A carbon monoxide purification process and purification apparatus

Abstract

The application discloses a carbon monoxide purification process and a purification device, wherein the carbon monoxide purification process comprises the following steps: decomposing carbonyl nickel into carbon monoxide and elemental nickel powder in a decomposition tower, collecting carbon monoxide with high purity from the decomposition tower, flowing the elemental nickel powder and the carbonyl nickel into a synthesis tower, adding carbon monoxide raw material with low purity to be purified into the synthesis tower, reacting the nickel powder and the carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, discharging impurities in the carbon monoxide raw material in the synthesis tower, and flowing the carbonyl nickel into the decomposition tower again to decompose carbon monoxide with high purity. Through the synthesis and decomposition reactions, the carbon monoxide raw material with low purity is purified, carbon monoxide with higher purity can be obtained, the carbon monoxide is beneficial to use in the integrated circuit and semiconductor industries, the purification process is relatively simple, the carbonyl nickel can be recycled, and the purification cost is relatively low.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of carbon monoxide production, in particular to a carbon monoxide purification process and purification equipment. BACKGROUND

[0002] With the rapid development of the industry and the semiconductor industry, high-purity carbon monoxide is used more and more in the field of semiconductor chip etching gas, and high-purity carbon monoxide with a purity of 5N (99.999%) or above is often required in the integrated circuit and semiconductor industry, so it is of great significance to produce high-purity carbon monoxide. At present, there are three main methods for producing carbon monoxide: first, using coke, oxygen and carbon dioxide as raw materials to prepare carbon monoxide under high-temperature catalyst conditions, and obtaining carbon monoxide with a purity of about 98% after purification. This method produces carbon monoxide with low purity and complex impurities; second, using methanol to crack at high temperature and then using pressure swing adsorption to purify carbon monoxide to obtain carbon monoxide with a purity of 99%. The shortcomings are that the methanol cracking catalyst is expensive, and the purity is unstable and the utilization rate is not high in production; third, using formic acid to dehydrate under the catalytic action of concentrated sulfuric acid to obtain carbon monoxide gas, and then obtaining carbon monoxide products with a purity of 99.9% through condensation, water washing, alkali washing, acid washing and adsorption purification processes.

[0003] Although there are many methods for producing carbon monoxide at present, the purity of carbon monoxide can only reach 4N (99.99%), and it is very difficult to further improve the purity to 5N or above, which limits the application of carbon monoxide in the integrated circuit and semiconductor industry. Therefore, it is necessary to study a new purification process and equipment to obtain carbon monoxide with higher purity. SUMMARY

[0004] The main purpose of the present application is to provide a carbon monoxide purification process and purification equipment, which aims to solve the technical problem that the purity of carbon monoxide produced by the prior art needs to be further improved.

[0005] To achieve the above-mentioned purpose, the present application provides a carbon monoxide purification process, which comprises the following steps:

[0006] S1: injecting carbonyl nickel into the synthesis tower and the decomposition tower, wherein the synthesis tower and the decomposition tower are connected through a first pipeline and a second pipeline, the first pipeline is provided with a first control valve, the second pipeline is provided with a second control valve, the first pipeline connects the bottom of the synthesis tower and the upper middle part of the decomposition tower, the second pipeline connects the bottom of the decomposition tower and the upper middle part of the synthesis tower, and a circulating pump is arranged on the second pipeline, and the feeding direction of the circulating pump is from the decomposition tower to the synthesis tower;

[0007] S2: introducing the carbon monoxide raw material to be purified into the synthesis tower, increasing the pressure in the synthesis tower to a set first pressure value, and the pressure in the decomposition tower is less than or equal to the first pressure value, then opening the first control valve, the second control valve and the circulating pump, so that the nickel carbonyl in the synthesis tower flows to the decomposition tower through the first pipeline, and the nickel carbonyl in the decomposition tower flows to the synthesis tower through the second pipeline;

[0008] S3: continuously introducing the carbon monoxide raw material to be purified into the synthesis tower, maintaining the pressure in the synthesis tower at the first pressure value, keeping the circulating pump running, controlling the temperature in the synthesis tower at a set synthesis temperature, heating the decomposition tower and maintaining it at a set decomposition temperature, so that the nickel carbonyl in the decomposition tower decomposes to generate carbon monoxide and nickel powder, collecting the carbon monoxide generated by decomposition from the upper part of the decomposition tower, while the nickel powder generated by decomposition and the un-decomposed nickel carbonyl in the decomposition tower are extracted into the synthesis tower through the circulating pump on the second pipeline, and the nickel powder reacts with the carbon monoxide to be purified in the synthesis tower to generate nickel carbonyl, forming a continuous reaction cycle.

[0009] The carbon monoxide purification process utilizes the reaction of elemental nickel and carbon monoxide at low temperature to synthesize nickel carbonyl, and the decomposition of nickel carbonyl at high temperature into elemental nickel and carbon monoxide, and the specific synthesis and decomposition reaction formulae are as follows:

[0010]

[0011] Through the above synthesis and decomposition reactions, the nickel carbonyl is decomposed into carbon monoxide and elemental nickel powder in the decomposition tower, and high-purity carbon monoxide can be collected from the decomposition tower. The low-purity carbon monoxide raw material to be purified is added to the synthesis tower, the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize nickel carbonyl, while the impurities in the carbon monoxide raw material remain in the synthesis tower and are discharged. The nickel carbonyl then flows to the decomposition tower to decompose high-purity carbon monoxide. Through the synthesis and decomposition reactions, the low-purity carbon monoxide raw material is purified, high-purity carbon monoxide is obtained, which is beneficial to use in the integrated circuit and semiconductor industries, and the purification process is simple, the nickel carbonyl can be recycled, and the purification cost is low.

[0012] Preferably, in step S2, the first pressure value is 1-3 MPa, the pressure in the decomposition tower is 1-3 MPa, and the first control valve and the second control valve are adjusted to control the flow of materials in the first pipeline and the second pipeline respectively, so that a material circulation balance is formed between the synthesis tower and the decomposition tower.

[0013] The pressure in the decomposition tower is less than or equal to the pressure in the synthesis tower, so that the carbonyl nickel in the synthesis tower can flow into the decomposition tower by itself through the first pipeline, and the appropriate pressure in the tower during the reaction can increase the boiling point of the carbonyl nickel and reduce the gasification of the carbonyl nickel.

[0014] Preferably, the liquid content of the synthesis tower and the decomposition tower is controlled to be no less than 30% of the tower volume.

[0015] The liquid content of the synthesis tower and the decomposition tower is greater than or equal to 30%, which can balance the material circulation of the two towers.

[0016] Preferably, in step S3, when the pressure in the synthesis tower is greater than or equal to the first pressure value, the pressure in the synthesis tower is reduced by discharging the impure gas in the synthesis tower. In this way, while maintaining the pressure in the synthesis tower, the amount of carbon monoxide raw material can be maintained, and the accumulated impure gas can be discharged.

[0017] Preferably, before discharging the impure gas in the synthesis tower, a step of cooling the impure gas to condense the carbonyl nickel mixed in the impure gas is further included.

[0018] Cooling the impure gas before discharging can condense the gaseous carbonyl nickel mixed in the impure gas and return it to the synthesis tower, reducing the loss of carbonyl nickel in the purification process.

[0019] Preferably, before collecting the carbon monoxide generated by decomposition in the decomposition tower in step S3, a step of cooling the carbon monoxide generated by decomposition to condense the carbonyl nickel mixed in the carbon monoxide is further included.

[0020] Cooling the carbon monoxide before discharging can condense the gaseous carbonyl nickel mixed in the carbon monoxide and return it to the decomposition tower, further improving the purity of the collected carbon monoxide and reducing the loss of carbonyl nickel in the purification process.

[0021] Preferably, in step S3, a step of cooling the mixed liquid of carbonyl nickel and nickel powder in the second pipeline is further included, so that the temperature of the mixed liquid flowing into the synthesis tower is 50-90°C.

[0022] Since the temperature in the decomposition tower is higher than the temperature in the synthesis tower, the temperature of the nickel powder and the carbonyl nickel generated by decomposition in the decomposition tower is also higher, so the cooling is performed when the mixed liquid is extracted from the second pipeline to the synthesis tower by the circulating pump, so that the temperature of the mixed liquid of carbonyl nickel and nickel powder is basically consistent with the temperature in the synthesis tower when it enters the synthesis tower, reducing the influence on the reaction process caused by the influence on the temperature in the synthesis tower.

[0023] In another aspect of the present application, a purification device is provided, which comprises a synthesis tower and a decomposition tower, the synthesis tower is provided with a raw material inlet for adding carbon monoxide raw material to be purified, the upper side of the synthesis tower is further provided with a mixed gas outlet for discharging mixed gas, the mixed gas outlet is connected with a mixed gas discharge valve, the upper side of the decomposition tower is provided with a product outlet for discharging purified carbon monoxide gas, the product outlet is connected with a product discharge valve, the first pipeline and the second pipeline are connected between the synthesis tower and the decomposition tower, the first pipeline is provided with a first control valve, the second pipeline is provided with a second control valve, the first pipeline is connected with the bottom of the synthesis tower and the middle-upper part of the decomposition tower, the second pipeline is connected with the bottom of the decomposition tower and the middle-upper part of the synthesis tower, and the second pipeline is provided with a circulating pump, the feeding direction of the circulating pump is from the decomposition tower to the synthesis tower.

[0024] The purification device further comprises a first heating device and a second heating device, the first heating device is connected with the synthesis tower, the first heating device can heat the synthesis tower, the second heating device is connected with the decomposition tower, and the second heating device can heat the decomposition tower.

[0025] The carbonyl nickel is decomposed into carbon monoxide and elemental nickel powder in the decomposition tower, high-purity carbon monoxide can be collected from the product outlet of the decomposition tower, the elemental nickel powder and the carbonyl nickel flow into the synthesis tower through the second pipeline and the circulating pump, the low-purity carbon monoxide raw material to be purified is added into the synthesis tower from the product outlet, the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, the impurities in the carbon monoxide raw material remain in the synthesis tower and are discharged from the mixed gas discharge valve, and the carbonyl nickel flows into the decomposition tower through the first pipeline to be decomposed into high-purity carbon monoxide, so that the low-purity carbon monoxide raw material is purified through the synthesis and decomposition reactions, high-purity carbon monoxide can be obtained, the use requirements of the integrated circuit and semiconductor industries can be met, the structure of the purification device is relatively simple, the carbonyl nickel can be recycled, and the purification cost is relatively low.

[0026] Preferably, the purification device further comprises a first cooling device, the first cooling device is connected with the mixed gas outlet, and the first cooling device can cool the mixed gas before being discharged from the mixed gas outlet.

[0027] The gaseous carbonyl nickel mixed in the mixed gas can be condensed and flowed back into the synthesis tower through the first cooling device before the mixed gas is discharged, so that the loss of carbonyl nickel in the purification process is reduced.

[0028] Preferably, the purification device further comprises a second cooling device, the second cooling device is connected with the product outlet, and the second cooling device can cool the carbon monoxide gas before being discharged from the product outlet.

[0029] The gaseous carbonyl nickel mixed in the carbon monoxide is condensed and flows back to the decomposition tower by cooling the carbon monoxide through the second cooling device before the carbon monoxide is discharged, so that the purity of the collected carbon monoxide is further improved, and the loss of the carbonyl nickel in the purification process is reduced.

[0030] Preferably, the third cooling device is arranged on the second pipeline, and the third cooling device is connected with the second pipeline, and the third cooling device is capable of cooling the fluid in the second pipeline.

[0031] Since the temperature in the decomposition tower is higher than that in the synthesis tower, the temperature of the nickel powder and the carbonyl nickel generated by the decomposition in the decomposition tower is high, so that the mixed solution of the carbonyl nickel and the nickel powder is cooled through the third cooling device when being extracted from the second pipeline to the synthesis tower by the circulating pump, so that the temperature of the mixed solution of the carbonyl nickel and the nickel powder is basically consistent with the temperature in the synthesis tower when entering the synthesis tower, and the influence of the temperature in the synthesis tower on the reaction process is reduced. BRIEF DESCRIPTION OF DRAWINGS

[0032] In order to more clearly illustrate the technical solutions in the embodiments of the present application or the prior art, the drawings needed to be used in the embodiments or the prior art description will be briefly introduced below. Obviously, the drawings in the following description are only some embodiments of the present application, and other drawings can also be obtained according to the structures shown in the drawings without creative labor for those skilled in the art.

[0033] Figure 1 It is a structural schematic diagram of the purification equipment of the present application.

[0034] In the drawings: 1-synthesis tower, 11-raw material gas inlet, 12-mixed gas discharge port, 13-mixed gas discharge valve, 14-first cooling device, 2-decomposition tower, 21-finished product discharge port, 22-finished product discharge valve, 23-second cooling device, 3-first pipeline, 31-first control valve, 32-first flow meter, 4-second pipeline, 41-second control valve, 42-circulating pump, 43-third cooling device, 44-second flow meter, 5-first heating device, 6-second heating device.

[0035] The implementation, functional features and advantages of the present application will be further described with reference to the embodiments and the drawings. DETAILED DESCRIPTION

[0036] The technical solutions in the embodiments of the present application will be clearly and completely described with reference to the drawings in the embodiments of the present application. Obviously, the described embodiments are only a part of the embodiments of the present application, rather than all the embodiments of the present application. Based on the embodiments in the present application, all other embodiments obtained by a person of ordinary skill in the art without creative effort belong to the scope of protection of the present application.

[0037] It should be noted that if the embodiments of the present application involve directional indications, such as up, down, left, right, front, back, etc., the directional indications are only used to explain the relative positional relationship, movement condition, etc. between components in a certain posture, and if the certain posture changes, the directional indications also change accordingly.

[0038] In addition, if the embodiments of the present application involve descriptions such as "first", "second", etc., the descriptions of "first", "second", etc. are only for description purposes, and cannot be understood as indicating or implying the relative importance of the indicated technical features or implicitly indicating the number of the indicated technical features. Therefore, the features limited by "first", "second" can explicitly or implicitly include at least one of the features. In addition, the technical solutions of each embodiment can be combined with each other, but it must be based on the realization of a person of ordinary skill in the art, and when the combination of technical solutions contradicts each other or cannot be realized, it should be considered that the combination of technical solutions does not exist and is not within the scope of protection required by the present application.

[0039] With reference to Figure 1 A carbon monoxide purification process, comprising the following steps:

[0040] S1: injecting carbonyl nickel into the synthesis tower 1 and the decomposition tower 2, wherein the synthesis tower 1 and the decomposition tower 2 are connected through a first pipeline 3 and a second pipeline 4, the first pipeline 3 is provided with a first control valve 31, the second pipeline 4 is provided with a second control valve 41, the first pipeline 3 connects the bottom of the synthesis tower 1 and the upper middle part of the decomposition tower 2, the second pipeline 4 connects the bottom of the decomposition tower 2 and the upper middle part of the synthesis tower 1, and the second pipeline 4 is provided with a circulating pump 42, and the feeding direction of the circulating pump 42 is from the decomposition tower 2 to the synthesis tower 1;

[0041] S2: introducing the carbon monoxide raw material to be purified into the synthesis tower 1, so that the pressure in the synthesis tower 1 is increased to a set first pressure value, and the pressure in the decomposition tower 2 is less than the first pressure value, then the first control valve 31, the second control valve 41 and the circulating pump 42 are opened, so that the carbonyl nickel in the synthesis tower 1 flows to the decomposition tower 2 through the first pipeline 3, and the carbonyl nickel in the decomposition tower 2 flows to the synthesis tower 1 through the second pipeline 4;

[0042] S3: continuously feeding the carbon monoxide raw material to be purified into the synthesis tower 1, maintaining the pressure in the synthesis tower 1 at the first pressure value, keeping the circulating pump 42 running, controlling the temperature in the synthesis tower 1 at the set synthesis temperature, the synthesis temperature being 50-90℃, heating and maintaining the decomposition tower 2 at the set decomposition temperature, the decomposition temperature being 150-250℃, decomposing the nickel carbonyl in the decomposition tower 2 to generate carbon monoxide and nickel powder, collecting the carbon monoxide generated by decomposition from the upper part of the decomposition tower 2, and at the same time, the nickel powder and the undecomposed nickel carbonyl generated by decomposition in the decomposition tower 2 are extracted into the synthesis tower 1 through the circulating pump 42 in the second pipeline 4, and the nickel powder reacts with the carbon monoxide raw material to be purified in the synthesis tower 1 to generate nickel carbonyl, so as to form a continuous reaction cycle, which is the synthesis of nickel carbonyl by the reaction of nickel powder with the carbon monoxide raw material to be purified in the synthesis tower 1, and the synthesis and decomposition reaction of the decomposition of nickel carbonyl in the decomposition tower 2 to generate carbon monoxide and nickel powder.

[0043] The carbon monoxide purification process utilizes the reaction of elemental nickel and carbon monoxide at low temperature to synthesize nickel carbonyl, and the decomposition of nickel carbonyl at high temperature into elemental nickel and carbon monoxide, and the specific synthesis and decomposition reaction formulae are as follows:

[0044]

[0045] By utilizing the above synthesis and decomposition reactions, the nickel carbonyl is decomposed into carbon monoxide and elemental nickel powder in the decomposition tower 2, and the carbon monoxide with higher purity can be collected from the decomposition tower 2, the elemental nickel powder flows into the synthesis tower 1, the carbon monoxide raw material with lower purity to be purified is added into the synthesis tower 1, the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize nickel carbonyl, while the impurities in the carbon monoxide raw material remain in the synthesis tower 1 and are discharged, and the nickel carbonyl flows into the decomposition tower 2 to decompose the carbon monoxide with higher purity, so that through the synthesis and decomposition reactions, the carbon monoxide raw material with lower purity is purified, the carbon monoxide with higher purity can be obtained, which is beneficial to the use in the integrated circuit and semiconductor industries, and the purification process is relatively simple, the nickel carbonyl can be recycled, and the purification cost is relatively low.

[0046] In some embodiments, in step S2, the first pressure value is 1-3 MPa, the pressure in the decomposition tower 2 is 1-3 MPa, and the first control valve 31 and the second control valve 41 are adjusted to control the flow of the material in the first pipeline 3 and the second pipeline 4, respectively, so as to form a material circulation balance between the synthesis tower 1 and the decomposition tower 2.

[0047] The pressure in the decomposition tower 2 is less than the pressure in the synthesis tower 1, so that the carbonyl nickel in the synthesis tower 1 can flow into the decomposition tower 2 through the first pipeline 3, and the appropriate pressure in the synthesis tower 1 and the decomposition tower 2 during the reaction process can increase the boiling point of the carbonyl nickel and reduce the gasification of the carbonyl nickel. After the flow of the materials in the first pipeline 3 and the second pipeline 4 is adjusted by the first control valve 31 and the second control valve 41, the material circulation balance is formed between the synthesis tower 1 and the decomposition tower 2, and the high-purity carbon monoxide can be stably generated.

[0048] Further, the liquid content of the synthesis tower 1 and the decomposition tower 2 is not less than 30% of the volume of the tower.

[0049] The liquid content of the synthesis tower 1 and the decomposition tower 2 is not less than 30% of the volume of the tower.

[0050] In some embodiments, in step S3, when the pressure in the synthesis tower 1 is greater than or equal to the first pressure value, the pressure in the synthesis tower 1 is reduced by discharging the mixed gas in the synthesis tower 1. In this way, while the pressure in the synthesis tower 1 is maintained, the amount of carbon monoxide raw material can be maintained, and the accumulated mixed gas can be discharged.

[0051] Further, before discharging the mixed gas in the synthesis tower 1, the step of cooling the mixed gas to condense the carbonyl nickel mixed in the mixed gas is further included.

[0052] Cooling the mixed gas before discharging the mixed gas can condense the gaseous carbonyl nickel mixed in the mixed gas and flow back into the synthesis tower 1, thereby reducing the loss of carbonyl nickel in the purification process.

[0053] In some embodiments, before collecting the carbon monoxide generated by decomposition in the decomposition tower 2 in step S3, the step of cooling the carbon monoxide generated by decomposition to condense the carbonyl nickel mixed in the carbon monoxide is further included.

[0054] Cooling the carbon monoxide before discharging the carbon monoxide can condense the gaseous carbonyl nickel mixed in the carbon monoxide and flow back into the decomposition tower 2, thereby further improving the purity of the collected carbon monoxide and reducing the loss of carbonyl nickel in the purification process.

[0055] In some embodiments, step S3 further includes the step of cooling the mixed liquid of the carbonyl nickel and the nickel powder in the second pipeline 4, so that the temperature of the mixed liquid flowing into the synthesis tower 1 is 50-90°C.

[0056] Since the temperature in the decomposition tower 2 is higher than that in the synthesis tower 1, the temperature of the nickel powder and the carbonyl nickel produced by the decomposition in the decomposition tower 2 is higher, and thus the temperature of the mixed solution of the nickel powder and the carbonyl nickel is reduced when it is extracted from the second pipeline 4 to the synthesis tower 1, so that the temperature of the mixed solution of the nickel powder and the carbonyl nickel is basically consistent with the temperature in the synthesis tower 1 when it enters the synthesis tower 1, thereby reducing the influence of the temperature in the synthesis tower 1 on the reaction process.

[0057] On the other hand, with reference to Figure 1 A purification device capable of realizing the above-mentioned purification process, comprising a synthesis tower 1 and a decomposition tower 2, the synthesis tower 1 is provided with a raw material gas inlet 11 for adding the carbon monoxide raw material to be purified, and the upper side of the synthesis tower 1 is further provided with a mixed gas discharge outlet 12 for discharging mixed gas, the mixed gas discharge outlet 12 is connected with a mixed gas discharge valve 13, the upper side of the decomposition tower 2 is provided with a product discharge outlet 21 for discharging the purified carbon monoxide gas, the product discharge outlet 21 is connected with a product discharge valve 22, the synthesis tower 1 and the decomposition tower 2 are connected with a first pipeline 3 and a second pipeline 4, the first pipeline 3 is provided with a first control valve 31, the second pipeline 4 is provided with a second control valve 41, the first pipeline 3 connects the bottom of the synthesis tower 1 and the middle and upper part of the decomposition tower 2, the second pipeline 4 connects the bottom of the decomposition tower 2 and the middle and upper part of the synthesis tower 1, the second pipeline 4 is provided with a circulating pump 42, and the feeding direction of the circulating pump 42 is from the decomposition tower 2 to the synthesis tower 1;

[0058] The purification device further comprises a first heating device 5 and a second heating device 6, the first heating device 5 is connected with the synthesis tower 1, the first heating device 5 can heat the synthesis tower 1, the second heating device 6 is connected with the decomposition tower 2, and the second heating device 6 can heat the decomposition tower 2.

[0059] The carbonyl nickel is decomposed into carbon monoxide and elemental nickel powder in the decomposition tower 2, the carbon monoxide with higher purity can be collected from the product discharge outlet 21 of the decomposition tower 2, and the elemental nickel powder and the carbonyl nickel flow into the synthesis tower 1 through the second pipeline 4 and the circulating pump 42; the carbon monoxide raw material with lower purity to be purified is added into the synthesis tower 1 from the product discharge outlet 21, the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, and the impurities in the carbon monoxide raw material remain in the synthesis tower 1 and are discharged from the mixed gas discharge valve 13, and the carbonyl nickel flows into the decomposition tower 2 through the first pipeline 3 to decompose the carbon monoxide with higher purity, so that the carbon monoxide raw material with lower purity is purified through the synthesis and decomposition reactions, the carbon monoxide with higher purity can be obtained, the use requirements of the integrated circuit and semiconductor industries can be met, the structure of the purification device is relatively simple, the carbonyl nickel can be recycled, and the purification cost is relatively low. The first heating device 5 heats the synthesis tower 1 to keep the temperature in the synthesis tower 1 at the synthesis temperature. The second heating device 6 heats the decomposition tower 2 to keep the temperature in the decomposition tower 2 at the decomposition temperature.

[0060] In some embodiments, the first pipeline 3 is further provided with a first flow meter 32, and the second pipeline 4 is further provided with a second flow meter 44. The first flow meter 32 can facilitate the observation of the flow of the material in the first pipeline 3, and the second flow meter 44 can facilitate the observation of the flow of the material in the second pipeline 4.

[0061] In some embodiments, the purification device further comprises a first cooling device 14, which is connected to the off-gas discharge port 12 and can cool the off-gas before it is discharged from the off-gas discharge port 12.

[0062] The cooling of the off-gas by the first cooling device 14 before it is discharged can cause the gaseous nickel carbonyl mixed in the off-gas to condense and flow back into the synthesis tower 1, thereby reducing the loss of nickel carbonyl during the purification process.

[0063] In some embodiments, the purification device further comprises a second cooling device 23, which is connected to the finished product discharge port 21 and can cool the carbon monoxide gas before it is discharged from the finished product discharge port 21.

[0064] The cooling of the carbon monoxide by the second cooling device 23 before it is discharged can cause the gaseous nickel carbonyl mixed in the carbon monoxide to condense and flow back into the decomposition tower 2, thereby further improving the purity of the collected carbon monoxide and reducing the loss of nickel carbonyl during the purification process.

[0065] In some embodiments, the second pipeline 4 is provided with a third cooling device 43, which is connected to the second pipeline 4 and can cool the fluid in the second pipeline 4.

[0066] Since the temperature in the decomposition tower 2 is higher than that in the synthesis tower 1, the temperature of the nickel powder and nickel carbonyl produced by decomposition in the decomposition tower 2 is also higher. Therefore, when the mixture of nickel powder and nickel carbonyl is extracted from the second pipeline 4 by the circulating pump 42 and enters the synthesis tower 1, the mixture is cooled by the third cooling device 43 to make the temperature of the mixture consistent with the temperature in the synthesis tower 1, thereby reducing the impact of the temperature of the mixture on the reaction process in the synthesis tower 1.

[0067] Further, the first cooling device 14, the second cooling device 23, and the third cooling device 43 can use existing cooling devices such as heat exchangers to cool the fluid using low-temperature refrigerants. The first heating device 5 and the second heating device 6 can use existing heating devices such as heat exchangers to heat the fluid using high-temperature heat media.

[0068] The purification process will be described in detail below in combination with the carbon monoxide purification process and the purification device.

[0069] Example One:

[0070] Carbonyl nickel is injected into the synthesis column 1 and the decomposition column 2, the impurity gas exhaust valve 13 and the product exhaust valve 22 are controlled to be closed, the first control valve 31 and the second control valve 41 are closed, then the carbon monoxide raw gas with a purity of 99.5% is introduced into the synthesis column 1, the pressure in the synthesis column 1 is 1.2 MPa, and the pressure in the decomposition column 2 is 1.0 MPa;

[0071] The first control valve 31 and the second control valve 41 are opened, and the circulating pump 42 on the second pipeline 4 is started, under the action of the pressure difference, the carbonyl nickel in the synthesis column 1 enters the decomposition column 2 through the first pipeline 3, and the carbonyl nickel in the decomposition column 2 is transported back to the synthesis column 1 through the second pipeline 4, the flow rate is adjusted to 2 m 3 / h in the first pipeline 3 and 2 m 3 / h in the second pipeline 4, and after the material circulation balance is formed, the content of carbonyl nickel in the synthesis column 1 is 30% of the volume of the column, and the content of carbonyl nickel in the decomposition column 2 is 30% of the volume of the column.

[0072] The first heating device 5 and the first cooling device 14 are started, the temperature of the column bottom of the synthesis column 1 is controlled to be 60°C, the temperature of the column top of the synthesis column 1 is controlled to be 10°C, the second heating device 6 and the second cooling device 23 are started, the temperature of the column bottom of the decomposition column 2 is controlled to be 170°C, and the temperature of the column top of the decomposition column 2 is controlled to be 35°C.

[0073] The solution in the synthesis column 1 enters the first heating device 5 from the bottom of the column after being heated, and returns to the column from the middle and lower part of the synthesis column 1, and the solution in the decomposition column 2 enters the second heating device 6 after being heated, and returns to the column from the middle and lower part of the decomposition column 2, and the circulation provides temperature for the reaction.

[0074] The carbonyl nickel is decomposed into nickel powder and carbon monoxide in the decomposition column 2, the nickel powder and the remaining carbonyl nickel enter the second pipeline 4, the third cooling device 43 is started, the mixture of carbonyl nickel and nickel powder in the second pipeline 4 is cooled to 60°C after passing through the third cooling device 43, and is pumped into the synthesis column 1 under the action of the circulating pump 42, the carbon monoxide raw gas to be purified is continuously introduced into the synthesis column 1 to react with the nickel powder in the synthesis column 1 to generate carbonyl nickel, the carbonyl nickel enters the decomposition column 2 through the first pipeline 3 under the action of the pressure difference, and the material circulation balance is maintained.

[0075] When the pressure in the synthesis column 1 exceeds 1.2 MPa, the impurity gas exhaust valve 13 is opened to exhaust the impurity gas, and the impurity gas is cooled and cooled by the first cooling device 14 to remove the carbonyl nickel in the impurity gas.

[0076] When the pressure in the decomposition column 2 exceeds 1.0 MPa, the product exhaust valve is opened to exhaust the carbon monoxide, and the carbon monoxide is cooled and cooled by the second cooling device 23 to remove the carbonyl nickel in the carbon monoxide, and high-purity carbon monoxide is obtained.

[0077] The purity of the carbon monoxide product gas collected from the decomposition tower 2 was analyzed, and the results are shown in Table 1 below:

[0078]

[0079] Table 1

[0080] Example Two:

[0081] Carbonyl nickel was injected into the synthesis tower 1 and the decomposition tower 2, the impurity discharge valve 13 and the product discharge valve 22 were controlled to be closed, the first control valve 31 and the second control valve 41 were closed, then carbon monoxide raw gas with a purity of 99.8% was introduced into the synthesis tower 1, the pressure in the synthesis tower 1 reached 2 MPa, and the pressure in the decomposition tower 2 reached 1.5 MPa;

[0082] The first control valve 31 and the second control valve 41 were opened, and the circulating pump 42 on the second pipeline 4 was started, under the action of the pressure difference, the carbonyl nickel in the synthesis tower 1 entered the decomposition tower 2 through the first pipeline 3, and the carbonyl nickel in the decomposition tower 2 was transported back to the synthesis tower 1 through the second pipeline 4, the flow rate was adjusted so that the flow rate in the first pipeline 3 was 3 m 3 / h, and the flow rate in the second pipeline 4 was 3 m 3 / h, after the material circulation balance was formed, the content of carbonyl nickel in the synthesis tower 1 was 50% of the tower volume, and the content of carbonyl nickel in the decomposition tower 2 was 50% of the tower volume.

[0083] The first heating device 5 and the first cooling device 14 were started, the temperature of the synthesis tower 1 was controlled to be 85°C, the temperature of the top of the synthesis tower 1 was controlled to be 20°C, the second heating device 6 and the second cooling device 23 were started, the temperature of the decomposition tower 2 was controlled to be 230°C, and the temperature of the top of the decomposition tower 2 was controlled to be 30°C.

[0084] The solution in the synthesis tower 1 entered the first heating device 5 after being heated, and returned to the tower from the middle and lower part of the synthesis tower 1, and the solution in the decomposition tower 2 entered the second heating device 6 after being heated, and returned to the tower from the middle and lower part of the decomposition tower 2, which provided temperature for the reaction.

[0085] The carbonyl nickel was decomposed in the decomposition tower 2 to generate nickel powder and carbon monoxide, the nickel powder and the remaining carbonyl nickel entered the second pipeline 4, the third cooling device 43 was started, the carbonyl nickel and the nickel powder mixture in the second pipeline 4 were cooled to 85°C after passing through the third cooling device 43, and were sucked into the synthesis tower 1 under the action of the circulating pump 42, the carbon monoxide raw gas to be purified was continuously introduced into the synthesis tower 1 to react with the nickel powder in the synthesis tower 1 to generate carbonyl nickel, the carbonyl nickel entered the decomposition tower 2 through the first pipeline 3 under the action of the pressure difference, and the material circulation balance was maintained.

[0086] When the pressure in the synthesis tower 1 exceeds 2 MPa, the waste gas discharge valve 13 is opened to discharge the waste gas, which is cooled by the first cooling device 14 to remove the carbonyl nickel in the waste gas, and then discharged.

[0087] When the pressure in the decomposition tower 2 exceeds 1.5 MPa, the product discharge valve is opened to discharge the carbon monoxide, which is cooled by the second cooling device 23 to remove the carbonyl nickel in the carbon monoxide, and then collected to obtain high-purity carbon monoxide.

[0088] The purity of the carbon monoxide product gas discharged from the decomposition tower 2 is analyzed, and the results are shown in Table 2 below:

[0089]

[0090] Table 2

[0091] From the analysis results in Tables 1 and 2 above, it can be seen that the purity of the low-purity carbon monoxide can be effectively improved after being purified by the purification process and the purification equipment, and the purity of the carbon monoxide can reach 5N or above.

[0092] The above description is only the preferred embodiments of the present application, and does not limit the patent scope of the present application. Any equivalent structural transformation, direct / indirect application in other related technical fields, or direct / indirect application in other related technical fields under the inventive concept of the present application, as described in the specification and drawings, are included in the patent protection scope of the present application.

Claims

1. A carbon monoxide purification process, characterized by, The method comprises the following steps: S1: injecting carbonyl nickel into a synthesis tower (1) and a decomposition tower (2), wherein the synthesis tower (1) and the decomposition tower (2) are connected through a first pipeline (3) and a second pipeline (4), the first pipeline (3) is provided with a first control valve (31), the second pipeline (4) is provided with a second control valve (41), the first pipeline (3) is connected to the bottom of the synthesis tower (1) and the upper middle part of the decomposition tower (2), the second pipeline (4) is connected to the bottom of the decomposition tower (2) and the upper middle part of the synthesis tower (1), the second pipeline (4) is provided with a circulating pump (42), and the feeding direction of the circulating pump (42) is from the decomposition tower (2) to the synthesis tower (1); S2: introducing a carbon monoxide raw material to be purified into the synthesis tower (1), increasing the pressure in the synthesis tower (1) to a set first pressure value, and ensuring that the pressure in the decomposition tower (2) is less than or equal to the first pressure value, then opening the first control valve (31), the second control valve (41) and the circulating pump (42), so that the carbonyl nickel in the synthesis tower (1) flows to the decomposition tower (2) through the first pipeline (3), and the carbonyl nickel in the decomposition tower (2) flows to the synthesis tower (1) through the second pipeline (4); S3: continuously introducing the carbon monoxide raw material to be purified into the synthesis tower (1), maintaining the pressure in the synthesis tower (1) at the first pressure value, keeping the circulating pump (42) running, controlling the temperature in the synthesis tower (1) at a set synthesis temperature, heating the decomposition tower (2) and maintaining it at a set decomposition temperature, so that the carbonyl nickel in the decomposition tower (2) decomposes to generate carbon monoxide and nickel powder, collecting the generated carbon monoxide from the upper part of the decomposition tower (2), and at the same time, the generated nickel powder and the undecomposed carbonyl nickel in the decomposition tower (2) are extracted into the synthesis tower (1) through the circulating pump (42) on the second pipeline (4), and the nickel powder reacts with the carbon monoxide to be purified in the synthesis tower (1) to generate carbonyl nickel, so as to form a continuous reaction cycle.

2. The carbon monoxide purification process of claim 1, wherein, In step S2, the first pressure value is 1-3 MPa, the pressure in the decomposition tower (2) is 1-3 MPa, and the first control valve (31) and the second control valve (41) are adjusted to control the flow of materials in the first pipeline (3) and the second pipeline (4) respectively, so as to form a material circulation balance between the synthesis tower (1) and the decomposition tower (2).

3. The carbon monoxide purification process of claim 1, wherein, In step S3, when the pressure in the synthesis tower (1) is greater than or equal to the first pressure value, the pressure in the synthesis tower (1) is reduced by discharging the mixed gas in the synthesis tower (1).

4. The carbon monoxide purification process of claim 3, wherein, Before discharging the mixed gas in the synthesis tower (1), the step of cooling the mixed gas and condensing the carbonyl nickel mixed in the mixed gas is further included.

5. The carbon monoxide purification process of claim 1 wherein, Before collecting the generated carbon monoxide in the decomposition tower (2) in step S3, the step of cooling the generated carbon monoxide and condensing the carbonyl nickel mixed in the carbon monoxide is further included.

6. The carbon monoxide purification process of claim 1 wherein, The step S3 further comprises a step of cooling the mixed solution of the carbonyl nickel and the nickel powder in the second pipe (4) to a temperature of 50-90 ℃ when the mixed solution flows into the synthesis tower (1).

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