat loss during material transfer, effectively reduces equipment footprint and energy costs, and improves the overall energy efficiency of gas ultrapurification operations. Furthermore, this invention employs a variable temperature control strategy to preheat and activate the adsorbent in situ under an inert gas atmosphere, ensuring that the adsorbent reaches its optimal activity state before use. Subsequently, precise temperature control enables low-temperature deep adsorption and purification of the gas, effectively removing trace impurities from the raw gas. After adsorption saturation, high-temperature desorption and regeneration achieve efficient desorption and activity recovery of the adsorbent, which is then controlled and cooled before being put into standby mode. This integrated closed-loop process not only ensures the high purity output of the product gas, but also significantly extends the service life of the adsorbent through in-situ activation-regeneration cycle, solving the technical bottleneck of the difficulty in simultaneously achieving high-purity gas preparation and adsorbent activation in existing technologies.

[0058] In some embodiments, the temperature control system controls the temperature of the adsorption system within a range of -80 to 350°C.

[0059] The refrigerant circulation loop is used to control the temperature of the adsorption system to -80~25℃.

[0060] The heat medium circulation loop is used to control the temperature of the adsorption system to 150~350℃.

[0061] In some embodiments, the temperature control system controls the temperature of the adsorption system within a range of -80 to 320°C.

[0062] The refrigerant circulation loop is used to control the temperature of the adsorption system to -80~-20℃.

[0063] The heat medium circulation loop is used to control the temperature of the adsorption system to 200~320℃.

[0064] In some embodiments, the adsorption system is a modularly replaceable structure.

[0065] The adsorbent includes one or more of molecular sieves, activated alumina, activated carbon, and metal-organic frameworks (MOFs).

[0066] In some embodiments, the adsorbent includes one or more of 13X molecular sieves, activated carbon, and metal-organic frameworks (MOFs).

[0067] In some embodiments, the adsorbent comprises 13X molecular sieve and activated carbon. It is used to remove H2O, O2, N2, and trace heavy metal carbonyl compounds from AsH3.

[0068] In some embodiments, the adsorbent comprises metal-organic framework materials (MOFs).

[0069] In some embodiments, the integrated sealed cavity is made of a corrosion-resistant, low-desorption material.

[0070] The inner wall of the integrated sealed cavity is electrochemically polished, with a surface roughness Ra<10μm.

[0071] The gas pipeline system uses EP-grade stainless steel pipelines.

[0072] In some embodiments, the displacement gas inlet is used to introduce inert gas.

[0073] The inert gas is used for purging activation and impurity replacement.

[0074] The inert gas includes at least one of argon and nitrogen.

[0075] In some embodiments, the flow rate of the inert gas is 1~8 L / min, and ultra-high purity nitrogen is introduced from the replacement gas inlet for purging and activation. The purging and activation is continued for 1~2 hours to activate the adsorbent to the initial high-performance state (the water content of the inner layer of the adsorbent is <10 ppm).

[0076] In some embodiments, the flow rate of the inert gas is 2 to 5 L / min.

[0077] In some embodiments, the gas pipeline system is equipped with a filter assembly and a one-way valve for both the raw material inlet and the displacement gas inlet.

[0078] Both the product gas outlet and the analytical gas outlet are equipped with isolation valves.

[0079] The apparatus and method of the present invention are simple, easy to operate, and capable of continuous production, and have broad prospects for industrial application.

[0080] The present invention also provides a method for gas ultrapurification, employing the aforementioned integrated gas ultrapurification device, comprising the following steps: S1: Start the heat medium circulation loop to heat the adsorption system to the first temperature, and at the same time, introduce inert gas from the displacement gas inlet for purging and activation.

[0081] S2: Switch to the refrigerant circulation loop, cool the adsorption system to the second temperature, then introduce raw material gas from the raw material inlet for low-temperature adsorption and purification, and obtain ultrapure gas from the product gas outlet. S3: When adsorption reaches saturation or the purity of the product gas falls below a set threshold, stop the supply of raw material gas. Switch to the heat medium circulation loop, heat the adsorption system to the third temperature, and introduce inert gas from the displacement gas inlet to discharge the desorbed impurity gas from the desorbed gas outlet.

[0082] S4: After the analysis is completed, switch back to the refrigerant circulation loop to cool the adsorption system to the second temperature and enter the next cycle.

[0083] In some embodiments, the first temperature is 180~350°C.

[0084] The second temperature is -80~-30℃.

[0085] The third temperature is 150~300℃.

[0086] In some embodiments, the first temperature is 180~300°C.

[0087] The second temperature is -60~-20℃.

[0088] The third temperature is 200~260℃.

[0089] In some embodiments, the analysis in step S3 is combined with the activation in step S1. That is, after the impurities are analyzed at high temperature, the high temperature is maintained and the process is switched to inert gas purging to complete the deep activation of the adsorbent.

[0090] The purging activation time is 1-3 hours.

[0091] In some embodiments, the volume ratio of water in the desorbed impurity gas is less than 100 ppb.

[0092] The concentration of impurities at the product gas outlet is monitored in real time by online mass spectrometry to determine the adsorption saturation state.

[0093] In some embodiments, the desorbed impurity gas is discharged from the desorbed gas exhaust port; the desorption process lasts for 1 to 2 hours.

[0094] In some embodiments, the method is used for gas ultrapurification in the fields of electronic semiconductors, fine chemicals, new energy, or scientific research experiments.

[0095] The feed gas includes electronic-grade arsine or silane.

[0096] The electronic-grade arsine has a purity of 99.999%, and impurities include H2O ≤ 5 ppm and O2 ≤ 3 ppm.

[0097] The silane contains >50 ppb of B and >50 ppb of P impurities.

[0098] The purity of the product gas is ppb or ppt.

[0099] In some embodiments, the method can be used for the purification and adsorbent regeneration of ultra-high purity arsine (AsH3) or for the deep removal of trace boron and phosphorus impurities in the production of silane (SiH4).

[0100] In some embodiments, the space velocity of arsine (feed gas) is 800 h⁻¹. -1 After continuous operation for 60-72 hours, the total impurity content at the product gas outlet was consistently <100 ppb, with H2O content <0.5 ppb and O2 content <2 ppb, meeting the ultra-high purity arsine (≥99.999999%) standard. Ultra-pure gas was obtained from the product gas outlet.

[0101] In some embodiments, the total downtime from the end of adsorption to the completion of regeneration and readiness for the next use is only 3 to 3.5 hours. Moreover, the entire regeneration process of the present invention is completed in a closed environment with a high-purity protective gas, ensuring the recovery of adsorbent activity while avoiding secondary pollution.

[0102] In some embodiments, the space velocity of silane (feed gas) is 800 h⁻¹. -1 After 72 hours of continuous operation, the product gas outlet was tested by an online laser trace moisture analyzer and GC-MS. The impurity content of element B was <0.1 ppb (100 ppt), which meets the requirements of advanced semiconductor manufacturing processes.

[0103] To further illustrate the present invention, the following examples are provided: Example 1 An integrated device for gas ultrapurification, see [link / reference] Figure 1 and Figure 3 This integrated gas purification unit, featuring a sealed chamber, is used for the purification and adsorbent regeneration of ultra-high purity arsine (AsH3). The raw material is electronic-grade arsine (99.999% purity), with main impurities being H2O ≤ 5 ppm and O2 ≤ 3 ppm.

[0104] The adsorption system is housed inside an integrated sealed cavity, which is filled with at least one adsorbent. The adsorbent is a composite adsorbent composed of 13X molecular sieve and activated carbon, used to remove H2O, O2, N2, and trace heavy metal carbonyl compounds from AsH3.

[0105] The temperature control system is located inside the integrated sealed cavity and includes independent refrigerant circulation loops and heat transfer fluid circulation loops for variable temperature control of the adsorption system. The refrigerant circulation loop uses liquid nitrogen with a temperature control of -80℃; the heat transfer fluid circulation loop uses high-temperature heat transfer oil with a temperature control of 320℃.

[0106] The gas pipeline system includes a raw material inlet, a displacement gas inlet, a product gas outlet, and a desorption gas outlet, each of which is connected to an integrated sealed cavity.

[0107] The temperature control system controls the temperature of the adsorption system, enabling the continuous processes of preheating and activation of the adsorbent, low-temperature adsorption and purification of the gas, high-temperature desorption and regeneration, and cooling of the adsorbent for later use to be executed sequentially within the integrated gas ultrapurification device under the condition of inert gas introduction.

[0108] See Figure 2 A method for gas ultrapurification, employing the aforementioned integrated gas ultrapurification device for the purification and adsorbent regeneration of ultra-high purity arsine (AsH3), comprises the following steps: S1: Start the heat medium circulation loop to heat the adsorption system to the first temperature of 280℃. At the same time, introduce ultra-high purity nitrogen (inert gas) at a flow rate of 5 L / min from the replacement gas inlet for purging and activation. Continue purging and activation for 2 hours to activate the adsorbent to the initial high-performance state (the water content of the inner layer of the adsorbent is <10 ppm).

[0109] S2: Switch to the refrigerant circulation loop, cool the adsorption system to the second temperature of -60℃, and maintain the temperature stability. Then, introduce arsine (raw material gas) through the raw material inlet for low-temperature adsorption and purification. The space velocity of the arsine (raw material gas) is 800 h⁻¹. -1 After 72 hours of continuous operation, the total impurity content at the product gas outlet was consistently <100 ppb, with H2O content <0.5 ppb and O2 content <2 ppb, meeting the ultra-high purity arsine (≥99.999999%) standard. Ultra-pure gas was obtained from the product gas outlet.

[0110] S3: When the adsorption reaches saturation, stop the feed gas supply; switch to the heat medium circulation loop, heat the adsorption system to the third temperature of 260℃, and introduce ultra-high purity nitrogen (inert gas) from the replacement gas inlet at a flow rate of 2 L / min, and discharge the desorbed impurity gas from the desorption gas exhaust port; the desorption process lasts for 1.5 hours.

[0111] S4: After the analysis is completed, switch back to the refrigerant circulation loop to cool the adsorption system to the second temperature of -60℃ and enter the next purification cycle.

[0112] In this embodiment 1, the total downtime from the end of adsorption to the completion of regeneration and readiness for the next use is only 3.5 hours. If the traditional method (disassembling the adsorbent to an external activation furnace) is used, this process would take at least 12 hours and carries the risk of adsorbent exposure and contamination. Furthermore, the entire regeneration process of this invention is completed in a closed environment with a high-purity protective gas supply, ensuring the restoration of adsorbent activity while avoiding secondary contamination.

[0113] Example 2 An integrated gas ultrapurification device is disclosed for the deep removal of trace boron and phosphorus impurities in silane (SiH4) production. The device features an integrated sealed chamber. The raw material is silane, with trace amounts of B2H6 and PH3 as the main impurities. The impurity content of boron is 50 ppb, the impurity content of phosphorus is 50 ppb, and the total impurity content is consistently maintained at 100 ppb.

[0114] The adsorption system is housed within an integrated sealed cavity, and the interior of the adsorption system is filled with at least one adsorbent. The adsorbent is a metal-organic framework (MOF).

[0115] The temperature control system is located inside the integrated sealed cavity and includes independent refrigerant circulation loops and heating medium circulation loops for variable temperature control of the adsorption system. The refrigerant circulation loop uses an ethylene glycol aqueous solution with a temperature control of -20℃; the heating medium circulation loop uses electric heating with a temperature control of 200℃.

[0116] The gas pipeline system includes a raw material inlet, a displacement gas inlet, a product gas outlet, and a desorption gas outlet, each of which is connected to an integrated sealed cavity.

[0117] The temperature control system controls the temperature of the adsorption system, enabling the continuous processes of preheating and activation of the adsorbent, low-temperature adsorption and purification of the gas, high-temperature desorption and regeneration, and cooling of the adsorbent for later use to be executed sequentially within the integrated gas ultrapurification device under the condition of inert gas introduction.

[0118] A method for gas ultrapurification, employing the aforementioned integrated gas ultrapurification device, is used for the deep removal of trace boron and phosphorus impurities in silane (SiH4) production. The steps are as follows: S1: Start the heat transfer medium circulation loop to heat the adsorption system to the first temperature of 180℃. Simultaneously, introduce ultra-high purity nitrogen (inert gas) at a flow rate of 5 L / min through the replacement gas inlet for purging and activation. Continue purging and activation for 1 hour to activate the adsorbent to its initial high-performance state (inner layer water content of the adsorbent <10 ppm). The adsorbent is a metal-organic framework (MOF) material.

[0119] S2: Switch to the refrigerant circulation loop, cool the adsorption system to the second temperature -20℃, and maintain the temperature stable. Then, introduce silane (raw material gas) through the raw material inlet for low-temperature adsorption and purification. The space velocity of silane (raw material gas) is 800 h⁻¹. -1 After 72 hours of continuous operation, the product gas outlet was tested by an online laser trace moisture analyzer and GC-MS. The impurity content of element B was <0.1 ppb (100 ppt), which meets the requirements of advanced semiconductor manufacturing processes.

[0120] S3: When the adsorption reaches saturation, stop the feed gas supply; switch to the heat medium circulation loop, heat the adsorption system to the third temperature of 200℃, and introduce ultra-high purity nitrogen (inert gas) from the replacement gas inlet at a flow rate of 2 L / min, and discharge the desorbed impurity gas from the desorption gas exhaust port; the desorption process lasts for 1 hour.

[0121] S4: After the analysis is completed, switch back to the refrigerant circulation loop to cool the adsorption system to the second temperature of -20℃ and enter the next purification cycle.

[0122] In Example 2, since MOFs materials are sensitive to temperature, the in-situ rapid thermal regeneration of the present invention avoids the collapse of the crystal structure caused by frequent transfer and long-term high-temperature treatment. The adsorption capacity still maintains more than 95% of the initial value after 100 consecutive cycles, while the adsorption capacity of the traditional external regeneration method will decrease to less than 80% after the same number of cycles, which proves the protective advantage of in-situ regeneration for sensitive materials.

[0123] The aforementioned integrated device and method for gas ultrapurification integrates the adsorption system, temperature control system, and gas pipeline system into a single sealed cavity, and configures independent refrigerant and heat circulation loops. This enables continuous execution of processes such as adsorbent preheating and activation, low-temperature gas adsorption and purification, high-temperature desorption and regeneration, and cooling for later use within the same device. Compared to traditional technologies where adsorbent activation and gas purification are separated into independent devices and require multiple material transfers or disassemblies, this invention significantly simplifies the process flow, avoids the risk of secondary pollution and heat loss during material transfer, effectively reduces equipment footprint and energy costs, and improves the overall energy efficiency of gas ultrapurification operations. Furthermore, this invention employs a variable temperature control strategy to preheat and activate the adsorbent in situ under an inert gas atmosphere, ensuring that the adsorbent reaches its optimal activity state before use. Subsequently, precise temperature control achieves low-temperature deep adsorption and purification of the gas, effectively removing trace impurities from the raw gas. After adsorption saturation, high-temperature desorption and regeneration achieve efficient desorption and activity recovery of the adsorbent, which is then controlled and cooled to a ready-to-use state. This integrated closed-loop process not only ensures the high purity output of the product gas, but also significantly extends the service life of the adsorbent through in-situ activation-regeneration cycle, solving the technical bottleneck of the difficulty in simultaneously achieving high-purity gas preparation and adsorbent activation in existing technologies.

[0124] The apparatus and method of the present invention are simple, easy to operate, and capable of continuous production, and have broad prospects for industrial application.

[0125] In summary, the above-described technical solutions of the present invention are merely preferred embodiments of the present invention and do not limit the patent scope of the present invention. All equivalent structural transformations made using the contents of the present invention's specification and drawings under the technical concept of the present invention, or direct / indirect applications in other related technical fields, are included within the patent protection scope of the present invention.

Claims

1. An integrated device for gas ultrapurification, characterized in that, include: Integrated sealed cavity; An adsorption system is disposed inside the integrated sealed cavity, and the adsorption system is filled with at least one adsorbent. A temperature control system, located inside the integrated sealed cavity, includes independent refrigerant circulation loops and heat transfer fluid circulation loops, used for variable temperature control of the adsorption system; The gas pipeline system includes a raw material inlet, a displacement gas inlet, a product gas outlet, and a desorption gas outlet, each of which is connected to the integrated sealed cavity. The temperature control system controls the temperature of the adsorption system, so that under the condition of introducing inert gas, the integrated gas ultrapurification device sequentially performs the following processes: preheating and activation of the adsorbent, low-temperature adsorption and purification of the gas, high-temperature desorption and regeneration, and cooling of the adsorbent for later use.

2. The integrated gas ultrapurification device according to claim 1, characterized in that, The temperature control system controls the temperature of the adsorption system within a range of -80 to 350°C. The refrigerant circulation loop is used to control the temperature of the adsorption system to -80~25℃; The heat medium circulation loop is used to control the temperature of the adsorption system to 150~350℃.

3. The integrated gas ultrapurification device according to claim 1, characterized in that, The adsorption system has a modular and replaceable structure; The adsorbent includes one or more of molecular sieves, activated alumina, activated carbon, and metal-organic frameworks (MOFs).

4. The integrated gas ultrapurification device according to claim 1, characterized in that, The integrated sealed cavity is made of a corrosion-resistant, low-desorption material; The inner wall of the integrated sealed cavity is electrochemically polished, with a surface roughness Ra<10μm; The gas pipeline system uses EP-grade stainless steel pipelines.

5. The integrated gas ultrapurification device according to claim 1, characterized in that, The displacement gas inlet is used to introduce inert gas; The inert gas is used for purging activation and impurity replacement; The inert gas includes at least one of argon and nitrogen; In the gas pipeline system, both the raw material inlet and the replacement gas inlet are equipped with filter components and one-way valves. Both the product gas outlet and the analytical gas outlet are equipped with isolation valves.

6. A method for gas ultrapurification, characterized in that, The integrated gas ultrapurification apparatus according to any one of claims 1 to 5 includes the following steps: S1: Start the heat medium circulation loop to heat the adsorption system to the first temperature, and at the same time, introduce inert gas from the replacement gas inlet for purging and activation. S2: Switch to the refrigerant circulation loop, cool the adsorption system to the second temperature, then introduce raw material gas from the raw material inlet for low-temperature adsorption and purification, and obtain ultrapure gas from the product gas outlet. S3: When the adsorption reaches saturation or the purity of the product gas is lower than the set threshold, stop the supply of raw material gas; switch to the heat medium circulation loop, heat the adsorption system to the third temperature, and introduce inert gas from the replacement gas inlet to discharge the desorbed impurity gas from the desorbed gas outlet. S4: After the analysis is completed, switch back to the refrigerant circulation loop to cool the adsorption system to the second temperature and enter the next cycle.

7. The gas ultrapurification method according to claim 6, characterized in that, The first temperature is 180~350℃; The second temperature is -80~-30℃; The third temperature is 150~300℃.

8. The gas ultrapurification method according to claim 6, characterized in that, The analysis in step S3 is combined with the activation in step S1. That is, after the impurities are analyzed at high temperature, the high temperature is maintained and the inert gas is switched to purge to complete the deep activation of the adsorbent. The purging activation time is 1-3 hours.

9. The gas ultrapurification method according to claim 6, characterized in that, The volume ratio of water in the extracted impurity gas is less than 100 ppb; The concentration of impurities at the product gas outlet is monitored in real time by online mass spectrometry to determine the adsorption saturation state.

10. The gas ultrapurification method according to any one of claims 6 to 9, characterized in that, The method is used for gas ultrapurification in the fields of electronic semiconductors, fine chemicals, new energy, or scientific research experiments. The raw material gas includes electronic-grade arsine or silane; The electronic-grade arsine has a purity of 99.999%, and impurities include H2O ≤ 5 ppm and O2 ≤ 3 ppm. The silane contains >50 ppb of B element impurities and >50 ppb of P element impurities. The purity of the product gas is ppb or ppt.

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