A separation system, separation method and application for carbonyl synthesis catalysts and carbonyl synthesis products.

By adjusting the combination and setup of chemical equipment, and utilizing the design of the evaporator lower head and cooler operating below the liquid level in the separator, the problem of long high-temperature residence time of the catalyst solution was solved, achieving efficient cooling of the catalyst and reducing energy consumption, thus extending the service life of the catalyst and ligands.

CN119925959BActive Publication Date: 2025-10-31CHINA PETROLEUM & CHEMICAL CORP +1
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Patent Information

Application Number
CN202311454343.0
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2023-11-03
Publication Date
2025-10-31
Estimated Expiration
2043-11-03

AI Technical Summary

Technical Problem

In existing technologies, during the separation process of carbonyl synthesis catalysts and products, the catalyst solution remains at high temperatures for a long time, resulting in a short ligand lifetime, requiring periodic replenishment. Furthermore, the separation process is energy-intensive, involves complex equipment, and incurs high operating costs.

Method used

By adjusting the combination of chemical equipment and utilizing the height difference between the evaporator, cooler, and separator, the catalyst solution can achieve the shortest residence time in the high-temperature region. The lower end cap of the evaporator is used for gas-liquid separation, and the cooler is set below the operating liquid level in the separator. By utilizing gravity flow and the principle of communicating vessels, catalyst entrainment and condensation are reduced, thus lowering energy consumption.

Benefits of technology

This technology enables efficient cooling of the catalyst solution, extends the service life of the catalyst and ligands, reduces operating costs and energy consumption, simplifies equipment structure, and improves system operating efficiency.

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Abstract

This invention provides a separation system, method, and application for separating carbonyl synthesis catalysts and carbonyl synthesis products. This invention utilizes only conventional chemical equipment combinations, adjusting the equipment elevation difference to achieve separation of the carbonyl synthesis catalyst and products. This minimizes the residence time of the catalyst solution in the high-temperature region and reduces the condensation of light components at the gas-liquid interface within the separation tank. The technical solution provided by this invention features low operating costs, simple equipment, low investment, and ease of operation and control.
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Description

Technical Field

[0001] This invention belongs to the field of carbonyl synthesis, specifically relating to a separation system, separation method and application of carbonyl synthesis catalyst and carbonyl synthesis product. Background Technology

[0002] Carbonyl synthesis is an addition reaction between carbon monoxide and organic compounds under the catalysis of organometallic compounds, producing aldehydes, acids, esters, etc.

[0003] Commonly used catalysts for carbonyl synthesis include rhodium, palladium, cobalt, platinum, copper, and nickel. Commonly used ligands are organophosphorus ligands, such as phosphate ester ligands, phosphite ester ligands, phosphine phosphate ligands, and oxamide phosphorus ligands. The reaction typically employs a homogeneous process, where olefins and CO, catalyzed by organometallic catalysts and ligands, insert a carbonyl group into the double bond of the olefin. However, organometallic catalysts and phosphorus ligands are sensitive to temperature changes and easily decompose at high temperatures, leading to a decrease in reaction rate. This necessitates periodic replenishment of ligands, increasing operating costs. Furthermore, when degraded ligands accumulate to a certain concentration, they need to be periodically discharged, requiring periodic catalyst unloading and regeneration, thus affecting the continuous operation of the unit.

[0004] To address the above issues, conventional catalyst-product separation methods employ... Figure 1a The process shown involves the reaction liquid (1') from carbonyl synthesis entering an evaporator (2'). In the evaporator (2'), the reaction liquid is heated, and the lighter components (mainly the product) become a gaseous phase. At the outlet of the evaporator (2'), a gas-liquid two-phase mixture is formed, which then enters a separator (3'). The gas and liquid phases are separated, and the gaseous phase (4') (mainly the product) passes through a demister inside the separator (3') and leaves as a crude product. The liquid phase at the bottom of the separator (mainly the catalyst), primarily a catalyst solution, is cooled by a cooler inside the separator and returned to the reaction zone as a catalyst solution (5') for recycling. Due to the limited coverage of the cooling coils (6') inside the separator and the low flow velocity of the fluid, heat transfer is slow, resulting in a long residence time of the catalyst solution (containing both catalyst and ligands) at high temperatures. This leads to a short ligand lifetime and a large ligand replenishment requirement.

[0005] For the conventional process 1a, current industry also adopts Figure 1b The method involves forced circulation of the catalyst solution (5') at the bottom of the separator (3') via a pump (9') at the bottom of the separator (3'), followed by cooling via an external cooler (6''). The solution is then divided into two parts: one part (5'a) returns to the separator, and the other part (5'b) returns to the reaction system. This method is similar to... Figure 1aCompared to the process shown, the residence time of the catalyst at low temperature is significantly shortened. However, the high-temperature gas phase at the gas-liquid interface of the separator (3') comes into contact with the cooled liquid phase, resulting in partial condensation, which reduces the amount of gas phase and ultimately leads to a greater heat load required for the evaporator (2'). Figure 1b The process employs a forced circulation cooling scheme, which requires the use of pumps for forced condensation. The circulation pumps have high power consumption, leading to increased power consumption and thus increased energy consumption of the entire system. Summary of the Invention

[0006] To address the problems existing in the prior art, this invention provides a novel method for separating carbonyl synthesis catalysts and carbonyl synthesis products. It utilizes only conventional chemical equipment combinations, adjusting the height difference between the equipment to achieve separation of the carbonyl synthesis catalyst and carbonyl synthesis products. This minimizes the residence time of the catalyst solution in the high-temperature region and reduces the condensation of light components at the gas-liquid interface within the separation tank. The method features low operating costs, simple equipment, low investment, and easy operation and control.

[0007] One objective of this invention is to provide a separation system for carbonyl synthesis catalysts and carbonyl synthesis products, comprising: an evaporator, a cooler, and a separation tank connected by pipelines, and optionally a receiving tank; wherein the highest point of the cooler is located below the operating liquid level of the separation tank.

[0008] According to the present invention, the evaporator is an evaporator separator, which can employ commonly used evaporator equipment in the art to achieve vaporization of light components in the reaction liquid and gas-liquid separation at the lower end cap. The evaporator is provided with an upper end cap and a lower end cap. The top of the upper end cap is provided with an inlet for the material to be separated, the bottom of the lower end cap is provided with a liquid phase outlet, and the side wall of the lower end cap is provided with a gas phase outlet.

[0009] According to the present invention, the cooler can be a cooler device commonly used in the art, and the material inlet of the cooler is connected to the liquid phase outlet at the bottom of the evaporator by a pipeline.

[0010] According to the present invention, the top cover of the separator is provided with a gas phase exhaust pipe; a gas phase inlet is provided on the side of the separator, which is connected to the gas phase outlet of the evaporator by a pipe; a liquid phase inlet is provided on the side of the separator below the gas phase inlet, which is connected to the outlet of the cooler by a pipe. A wire mesh demister is provided inside the separator near the top to reduce the amount of liquid phase entrained in the gas phase and reduce the entrainment loss of catalyst and ligands.

[0011] According to the present invention, the separation system is optionally provided with a receiving tank, which can be a material receiving device commonly used in the art.

[0012] According to one embodiment of the present invention, the separation system includes an evaporator, a cooler, and a separation tank connected by pipelines. The separation tank is divided into an upper section, a middle section, and a lower section from top to bottom. The upper section of the separation tank has a cylindrical structure, the middle section has an inverted conical structure, and the lower section has a cylindrical structure with a decreasing diameter. The upper end of the inverted conical section has the same dimensions as the upper cylindrical section, and its lower end has the same dimensions as the lower cylindrical section. A gas phase inlet is provided on the side of the upper section of the separation tank, connected by a pipeline to a gas phase outlet located on the side wall of the lower end cap of the evaporator. A liquid phase inlet is provided on the side of the lower section of the separation tank, connected by a pipeline to the cooler outlet. A liquid phase discharge pipeline is provided at the bottom of the lower section of the separation tank.

[0013] In the above embodiments, in the separator, the diameter ratio of the lower cylinder to the upper cylinder is less than 1, preferably (0.2~0.3):1; the upper side gas phase inlet of the separator is located at 1 / 8~1 / 2 of the upper cylinder from bottom to top, preferably 1 / 4~1 / 3; the lower side liquid phase inlet of the separator is located at 1 / 8~1 / 2 of the lower cylinder from bottom to top, preferably 1 / 8~1 / 4.

[0014] According to another embodiment of the present invention, the separation system further includes a receiving tank connected to a cooler by a pipeline, wherein the highest point of the cooler is located below the operating liquid level of the receiving tank; a liquid phase inlet is provided on the side of the receiving tank and connected to the cooler outlet by a pipeline; a liquid phase discharge pipeline is provided at the bottom of the receiving tank; a gas phase discharge pipeline is provided on the top cover of the receiving tank; the separation tank has a cylindrical structure; a gas phase inlet is provided on the side of the separation tank and connected to the gas phase outlet on the side wall of the lower end cap of the evaporator by a pipeline; a liquid phase outlet pipeline is provided at the bottom of the separation tank, which is connected to the liquid phase outlet pipeline provided at the bottom of the evaporator and connected to the cooler inlet.

[0015] In the above embodiments, the gas phase inlet of the separator tank side line is located at 1 / 10 to 3 / 4 of the separator tank from bottom to top, preferably 1 / 5 to 1 / 2; the liquid phase inlet of the receiving tank side line is located at 1 / 10 to 1 / 2 of the receiving tank from bottom to top, preferably 1 / 5 to 1 / 3; the gas phase exhaust pipe of the separator tank top cover is connected to the gas phase exhaust pipe of the receiving tank top cover.

[0016] The second objective of this invention is to provide a method for separating carbonyl synthesis catalysts and carbonyl synthesis products by employing the separation system described above.

[0017] According to the present invention, the separation method includes:

[0018] Method 1:

[0019] (1) The mixture after the carbonyl synthesis reaction enters the evaporator. In the evaporator, the carbonyl synthesis product is converted into a light component and evaporated into a gas phase. The solution containing the catalyst is in the liquid phase. Gas-liquid separation occurs at the lower end of the evaporator.

[0020] (2) The gas phase after gas-liquid separation in the evaporator enters the separation tank for further gas-liquid separation. Finally, the gas phase is discharged and the liquid phase enters the bottom of the separation tank.

[0021] (3) The liquid phase after gas-liquid separation in the evaporator enters the cooler for cooling. The cooled liquid phase enters the bottom of the separation tank and then the catalyst solution is discharged from the bottom of the separation tank and returned to the reaction system.

[0022] or,

[0023] Method 2:

[0024] (1) The mixture after the carbonyl synthesis reaction enters the evaporator. In the evaporator, the carbonyl synthesis product is converted into a light component and evaporated into a gas phase. The solution containing the catalyst is in the liquid phase. Gas-liquid separation occurs at the lower end of the evaporator.

[0025] (2) The gas phase after gas-liquid separation in the evaporator enters the separation tank for further gas-liquid separation. Finally, the gas phase is discharged and the liquid phase enters the bottom of the separation tank and is connected to the liquid phase discharge pipeline of the evaporator and sent to the cooler together.

[0026] (3) The liquid phase after gas-liquid separation in the evaporator and the liquid phase at the bottom of the separation tank enter the cooler for cooling. The cooled liquid phase enters the bottom of the receiving tank and then the catalyst solution is discharged from the bottom of the receiving tank and returned to the reaction system. The gas phase is discharged from the top of the receiving tank.

[0027] According to the present invention, in the separation method:

[0028] The carbonyl synthesis reaction is not particularly limited and can be a commonly used carbonyl synthesis reaction. For example, the carbonyl synthesis is at least one of hydroformylation, carbonyl esterification, and carbonyl oxidation.

[0029] The catalyst is not particularly limited and can be a catalyst commonly used in carbonyl synthesis reactions. For example, the catalyst is a metal ligand compound, preferably, the metal is selected from at least one of rhodium, palladium, cobalt, platinum, copper, and nickel; and / or, the ligand is selected from organophosphorus ligands, preferably from at least one of triphenylphosphine ligand, phosphate ester ligand, phosphite ester ligand, phosphine phosphate ligand, phosphine ligand, and oxamide phosphorus ligand.

[0030] The raw material for the carbonyl synthesis is an olefin compound, which can be a commonly used olefin compound in the field of carbonyl synthesis. For example, the raw material for the carbonyl synthesis is preferably selected from at least one of ethylene, propylene, butene, pentene, hexene, and octene.

[0031] According to the present invention, in the separation method, the operating conditions of the evaporator, cooler, and separation tank can be selected according to the product obtained from the specific carbonyl synthesis reaction and the catalyst used, with appropriate operating temperature and operating pressure. For example, the operating temperature of the evaporator can be selected in the range of 65~140°C, the operating conditions of the receiving tank are the same as those of the evaporator, and the outlet temperature of the cooler can be controlled to be no higher than 60°C.

[0032] The third objective of this invention is to provide a separation system or method for separating the carbonyl synthesis catalyst and carbonyl synthesis product, and its application in carbonyl synthesis reactions.

[0033] This invention provides a method for separating carbonyl synthesis catalysts and products. The reaction liquid of carbonyl synthesis enters an evaporator, where the carbonyl synthesis product is converted into a light component and evaporated into a gas phase. The catalyst solution is in the liquid phase. Gas-liquid separation occurs at the lower end of the evaporator. The gas phase enters a separation tank for further gas-liquid separation. Finally, the gas phase is discharged, and the liquid phase enters the bottom of the separation tank. The liquid phase (catalyst solution) at the lower end of the evaporator enters a cooler for cooling. The highest point of the cooler needs to be located below the operating liquid level in the separation tank to ensure that the catalyst solution always fills the cooler. After cooling, the catalyst solution enters the bottom of the separation tank and is then discharged back into the reaction system.

[0034] This invention combines conventional chemical equipment such as evaporators, coolers, and separation tanks. The evaporator's lower end cap performs the first gas-liquid separation, and the gas phase enters the separation tank for a second, deeper separation to reduce catalyst entrainment. The catalyst solution enters the cooler's tube side under its own gravity, is immediately cooled, and then enters the separation tank using the communicating vessel principle. The bottom of the separation tank reduces gas-liquid contact through a narrowing or additional receiving tank, ultimately achieving the separation of the carbonyl synthesis catalyst from the product. This invention is applicable to the separation of carbonyl synthesis catalysts, where the carbonyl synthesis reactions include hydroformylation, carbonyl esterification, and carbonyl oxidation.

[0035] In the separation system provided by this invention, the carbonyl synthesis reaction liquid passes through an evaporator to obtain a gas-liquid two-phase mixture. The gas and liquid phases are directly separated at the lower end of the evaporator. The liquid phase, under gravity, enters a cooler for cooling before entering the lower section of the separation tank. This allows the catalyst solution to cool down in the shortest possible time. Simultaneously, the catalyst solution flows due to the height difference and gravity, resulting in energy savings and convenient control. Furthermore, the cooler is positioned below the operating liquid level in the separation tank, ensuring the liquid always submerges the heat exchanger and keeps the catalyst solution constantly cooled. If the cooler is positioned above the liquid level in the separation tank, the catalyst solution will pass through the cooler too quickly, resulting in insufficient cooling time and inadequate cooling effect, which affects the lifespan of the catalyst and ligands. The carbonyl synthesis catalyst separation system and method of this invention can effectively separate the carbonyl synthesis catalyst from the product, while also protecting the catalyst and ligand lifespan, increasing their recycling value, reducing catalyst replenishment, and facilitating industrial energy conservation due to low energy consumption. Attached Figure Description

[0036] Figure 1a ~b is a schematic diagram of a separation device in the prior art.

[0037] Figure 2 This is a schematic diagram of the separation device used in Example 1. Figure 2 In the diagram, 1-Inlet for material to be separated, 2-Evaporator, 3-Cooler, 4-Separation tank, 5-Separation tank gas phase discharge pipeline, 6-Separation tank liquid phase discharge pipeline, 7-Evaporator upper end cap, 8-Evaporator lower end cap, 9-Evaporator side line gas phase outlet, 10-Separation tank side line gas phase inlet, 11-Evaporator liquid phase outlet, 12-Separation tank side line liquid phase inlet, 13-Wire mesh demister.

[0038] Figure 3 This is a schematic diagram of the separation device used in Example 2. Figure 3 In the diagram, 1-Inlet for material to be separated, 2-Evaporator, 3-Cooler, 4-Separation tank, 5-Separation tank gas phase discharge pipeline, 6-Separation tank liquid phase discharge pipeline, 7-Evaporator upper head, 8-Evaporator lower head, 9-Evaporator side gas phase outlet, 10-Separation tank side gas phase inlet, 11-Evaporator liquid phase outlet, 13-Wire mesh demister, 14-Receiving tank, 15-Receiving tank liquid phase inlet, 16-Receiving tank gas phase outlet, 17-Receiving tank liquid phase outlet. Detailed Implementation

[0039] The present invention will now be described in detail with reference to specific embodiments. It should be noted that the following embodiments are only used to further illustrate the present invention and should not be construed as limiting the scope of protection of the present invention. Some non-essential improvements and adjustments made by those skilled in the art based on the content of the present invention are still within the scope of protection of the present invention.

[0040] Example 1

[0041] The following is combined Figure 2 This invention describes the separation system and method for carbonyl synthesis catalysts and carbonyl synthesis products provided by this invention.

[0042] like Figure 2 As shown, the separation system for carbonyl synthesis catalyst and carbonyl synthesis product includes: an evaporator 2, a cooler 3, and a separation tank 4 connected by pipelines. The evaporator 2 has a material inlet 1 at its top and a liquid phase outlet 11 at its bottom. Inside, there is an upper evaporator head 7 and a lower evaporator head 8. A side-line gas phase outlet 9 is located on the side wall of the lower evaporator head 8. The cooler 3's material inlet is connected to the liquid phase outlet 11 at the bottom of the evaporator via a pipeline, and its material outlet is connected to the side-line liquid phase inlet 12 of the lower section of the separation tank via a pipeline. The top cover of the separation tank 4 has a gas phase exhaust pipeline 5, and a wire mesh demister 13 is installed at the gas phase outlet. The highest point of the cooler 3 is below the operating liquid level of the separation tank 4. The separation tank 4 is divided into an upper section, a middle section, and a lower section from top to bottom. The upper section is a cylindrical structure, the middle section is an inverted conical structure, and the lower section is a cylindrical structure with a decreasing diameter. The upper section of the separator 4 is equipped with a separator side gas inlet 10, which is connected to the evaporator side gas outlet 9 of the evaporator by a pipeline; the upper end of the middle section inverted cone has the same size as the upper section cylinder, and the lower end has the same size as the lower section cylinder; the bottom of the lower section of the separator 4 is equipped with a separator liquid phase discharge pipeline 6.

[0043] The diameter of the lower cylindrical section of the separator is 1 / 4 of the diameter of the upper cylindrical section; the gas phase inlet 10 of the separator is located at 1 / 8 of the upper cylindrical section from bottom to top; and the liquid phase inlet 12 of the lower cylindrical section is located at 1 / 8 of the lower cylindrical section from bottom to top.

[0044] Using the above Figure 2 The separation system separates the carbonyl synthesis catalyst from the carbonyl synthesis product. Specific separation methods include:

[0045] (1) Ethylene and syngas (hydrogen and carbon monoxide in a molar ratio of 1:1) undergo carbonyl synthesis reaction to produce propionaldehyde under the action of rhodium acetate catalyst and triphenylphosphine ligand. The conditions for carbonyl synthesis reaction are: reaction temperature 72℃ and reaction pressure 1.2MPaG.

[0046] (2) After passing through evaporator 2, about 3 / 4 of the carbonyl reaction products are vaporized and enter separation tank 4 through the side gas outlet 9 of the evaporator for further gas-liquid separation. The separated gas phase is discharged and the liquid phase enters the bottom of the separation tank. The operating conditions of the evaporator are: operating temperature 90℃ and operating pressure 0.08MPaG.

[0047] (3) The remaining 1 / 4 of the catalyst solution in evaporator 2, at a temperature of about 90°C, enters the cooler 3 through the bottom pipe of evaporator 2 and is cooled to 60°C. Then it enters the bottom of the lower cylindrical structure of the separator 4. The catalyst obtained from the secondary gas-liquid separation in the separator is discharged from the bottom of the system and returned to the reaction system for recycling.

[0048] In the entire separation system, only a small section of catalyst solution at 90°C accumulates in the pipeline at the same level as the liquid level in the lower section of the separator in the inlet pipeline from the cooler to the cooler. This section accounts for about 1 to 2% of the volume of the catalyst solution. The remaining catalyst temperature is all below 60°C. The proportion of catalyst in the high-temperature section is the smallest. The low temperature is very beneficial to the life of the catalyst and the stability of the ligands. It can extend the amount of catalyst and ligands to be added to the unit and extend the long-term operation time of the unit.

[0049] Example 2

[0050] The following is combined with Figure 3 This invention describes the separation system and method for carbonyl synthesis catalysts and carbonyl synthesis products provided by this invention.

[0051] like Figure 3 As shown, the separation system for carbonyl synthesis catalyst and carbonyl synthesis product includes: an evaporator 2, a cooler 3, a separation tank 4, and a receiving tank 14 connected by pipelines. The evaporator 2 has a material inlet 1 at the top and a liquid phase outlet 11 at the bottom. Inside, there is an upper evaporator head 7 and a lower evaporator head 8. A side-line gas phase outlet 9 is located on the side wall of the lower evaporator head 8. The cooler 3's material inlet is connected to the liquid phase outlet 11 at the bottom of the evaporator by a pipeline, and its material outlet is connected to the side-line receiving tank liquid phase inlet 15 of the receiving tank 14 by a pipeline. The top cover of the separation tank 4 has a separation tank gas phase exhaust pipeline 5, and the gas phase outlet is equipped with a wire mesh demister 13. A side-line separation tank gas phase inlet 10 is located on the side of the separation tank 4 and is connected by a pipeline to the evaporator side-line gas phase outlet 9 of the evaporator 2. The highest point of the cooler 3 is located below the operating liquid level of the separator 4 and the receiving tank 14. The separator 4 has a cylindrical structure. The liquid phase discharge pipe 6 at the bottom of the separator 4 is connected to the liquid phase outlet pipe at the bottom of the evaporator 2, and is connected to the inlet of the cooler 3. The receiving tank 14 has a receiving tank liquid phase outlet 17 at the bottom and a receiving tank gas phase outlet 16 on the top cover of the receiving tank 14, which is connected to the separator tank gas phase discharge pipe 5 on the top cover of the separator 4. The separator tank side gas phase inlet 10 is located at 1 / 8 of the separator tank from bottom to top; the receiving tank liquid phase inlet 15 is located at 1 / 4 of the receiving tank from bottom to top.

[0052] Using the above Figure 3 The separation system separates the carbonyl synthesis catalyst from the carbonyl synthesis product. Specific separation methods include:

[0053] (1) Propylene reacts with synthesis gas (hydrogen and carbon monoxide in a molar ratio of 1:1) under the action of rhodium acetylacetone catalyst and triphenylphosphine ligand to produce butyraldehyde. The reaction temperature is 80℃ and the reaction pressure is 1.35 MPaG.

[0054] (2) After the reaction products pass through evaporator 2, about 3 / 4 of the products are vaporized and enter the separator 4 through the side line of the lower end cap of evaporator 2 for further gas-liquid separation. The gas phase after the secondary separation in the separator is discharged, and the liquid phase enters the cooler 3. The operating conditions of the evaporator are: operating temperature 100℃ and operating pressure 0.08MPaG.

[0055] (3) The remaining 1 / 4 of the catalyst solution in evaporator 2, at a temperature of about 100°C, enters cooler 3 through the bottom pipe of evaporator 2 and is cooled to 60°C. Then it enters receiving tank 14. The catalyst is discharged from the bottom of the receiving tank and returned to the reaction system for recycling.

[0056] In the entire separation system, only a small section of catalyst solution at 100°C accumulates in the pipeline from the cooler to the cooler inlet at the same level as the lower section of the receiving tank. This section accounts for about 1-2% of the volume of the catalyst solution. The remaining catalyst temperature is below 60°C. The proportion of catalyst in the high-temperature section is the smallest. The low temperature is very beneficial to the life of the catalyst and the stability of the ligands. It can extend the amount of catalyst and ligands that can be added to the unit and extend the long-term operation time of the unit.

[0057] Comparative Example 1

[0058] The following is combined with Figure 1a Explain the existing methods for separating carbonyl synthesis catalysts from carbonyl synthesis products.

[0059] The carbonyl reaction product (same as in Example 1) 1′ enters the evaporator 2′ for separation of the catalyst and the product. The separated gas and liquid phases enter the separation tank 3′ for further gas-liquid phase separation. The gas phase product 4′ is discharged from the top of the separation tank, and the catalyst solution enters the lower part of the separation tank 3′ to form a certain liquid level. The separation tank 3′ has a built-in cooler 6′. Figure 1a The portion of the catalyst solution above the cooler is not yet cooled, while the portion below the cooler is cooled. Typically, at least 1 / 3 of the catalyst solution is not cooled and is in the high-temperature section, while 2 / 3 of the catalyst solution is cooled and is in the low-temperature section. At the same time, due to the large diameter of the separator and the low liquid flow rate, the heat transfer coefficient of the catalyst solution when it comes into contact with the cooler is small, resulting in a slow cooling rate.

[0060] Compared with Examples 1 and 2, the catalyst solution in Comparative Example 1 was in the high-temperature region, accounting for more than 1 / 3 of the catalyst solution, while in Examples 1 and 2, the catalyst solution in the high-temperature region accounted for only 1-2%. Examples 1 and 2 have a significant advantage in extending the service life of the catalyst and ligands.

[0061] Comparative Example 2

[0062] The following is combined Figure 1b Explain the existing methods for separating carbonyl synthesis catalysts from carbonyl synthesis products.

[0063] The carbonyl reaction product (same as in Example 1) 1′ enters the evaporator 2′ for catalyst and product separation. The separated gas and liquid phases enter the separation tank 3′ for further gas-liquid phase separation. The gas phase product 4′ is discharged from the top of the separation tank, and the catalyst solution enters the lower part of the separation tank 3′, forming a certain liquid level. The catalyst solution 5′ is discharged from the separation tank 3′ and enters the catalyst pump 9′. The catalyst solution at the pump outlet enters the cooler 6′ for cooling. After cooling, part of the catalyst 5′b is returned to the reaction system, and part of the catalyst 5′a is returned to the separation tank 3′ to mix and cool with the high-temperature catalyst from the evaporator 2′.

[0064] Comparative Example 2 used a catalyst pump. Since the reaction pressure of conventional carbonyl synthesis is greater than 1.0 MPaG, the head of the catalyst pump is typically greater than 120 m. Part of the catalyst solution is returned to the separator, resulting in significant energy consumption. Furthermore, in Comparative Example 2, to cool the catalyst in separator 3', the amount of catalyst in 5'a typically needs to be 2-3 times greater than the amount entering separator 3', leading to a larger catalyst circulation flow rate in 5'a and higher energy consumption. Additionally, because separator 3' has a larger diameter, fluid mixing is prone to unevenness, forming localized high-temperature dead zones, causing localized catalyst overheating and affecting catalyst lifespan. Moreover, the uniform diameter of separator 3' results in a large surface area of ​​the catalyst solution. Upon contact with the gas phase space in separator 3', the gas phase cools at the liquid surface, leading to product cooling and further high energy consumption. Compared to Examples 1-2, Comparative Example 2 has a more complex process and requires more electricity and energy.

Claims

1. A separation system for carbonyl synthesis catalysts and carbonyl synthesis products, comprising: An evaporator, a cooler, and a separator are connected by pipelines. The highest point of the cooler is located below the operating liquid level of the separator. The evaporator has an upper head and a lower head. The top of the upper head is provided with an inlet for the material to be separated, the bottom of the lower head is provided with a liquid phase outlet, and the side wall of the lower head is provided with a gas phase outlet. The material inlet of the cooler is connected to the liquid phase outlet at the bottom of the evaporator by a pipeline. A gas phase inlet is provided on the side of the separator and is connected to the gas phase outlet of the evaporator by a pipeline. A liquid phase inlet is provided on the side of the separator below the gas phase inlet and is connected to the cooler outlet by a pipeline.

2. The separation system according to claim 1, characterized in that, The top cover of the separator is equipped with a gas phase exhaust pipeline; and / or, A wire mesh demister is installed inside the upper section near the top of the separation tank.

3. The separation system according to claim 2, characterized in that, In the aforementioned separation system, the separation tank is divided into an upper section, a middle section, and a lower section from top to bottom; The upper section of the separation tank is a cylindrical structure, the middle section is an inverted conical structure, and the lower section is a cylindrical structure with a decreasing diameter. The upper side of the separator is provided with a gas phase inlet, which is connected by a pipeline to a gas phase outlet provided on the side wall of the lower end cap of the evaporator. The lower side of the separator is provided with a liquid phase inlet, which is connected to the cooler outlet by a pipeline; A liquid phase discharge pipeline is installed at the bottom of the lower section of the separator.

4. The separation system according to claim 3, characterized in that, In the separation tank, the ratio of the diameter of the lower cylinder to the diameter of the upper cylinder is less than 1; and / or, The gas phase inlet of the upper section of the separator is located at 1 / 8 to 1 / 2 of the upper cylindrical section of the separator from bottom to top; and / or, The side-line liquid phase inlet of the lower section of the separator is located at 1 / 8 to 1 / 2 of the bottom of the cylindrical section of the lower section of the separator.

5. The separation system according to claim 4, characterized in that, In the separation tank, the diameter ratio of the lower cylindrical section to the upper cylindrical section is (0.2~0.3):1; and / or, The gas phase inlet of the upper section of the separator is located at 1 / 4 to 1 / 3 of the upper cylindrical section of the separator from bottom to top; and / or, The liquid phase inlet of the lower section of the separator is located at 1 / 8 to 1 / 4 of the height of the lower cylindrical section of the separator from bottom to top.

6. A method for separating carbonyl synthesis catalyst and carbonyl synthesis product, wherein the separation of carbonyl synthesis catalyst and carbonyl synthesis product is performed by employing the separation system described in any one of claims 1 to 5.

7. The separation method according to claim 6, characterized in that, The separation method includes: (1) The mixture after the carbonyl synthesis reaction enters the evaporator. In the evaporator, the carbonyl synthesis product is converted into a light component and evaporated into a gas phase. The solution containing the catalyst is in the liquid phase. Gas-liquid separation occurs at the lower end of the evaporator. (2) The gas phase after gas-liquid separation in the evaporator enters the separation tank for further gas-liquid separation. Finally, the gas phase is discharged and the liquid phase enters the bottom of the separation tank. (3) The liquid phase after gas-liquid separation in the evaporator enters the cooler for cooling. The cooled liquid phase enters the bottom of the separation tank and then the catalyst solution is discharged from the bottom of the separation tank and returned to the reaction system.

8. The separation method according to claim 7, characterized in that, The carbonyl synthesis is at least one of hydroformylation, carbonyl esterification, and carbonyl oxidation; and / or, The catalyst is a metal ligand compound; and / or, The raw materials for the carbonyl synthesis are olefin compounds.

9. The separation method according to claim 8, characterized in that, In the aforementioned metal ligand compound, the metal is selected from at least one of rhodium, palladium, cobalt, platinum, copper, and nickel; and / or, the ligand is selected from organophosphorus ligands; and / or, The raw materials for the carbonyl synthesis are selected from at least one of ethylene, propylene, butene, pentene, hexene, and octene.

10. The separation method according to claim 9, characterized in that, The ligand is selected from at least one of triphenylphosphine ligand, phosphate ester ligand, phosphite ester ligand, phosphine phosphate ligand, phosphine ligand, and oxamidophosphine ligand.

11. The application of a separation system for carbonyl synthesis catalyst and carbonyl synthesis product according to any one of claims 1 to 5 or a separation method for carbonyl synthesis catalyst and carbonyl synthesis product according to any one of claims 6 to 10 in a carbonyl synthesis reaction.

Citation Information

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