Carbon monoxide purification process and purification equipment

Abstract

The invention discloses a carbon monoxide purification process and purification equipment, and the carbon monoxide purification process comprises the following steps: nickel carbonyl is decomposed into carbon monoxide and elemental nickel powder in a decomposition tower, the carbon monoxide with higher purity can be collected from the decomposition tower, and the elemental nickel powder and the nickel carbonyl flow into a synthesis tower; a low-purity carbon monoxide raw material to be purified is added into a synthesis tower, nickel powder reacts with carbon monoxide in the carbon monoxide raw material to synthesize nickel carbonyl, impurities in the carbon monoxide raw material remain in the synthesis tower to be discharged, nickel carbonyl flows into a decomposition tower to be decomposed into high-purity carbon monoxide, and through the synthesis and decomposition reaction, the high-purity carbon monoxide is obtained. According to the method, the carbon monoxide raw material with low purity is purified, carbon monoxide with higher purity can be obtained, use in integrated circuit and semiconductor industries is facilitated, the purification process is simple, nickel carbonyl can be recycled, and the purification cost is low.

Description

Technical Field

[0001] The invention relates to the technical field of carbon monoxide production, and in particular to a carbon monoxide purification process and purification equipment. Background Art

[0002] With the rapid development of industry and semiconductor industry, the amount of high-purity carbon monoxide used as etching gas for chips in the semiconductor field is increasing. In the integrated circuit and semiconductor industries, high-purity carbon monoxide with a purity of 5N (99.999%) or above is often required, so the production of high-purity carbon monoxide is of great significance. At present, there are three main methods for producing carbon monoxide: one is to use coking coal, oxygen, and carbon dioxide as raw materials to prepare carbon monoxide under high-temperature catalyst conditions, and after purification, carbon monoxide with a purity of about 98% can be obtained. The carbon monoxide produced by this method has low purity and complex impurities; the second is to use methanol high-temperature cracking and then pressure swing adsorption to purify carbon monoxide to obtain carbon monoxide with a purity of 99%. The disadvantage is that the methanol cracking catalyst is expensive, and the purity is unstable and the utilization rate is not high in production; the third is to use formic acid under the catalytic action of concentrated sulfuric acid to dehydrate to obtain carbon monoxide gas, and then obtain a carbon monoxide product with a purity of 99.9% through purification processes such as condensation, water washing, alkali washing, acid washing and adsorption.

[0003] Although the above-mentioned processes for producing carbon monoxide can only achieve 4N purity (99.99%), it is quite difficult to further increase the purity to 5N or above. The application of carbon monoxide in the integrated circuit and semiconductor industries is still limited. The purity of carbon monoxide needs to be further improved. Therefore, it is necessary to study a new purification process and equipment to obtain higher purity carbon monoxide. Summary of the invention

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

[0005] To achieve the above object, the present invention provides a carbon monoxide purification process, comprising the following steps:

[0006] S1: injecting carbonyl nickel into both a synthesis tower and a 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 middle and upper part of the decomposition tower, the second pipeline connects the bottom of the decomposition tower and the middle and upper part of the synthesis tower, the second pipeline is provided with a circulation pump, and the feeding direction of the circulation 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, so that the pressure in the synthesis tower is increased to a set first pressure value, and the pressure in the decomposition tower is less than or equal to the first pressure value, and then opening the first control valve, the second control valve and the circulation pump, so that the carbonyl nickel in the synthesis tower flows into the decomposition tower through the first pipeline, and the carbonyl nickel in the decomposition tower flows into the synthesis tower through the second pipeline;

[0008] S3: continuously introducing the carbon monoxide raw material to be purified into the synthesis tower, and maintaining the pressure in the synthesis tower at the first pressure value and the circulation pump running, controlling the temperature in the synthesis tower at the set synthesis temperature, heating the decomposition tower and maintaining it at the set decomposition temperature, so that the carbonyl nickel in the decomposition tower is decomposed to generate carbon monoxide and nickel powder, collecting the decomposed carbon monoxide from the upper part of the decomposition tower, and at the same time, the nickel powder decomposed in the decomposition tower and the undecomposed carbonyl nickel are pumped into the synthesis tower through the circulation pump on the second pipeline, and the nickel powder reacts with the carbon monoxide to be purified in the synthesis tower to generate carbonyl nickel, so as to form a continuous reaction cycle.

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

[0010]

[0011] By utilizing the above-mentioned synthesis and decomposition reactions, carbonyl nickel is decomposed into carbon monoxide and elemental nickel powder in a decomposition tower. Carbon monoxide with higher purity can be collected from the decomposition tower, and the elemental nickel powder flows into the synthesis tower. A carbon monoxide raw material with lower purity to be purified is added into the synthesis tower, and the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, while impurities in the carbon monoxide raw material are retained in the synthesis tower and discharged. The carbonyl nickel then flows into the decomposition tower to decompose carbon monoxide with higher purity. In this way, the carbon monoxide raw material with lower purity can be purified through the synthesis and decomposition reactions, and carbon monoxide with higher purity can be obtained, which is beneficial for use in the integrated circuit and semiconductor industries, and the purification process is relatively simple, the carbonyl nickel can be recycled, and the purification cost is relatively 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 rate 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 nickel carbonyl in the synthesis tower can flow into the decomposition tower through the first pipeline. During the reaction process of the synthesis tower and the decomposition tower, maintaining a suitable pressure in the tower can increase the boiling point of the nickel carbonyl and reduce the gasification of the nickel carbonyl.

[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 reaches more than 30%, which can enable the two towers to form a material circulation balance.

[0016] Preferably, in step S3, when the pressure in the synthesis tower is ≥ the first pressure value, the pressure in the synthesis tower is reduced by discharging the impurities in the synthesis tower. In this way, the amount of carbon monoxide raw material introduced can be maintained while the accumulated impurities can be discharged while maintaining the pressure in the synthesis tower.

[0017] Preferably, before the impurity gas in the synthesis tower is discharged, the method further comprises the step of cooling the impurity gas to condense the carbonyl nickel contained in the impurity gas.

[0018] By cooling the impurity gas before it is discharged, the gaseous carbonyl nickel contained in the impurity gas can be condensed and refluxed into the synthesis tower, thereby reducing the loss of carbonyl nickel during the purification process.

[0019] Preferably, before collecting the carbon monoxide generated by decomposition in the decomposition tower in step S3, the process further comprises cooling the carbon monoxide generated by decomposition to condense the carbonyl nickel contained in the carbon monoxide.

[0020] By cooling the carbon monoxide before it is discharged, the gaseous carbonyl nickel contained in the carbon monoxide can be condensed and refluxed into the decomposition tower, thereby further improving the purity of the collected carbon monoxide and reducing the loss of carbonyl nickel during the purification process.

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

[0022] Since the temperature in the decomposition tower is higher than that in the synthesis tower, the temperature of the nickel powder and carbonyl nickel produced by decomposition in the decomposition tower is relatively high. Therefore, the circulating pump cools the mixture when it is drawn from the second pipeline into the synthesis tower, so that the temperature of the carbonyl nickel and nickel powder mixture is basically consistent with the temperature in the synthesis tower when entering the synthesis tower, thereby reducing the impact on the temperature in the synthesis tower and affecting the reaction process.

[0023] On the other hand, the present invention also proposes a purification device, including a synthesis tower and a decomposition tower, wherein the synthesis tower is provided with a raw material air inlet for adding a carbon monoxide raw material to be purified, and the upper side of the synthesis tower is also provided with a miscellaneous gas outlet for discharging impurities, and the impurity gas outlet is connected to a miscellaneous gas outlet valve, and the upper side of the decomposition tower is provided with a finished product outlet for discharging purified carbon monoxide gas, and the finished product outlet is connected to a finished product outlet valve, and a first pipeline and a second pipeline are connected between the synthesis tower and the decomposition tower, and a first control valve is provided on the first pipeline, and a second control valve is provided on the second pipeline, and the first pipeline connects the bottom of the synthesis tower and the middle and upper part of the decomposition tower, and the second pipeline connects the bottom of the decomposition tower and the middle and upper part of the synthesis tower, and a circulation pump is provided on the second pipeline, and the feeding direction of the circulation pump is from the decomposition tower to the synthesis tower;

[0024] The purification equipment also includes a first heating device and a second heating device, wherein the first heating device is connected to the synthesis tower and can heat the synthesis tower, and the second heating device is connected to the decomposition tower and can heat the decomposition tower.

[0025] Carbonyl nickel is decomposed into carbon monoxide and elemental nickel powder in a decomposition tower, and carbon monoxide with higher purity can be collected from the finished product discharge port of the decomposition tower, and elemental nickel powder and carbonyl nickel flow into a synthesis tower through a second pipeline and a circulation pump; a carbon monoxide raw material with lower purity to be purified is added into the synthesis tower from the finished product discharge port, and nickel powder reacts with carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, while impurities in the carbon monoxide raw material remain in the synthesis tower and are discharged from a miscellaneous gas discharge valve, and the carbonyl nickel flows into the decomposition tower through the first pipeline to decompose carbon monoxide with higher purity, thus achieving purification of the carbon monoxide raw material with lower purity through synthesis and decomposition reactions, and obtaining carbon monoxide with higher purity, which meets the use requirements of the integrated circuit and semiconductor industries, and the structure of the purification equipment is relatively simple, the carbonyl nickel can be recycled, and the purification cost is relatively low.

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

[0027] Before the impurity gas is discharged, the impurity gas is cooled by the first cooling device, so that the gaseous carbonyl nickel mixed in the impurity gas can be condensed and refluxed into the synthesis tower, thereby reducing the loss of carbonyl nickel in the purification process.

[0028] Preferably, the purification equipment further comprises a second cooling device, the second cooling device is connected to the finished product discharge port, and the second cooling device can cool the carbon monoxide gas before being discharged from the finished product discharge port.

[0029] Before the carbon monoxide is discharged, the carbon monoxide is cooled by the second cooling device, so that the gaseous carbonyl nickel mixed in the carbon monoxide can be condensed and refluxed into the decomposition tower, further improving the purity of the collected carbon monoxide and reducing the loss of carbonyl nickel in the purification process.

[0030] Preferably, a third cooling device is provided on the second pipeline, and the third cooling device is connected to the second pipeline, and the third cooling device can cool 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 carbonyl nickel produced by decomposition in the decomposition tower is relatively high. Therefore, when the nickel powder and carbonyl nickel mixture are extracted from the second pipeline into the synthesis tower by the circulation pump, the third cooling device is used to cool the mixture, so that the temperature of the carbonyl nickel and nickel powder mixture is basically consistent with the temperature in the synthesis tower when entering the synthesis tower, thereby reducing the impact on the temperature in the synthesis tower and affecting the reaction process. BRIEF DESCRIPTION OF THE DRAWINGS

[0032] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings required for use in the embodiments or the description of the prior art will be briefly introduced below. Obviously, the drawings in the following description 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 paying any creative work.

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

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

[0035] The realization of the purpose, functional features and advantages of the present invention will be further explained in conjunction with embodiments and with reference to the accompanying drawings. DETAILED DESCRIPTION

[0036] The following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative work are within the scope of protection of the present invention.

[0037] It should be noted that if the embodiments of the present invention involve directional indications, such as up, down, left, right, front, back, etc., then the directional indications are only used to explain the relative position relationship, movement status, etc. between the components in a certain specific posture. If the specific posture changes, the directional indication will also change accordingly.

[0038] In addition, if there are descriptions involving "first", "second", etc. in the embodiments of the present invention, the descriptions of "first", "second", etc. are only used for descriptive purposes and cannot be understood as indicating or suggesting their relative importance or implicitly indicating the number of the indicated technical features. Therefore, the features defined as "first" and "second" may explicitly or implicitly include at least one of the features. In addition, the technical solutions between the various embodiments can be combined with each other, but they must be based on the ability of technical personnel in this field to implement them. When the combination of technical solutions is contradictory or cannot be implemented, it should be deemed that such a combination of technical solutions does not exist and is not within the scope of protection required by the present invention.

[0039] Reference Figure 1 , a carbon monoxide purification process, comprising the following steps:

[0040] S1: injecting carbonyl nickel into both 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, a first control valve 31 is provided on the first pipeline 3, a second control valve 41 is provided on the second pipeline 4, 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, and a circulation pump 42 is provided on the second pipeline 4, and the feeding direction of the circulation 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, and then opening the first control valve 31, the second control valve 41 and the circulation pump 42, so that the carbonyl nickel in the synthesis tower 1 flows into the decomposition tower 2 through the first pipeline 3, and the carbonyl nickel in the decomposition tower 2 flows into the synthesis tower 1 through the second pipeline 4;

[0042] S3: continuously introduce the carbon monoxide raw material to be purified into the synthesis tower 1, and maintain the pressure in the synthesis tower 1 at the first pressure value and keep the circulation pump 42 running, control the temperature in the synthesis tower 1 to be at the set synthesis temperature, the synthesis temperature is 50-90°C, heat the decomposition tower 2 and maintain it at the set decomposition temperature, the decomposition temperature is 150-250°C, decompose the carbonyl nickel in the decomposition tower 2 to generate carbon monoxide and nickel powder, collect the decomposed carbon monoxide from the upper part of the decomposition tower 2, and at the same time, the nickel powder decomposed in the decomposition tower 2 and the undecomposed carbonyl nickel are extracted into the synthesis tower 1 through the circulation 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, which is a synthesis and decomposition reaction of the nickel powder and the carbon monoxide to be purified in the synthesis tower 1 to synthesize carbonyl nickel, and the carbonyl nickel is decomposed in the decomposition tower 2 to generate carbon monoxide and nickel powder.

[0043] The carbon monoxide purification process uses the reaction of elemental nickel and carbon monoxide at low temperature to synthesize carbonyl nickel, where the carbonyl nickel is in liquid state, and the reaction of carbonyl nickel decomposing into elemental nickel and carbon monoxide at high temperature. The specific synthesis and decomposition reaction formulas are as follows:

[0044]

[0045] By utilizing the above-mentioned synthesis and decomposition reactions, the carbonyl nickel is decomposed into carbon monoxide and elemental nickel powder in the decomposition tower 2. Carbon monoxide with higher purity can be collected from the decomposition tower 2, and the elemental nickel powder flows into the synthesis tower 1. A carbon monoxide raw material with lower purity to be purified is added to the synthesis tower 1, and the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, while the impurities in the carbon monoxide raw material remain in the synthesis tower 1 and are discharged. The carbonyl nickel then flows into the decomposition tower 2 to decompose carbon monoxide with higher purity. In this way, the carbon monoxide raw material with lower purity can be purified through the synthesis and decomposition reactions, and 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 carbonyl nickel can be recycled, and the purification cost is relatively low.

[0046] In some specific 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 rate of materials in the first pipeline 3 and the second pipeline 4 respectively, so that a material circulation balance is formed between the synthesis tower 1 and the decomposition tower 2.

[0047] The pressure in the decomposition tower 2 is lower 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 during the reaction process of the synthesis tower 1 and the decomposition tower 2, maintaining a suitable pressure in the tower can increase the boiling point of the carbonyl nickel and reduce the gasification of the carbonyl nickel. After the flow rate of the material in the first pipeline 3 and the second pipeline 4 is adjusted in coordination with the first control valve 31 and the second control valve 41, a material circulation balance is formed between the synthesis tower 1 and the decomposition tower 2, and high-purity carbon monoxide can be stably generated.

[0048] Furthermore, the liquid content of the synthesis tower 1 and the decomposition tower 2 is controlled to be no less than 30% of the tower volume.

[0049] The liquid content of the synthesis tower 1 and the decomposition tower 2 reaches more than 30%, which can enable the two towers to form a material circulation balance.

[0050] In some specific embodiments, in step S3, when the pressure in the synthesis tower 1 is ≥ the first pressure value, the pressure in the synthesis tower 1 is reduced by discharging the impurities in the synthesis tower 1. In this way, while maintaining the pressure in the synthesis tower 1, the amount of carbon monoxide raw material introduced can be maintained and the accumulated impurities can be discharged.

[0051] Furthermore, before the impurity gas in the synthesis tower 1 is discharged, the method further includes a step of cooling the impurity gas to condense the carbonyl nickel contained in the impurity gas.

[0052] By cooling the impurity gas before it is discharged, the gaseous carbonyl nickel contained in the impurity gas can be condensed and refluxed into the synthesis tower 1, thereby reducing the loss of carbonyl nickel during the purification process.

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

[0054] By cooling the carbon monoxide before it is discharged, the gaseous nickel carbonyl contained in the carbon monoxide can be condensed and refluxed 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.

[0055] In some specific embodiments, step S3 also includes a step of cooling the mixed solution of carbonyl nickel and nickel powder in the second pipe 4 so that the temperature of the mixed solution when 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 carbonyl nickel produced by decomposition in the decomposition tower 2 is relatively high. Therefore, the circulating pump 42 cools the mixture when it is drawn from the second pipeline 4 to the synthesis tower 1, so that the temperature of the carbonyl nickel and nickel powder mixture is basically the same as the temperature in the synthesis tower 1 when it enters the synthesis tower 1, thereby reducing the impact on the temperature in the synthesis tower 1 and affecting the reaction process.

[0057] On the other hand, refer 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 being provided with a raw material inlet 11 for adding a carbon monoxide raw material to be purified, the upper side of the synthesis tower 1 being further provided with a miscellaneous gas outlet 12 for discharging miscellaneous gas, the miscellaneous gas outlet 12 being connected to a miscellaneous gas outlet valve 13, the upper side of the decomposition tower 2 being provided with a finished product outlet 21 for discharging purified carbon monoxide gas, the finished product outlet 21 being connected to a finished product outlet valve 22, a first pipeline 3 and a second pipeline 4 being connected between the synthesis tower 1 and the decomposition tower 2, a first control valve 31 being provided on the first pipeline 3, a second control valve 41 being provided on the second pipeline 4, the first pipeline 3 connecting the bottom of the synthesis tower 1 and the middle and upper part of the decomposition tower 2, the second pipeline 4 connecting the bottom of the decomposition tower 2 and the middle and upper part of the synthesis tower 1, a circulating pump 42 being provided on the second pipeline 4, the feeding direction of the circulating pump 42 being the direction from the decomposition tower 2 to the synthesis tower 1;

[0058] The purification equipment also includes a first heating device 5 and a second heating device 6. The first heating device 5 is connected to the synthesis tower 1 and can heat the synthesis tower 1. The second heating device 6 is connected to the decomposition tower 2 and can heat the decomposition tower 2.

[0059] The carbonyl nickel is decomposed into carbon monoxide and elemental nickel powder in the decomposition tower 2, and carbon monoxide with higher purity can be collected from the finished product discharge port 21 of the decomposition tower 2, and the elemental nickel powder and carbonyl nickel flow into the synthesis tower 1 through the second pipeline 4 and the circulation pump 42; the carbon monoxide raw material with lower purity to be purified is added into the synthesis tower 1 from the finished product discharge port 21, and the nickel powder reacts with the carbon monoxide in the carbon monoxide raw material to synthesize carbonyl nickel, while the impurities in the carbon monoxide raw material remain in the synthesis tower 1 and are discharged from the impurity 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 can be purified through the synthesis and decomposition reaction, and carbon monoxide with higher purity can be obtained, which meets the use requirements of the integrated circuit and semiconductor industries, and the structure of the purification equipment is simple, the carbonyl nickel can be recycled, and the purification cost is 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 specific embodiments, a first flow meter 32 is further provided on the first pipeline 3, and a second flow meter 44 is further provided on the second pipeline 4. The first flow meter 32 can conveniently check the flow of the material in the first pipeline 3, and the second flow meter 44 can conveniently check the flow of the material in the second pipeline 4.

[0061] In some specific embodiments, the purification device further includes a first cooling device 14 , which is connected to the impurity gas outlet 12 , and the first cooling device 14 can cool the impurity gas before being discharged from the impurity gas outlet 12 .

[0062] Before the impurity gas is discharged, the impurity gas is cooled by the first cooling device 14, so that the gaseous carbonyl nickel mixed in the impurity gas can be condensed and refluxed into the synthesis tower 1, thereby reducing the loss of carbonyl nickel in the purification process.

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

[0064] Before the carbon monoxide is discharged, the second cooling device 23 cools the carbon monoxide, so that the gaseous carbonyl nickel mixed in the carbon monoxide can be condensed and refluxed into the decomposition tower 2, further improving the purity of the collected carbon monoxide and reducing the loss of carbonyl nickel in the purification process.

[0065] In some specific embodiments, a third cooling device 43 is provided on the second pipeline 4 . The third cooling device 43 is connected to the second pipeline 4 . The third cooling device 43 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 carbonyl nickel produced by decomposition in the decomposition tower 2 is higher. Therefore, when the nickel powder and carbonyl nickel mixture are extracted from the second pipeline 4 to the synthesis tower 1 by the circulation pump 42, the third cooling device 43 is used to cool the nickel powder and carbonyl nickel mixture, so that the temperature of the carbonyl nickel and nickel powder mixture is basically the same as the temperature in the synthesis tower 1 when entering the synthesis tower 1, thereby reducing the impact on the temperature in the synthesis tower 1 and affecting the reaction process.

[0067] Furthermore, 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 refrigerant. 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 medium.

[0068] The purification process is described in detail below in conjunction with the carbon monoxide purification process and purification equipment.

[0069] Embodiment 1:

[0070] Injecting nickel carbonyl into the synthesis tower 1 and the decomposition tower 2, controlling the impurity gas discharge valve 13 and the finished product discharge valve 22 to be in a closed state, the first control valve 31 and the second control valve 41 to be in a closed state, and then introducing carbon monoxide raw material gas with a purity of 99.5% into the synthesis tower 1, so that the pressure in the synthesis tower 1 reaches 1.2 MPa, and the pressure in the decomposition tower 2 reaches 1.0 MPa;

[0071] Open the first control valve 31 and the second control valve 41, and start the circulation pump 42 on the second pipeline 4. Under the action of the pressure difference, the carbonyl nickel in the synthesis tower 1 will enter the decomposition tower 2 through the first pipeline 3, and the carbonyl nickel in the decomposition tower 2 will be transported back to the synthesis tower 1 through the second pipeline 4. Adjust the flow rate so that the flow rate in the first pipeline 3 is 2m 3 / h, the flow rate in the second pipe 4 is 2m 3 / h, after forming material circulation balance, the carbonyl nickel content in the synthesis tower 1 is 30% of the tower inner volume, and the carbonyl nickel content in the decomposition tower 2 is 30% of the tower inner volume.

[0072] The first heating device 5 and the first cooling device 14 are turned on to control the bottom temperature of the synthesis tower 1 to 60°C and the top temperature of the synthesis tower 1 to 10°C. The second heating device 6 and the second cooling device 23 are turned on to control the bottom temperature of the decomposition tower 2 to 170°C and the top temperature of the decomposition tower 2 to 35°C.

[0073] After the solution in the synthesis tower 1 enters the first heating device 5 from the bottom of the tower for heating, it returns to the tower from the middle and lower part of the synthesis tower 1. At the same time, after the solution in the decomposition tower 2 enters the second heating device 6 for heating, it returns to the tower from the middle and lower part of the decomposition tower 2. The cycle is repeated to provide temperature for the reaction.

[0074] The carbonyl nickel is decomposed in the decomposition tower 2 to generate nickel powder and carbon monoxide. The nickel powder and the remaining carbonyl nickel enter the second pipeline 4. The third cooling device 43 is turned on. 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. The mixture is pumped into the synthesis tower 1 under the action of the circulation pump 42. The carbon monoxide raw material to be purified is 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 enters the decomposition tower 2 through the first pipeline 3 under the action of the pressure difference to maintain the material circulation balance.

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

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

[0077] The carbon monoxide finished gas collected from the decomposition tower 2 is discharged and subjected to purity analysis. The result is shown in Table 1 below:

[0078]

[0079] Table 1

[0080] Embodiment 2:

[0081] Injecting nickel carbonyl into the synthesis tower 1 and the decomposition tower 2, controlling the impurity gas discharge valve 13 and the finished product discharge valve 22 to be in a closed state, the first control valve 31 and the second control valve 41 to be in a closed state, and then introducing carbon monoxide raw material gas with a purity of 99.8% into the synthesis tower 1, so that the pressure in the synthesis tower 1 reaches 2MPa, and the pressure in the decomposition tower 2 reaches 1.5MPa;

[0082] Open the first control valve 31 and the second control valve 41, and start the circulation pump 42 on the second pipeline 4. Under the action of the pressure difference, the carbonyl nickel in the synthesis tower 1 will enter the decomposition tower 2 through the first pipeline 3, and the carbonyl nickel in the decomposition tower 2 will be transported back to the synthesis tower 1 through the second pipeline 4. The flow rate is adjusted so that the flow rate in the first pipeline 3 is 3m 3 / h, the flow rate in the second pipeline 4 is 3m 3 / h, after forming material circulation balance, the carbonyl nickel content in the synthesis tower 1 is 50% of the tower inner volume, and the carbonyl nickel content in the decomposition tower 2 is 50% of the tower inner volume.

[0083] The first heating device 5 and the first cooling device 14 are turned on to control the bottom temperature of the synthesis tower 1 to 85°C and the top temperature of the synthesis tower 1 to 20°C. The second heating device 6 and the second cooling device 23 are turned on to control the bottom temperature of the decomposition tower 2 to 230°C and the top temperature of the decomposition tower 2 to 30°C.

[0084] After the solution in the synthesis tower 1 enters the first heating device 5 from the bottom of the tower for heating, it returns to the tower from the middle and lower part of the synthesis tower 1. At the same time, after the solution in the decomposition tower 2 enters the second heating device 6 for heating, it returns to the tower from the middle and lower part of the decomposition tower 2. The cycle is repeated to provide temperature for the reaction.

[0085] The carbonyl nickel is decomposed in the decomposition tower 2 to generate nickel powder and carbon monoxide. The nickel powder and the remaining carbonyl nickel enter the second pipeline 4. The third cooling device 43 is turned on. The mixture of carbonyl nickel and nickel powder in the second pipeline 4 is cooled to 85° C. after passing through the third cooling device 43. The mixture is pumped into the synthesis tower 1 under the action of the circulation pump 42. The carbon monoxide raw material to be purified is 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 enters the decomposition tower 2 through the first pipeline 3 under the action of the pressure difference to maintain the material circulation balance.

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

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

[0088] The carbon monoxide finished gas collected from the decomposition tower 2 is discharged and subjected to purity analysis. The result is shown in Table 2 below:

[0089]

[0090] Table 2

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

[0092] The above description is only a preferred embodiment of the present invention, and does not limit the patent scope of the present invention. All equivalent structural changes made by using the contents of the present invention specification and drawings under the inventive concept of the present invention, or directly / indirectly applied in other related technical fields are included in the patent protection scope of the present invention.

Claims

1. A carbon monoxide purification process, characterized in that: The steps include: S1: injecting carbonyl nickel into both a synthesis tower (1) and a decomposition tower (2), wherein the synthesis tower (1) and the decomposition tower (2) are connected via 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 circulation pump (42), and the feeding direction of the circulation pump (42) is from the decomposition tower (2) to the synthesis tower (1); S2: introducing the carbon monoxide raw material to be purified into the synthesis tower (1), so that the pressure in the synthesis tower (1) increases to a set first pressure value, and the pressure in the decomposition tower (2) is less than or equal to the first pressure value, and then opening the first control valve (31), the second control valve (41) and the circulation pump (42), so that the carbonyl nickel in the synthesis tower (1) flows into the decomposition tower (2) through the first pipeline (3), and the carbonyl nickel in the decomposition tower (2) flows into 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 and keeping the circulation 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 decomposed carbon monoxide from the upper part of the decomposition tower (2), and at the same time, the nickel powder decomposed in the decomposition tower (2) and the undecomposed carbonyl nickel are pumped into the synthesis tower (1) through the circulation 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 according to claim 1, characterized in that: In step S2, the first pressure value is 1 to 3 MPa, the pressure in the decomposition tower (2) is 1 to 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 that a material circulation balance is formed between the synthesis tower (1) and the decomposition tower (2).

3. The carbon monoxide purification process according to claim 1, characterized in that: In step S3, when the pressure in the synthesis tower (1) is ≥ the first pressure value, the pressure in the synthesis tower (1) is reduced by discharging impurities in the synthesis tower (1).

4. The carbon monoxide purification process according to claim 3, characterized in that: Before the impurity gas in the synthesis tower (1) is discharged, the step of cooling the impurity gas to condense the carbonyl nickel contained in the impurity gas is also included.

5. The carbon monoxide purification process according to claim 1, characterized in that: 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 also included.

6. The carbon monoxide purification process according to claim 1, characterized in that: Step S3 also includes a step of cooling the mixed solution of carbonyl nickel and nickel powder in the second pipe (4) so ​​that the temperature of the mixed solution when it flows into the synthesis tower (1) is 50-90°C.

7. A purification device, characterized in that: The invention comprises a synthesis tower (1) and a decomposition tower (2), wherein the synthesis tower (1) is provided with a raw material inlet (11) for adding a raw material of carbon monoxide to be purified, the upper side of the synthesis tower (1) is also provided with a miscellaneous gas outlet (12) for discharging miscellaneous gas, the miscellaneous gas outlet (12) is connected to a miscellaneous gas outlet valve (13), the upper side of the decomposition tower (2) is provided with a finished product outlet (21) for discharging purified carbon monoxide gas, the finished product outlet (21) is connected to a finished product outlet valve (22), and the synthesis tower (1) and the decomposition tower (2) are connected to each other. A first pipeline (3) and a second pipeline (4) are provided, wherein the first pipeline (3) is provided with a first control valve (31), and 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), and the second pipeline (4) is provided with a circulation pump (42), and the feeding direction of the circulation pump (42) is from the decomposition tower (2) to the synthesis tower (1); The purification equipment further comprises a first heating device (5) and a second heating device (6), wherein the first heating device (5) is connected to the synthesis tower (1) and can heat the synthesis tower (1), and the second heating device (6) is connected to the decomposition tower (2) and can heat the decomposition tower (2).

8. The purification device according to claim 7, characterized in that The purification equipment further comprises a first cooling device (14), the first cooling device (14) being connected to the impurity gas outlet (12), and the first cooling device (14) being capable of cooling the impurity gas before being discharged from the impurity gas outlet (12).

9. The purification device according to claim 7, characterized in that: The purification equipment further comprises a second cooling device (23), wherein the second cooling device (23) is connected to the finished product discharge port (21), and the second cooling device (23) is capable of cooling the carbon monoxide gas before being discharged from the finished product discharge port (21).

10. The purification device according to claim 7, characterized in that A third cooling device (43) is provided on the second pipeline (4), the third cooling device (43) is connected to the second pipeline (4), and the third cooling device (43) is capable of cooling the fluid in the second pipeline (4).

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