Synthesis Device for High-Purity Metal Complex Precursors

Abstract

The present invention relates to the technical field of electronic materials, and provides a synthesis device for a high-purity metal complex precursor. The reaction is carried out by setting a reaction kettle. The reaction kettle is connected to a n-hexane / tetrahydrofuran storage tank, a n-butyllithium storage tank, a DMSO storage tank, a hydrochloric acid aqueous solution dropping tank, a cyclopentadiene / substituted cyclopentadiene dropping tank, a bromopropane / liquefied dimethylamine dropping tank and a solid feeder for adding raw materials. The reaction kettle is connected to a cylinder-cone type three-in-one filter for filtration. The cylinder-cone type three-in-one filter is connected to a distillation kettle / liquid separation kettle for distillation or liquid separation. The distillation kettle / liquid separation kettle is connected to a rectifying column for rectification. The distillation kettle / liquid separation kettle is connected to the reaction kettle for recycling; the distillation kettle / liquid separation kettle is connected to a distillation condenser for distillation condensation to recover raw materials; the present invention can first prepare n-propylcyclopentadiene, then prepare n-propylcyclopentadienyl zirconium trichloride; and finally prepare n-propylcyclopentadienyl tris(dimethylamino)zirconium.

Description

Technical Field

[0001] The present invention relates to the technical field of electronic materials, and particularly to a synthesis device for a high-purity metal complex precursor. Background Art

[0002] The application of high dielectric constant materials (High-K) in ultra-large scale integrated circuits (ULSI) is very necessary. The reason is that when the device size is reduced, the area A of the planar structure also decreases. In order to ensure the capacitance, high dielectric constant materials need to be used. Conventional high dielectric constant materials include oxides of Hf (hafnium), Zr (zirconium), Ta (tantalum), Ti (titanium), Y (yttrium), etc., as well as new materials such as titanate-based doped alkaline earth metal materials, for example: barium strontium titanate (BST), barium zirconate titanate (BZT), etc. Generally, precursor materials of elements such as Hf, Zr, Ta, Ti, Y are used to obtain the above high dielectric constant materials through atomic layer deposition (ALD) or chemical vapor deposition (CVD). Therefore, high-quality precursor materials are the key support for realizing High-K thin film deposition.

[0003] Zirconia thin film has a moderate dielectric constant (K~25) and good compatibility with traditional silicon-based integrated circuit processes. Therefore, it is regarded as the most promising new gate dielectric material. Atomic layer deposition (ALD) technology, as a cutting-edge nanostructure manufacturing technology, forms a smooth, uniform, controllable and high-quality thin film through an ordered self-limiting saturation chemical reaction on the substrate surface, and has good repeatability, making it widely used in the fields of microelectronics science, optical thin films and nanotechnology. In the ALD technology, the process of obtaining an oxide thin film is first to introduce a gaseous precursor, and then the precursor undergoes a chemical reaction on the wafer surface to form the required thin film structure.

[0004] When preparing ZrO2 thin films by atomic layer deposition (ALD) technology, common precursor sources include zirconium tetrakis(dimethylamino), zirconium tetrakis(diethylamino), zirconium tetrakis(methylethylamino), cyclopentadienyltris(dimethylamino)zirconium, etc. These high-purity precursor sources are expensive and mostly need to be imported from abroad. In addition, when using zirconium tetrakis(dimethylamino), zirconium tetrakis(diethylamino), zirconium tetrakis(methylethylamino) as precursors to deposit zirconia thin films, although the film growth rate reaches 0.1 nm / cycle, this rate still cannot fully meet the requirements. Therefore, developing a source material with a faster deposition rate, a simple synthesis process and stable properties is of great significance for improving production efficiency and reducing costs.

[0005] The prior art CN119143814A discloses a synthesis method and device for a metal precursor organic carbonyl cobalt compound. The device includes a reaction kettle, on which a distribution mechanism is arranged. The distribution mechanism includes a rotating shaft and a distribution paddle movably arranged at the first end of the rotating shaft. The distribution paddle is driven to rotate forward to collect filter solids and rotate backward to disperse the filter solids in the distribution paddle. A filter plate is arranged at the first end of the distribution paddle, and a uniform dispersion opening is formed on one side of the distribution paddle. The distribution paddle is driven to rotate forward to collect the filter solids on the filter plate through the uniform dispersion opening. An arc surface part is arranged on the other side of the distribution paddle, and a diversion angle is arranged at the first end of the distribution paddle. The distribution paddle is driven to rotate backward to guide the liquid to flow along the diversion angle and flow rapidly along both ends of the uniform dispersion opening to form a rapid flow area. A dropping mechanism is arranged on the reaction kettle. The dropping mechanism includes a dropping head. A hollow cavity is formed on the rotating shaft, and an annular groove is formed on the hollow cavity. The dropping head alternately sprays liquid drops at a fast and a slow speed. The two liquid drops collide in the annular groove to disperse the liquid drops to the rapid flow area. The distribution paddle is slidably connected to the first end of the rotating shaft. The two distribution paddles are attached to each other and kept in an inclined state as the rotating shaft rises, and the two distribution paddles are attached to the bottom of the reaction kettle and kept in a horizontal state as the rotating shaft descends. Preferably, a rotating chute is formed on the rotating shaft, and a flipping connecting plate arranged on the distribution paddle is slidably connected in the rotating chute. Then this patent is for the synthesis of a metal precursor organic carbonyl cobalt compound. However, currently, it is necessary to synthesize n-propylcyclopentadienyl tris(dimethylamino)zirconium. It is necessary to first synthesize n-propylcyclopentadiene, then synthesize n-propylcyclopentadiene trichloride, and finally synthesize n-propylcyclopentadienyl tris(dimethylamino)zirconium. Therefore, a device that meets this synthesis route is needed. Summary of the Invention

[0006] In view of this, the purpose of the present invention is to provide a synthesis device for a high-purity metal complex precursor to solve the problems in the background technology.

[0007] For the above purposes, the present invention provides a synthesis device for high-purity metal complex precursors, comprising a reaction kettle. A plurality of feeding ports are arranged at the top of the reaction kettle. The plurality of feeding ports are respectively connected through pipelines to a n-hexane / tetrahydrofuran storage tank, a n-butyllithium storage tank, a DMSO storage tank, a hydrochloric acid aqueous solution dropping tank, a cyclopentadiene / substituted cyclopentadiene dropping tank, a bromopropane / liquefied dimethylamine dropping tank, and a solid feeder; the bottom discharge port of the reaction kettle is connected through a pipeline to a cylinder-cone type three-in-one filter. The bottom of the cylinder-cone type three-in-one filter is connected through a pipeline to a distillation kettle / liquid separation kettle. The bottom of the distillation kettle / liquid separation kettle is connected through a pipeline to the reaction kettle. The bottom of the distillation kettle / liquid separation kettle is connected through a pipeline to a rectification column. The bottom of the distillation kettle / liquid separation kettle is also connected through a pipeline to a solid feeding device. The top of the distillation kettle / liquid separation kettle is connected through a pipeline to a distillation condenser. The bottom of the distillation condenser is connected through two pipelines to a DMSO / n-hexane recovery tank and a substituted cyclopentadiene recovery tank respectively. The bottom of the DMSO / n-hexane recovery tank is connected through two pipelines to the n-hexane / tetrahydrofuran storage tank and the DMSO storage tank respectively. The substituted cyclopentadiene recovery tank is connected through a pipeline to the cyclopentadiene / substituted cyclopentadiene dropping tank. The top of the cyclopentadiene / substituted cyclopentadiene dropping tank is also connected through a pipeline to a cyclopentadiene cracking device.

[0008] Preferably, the n-hexane / tetrahydrofuran storage tank, the n-butyllithium storage tank, the DMSO storage tank, the solid feeder, and the top of the distillation kettle / liquid separation kettle are all connected through pipelines to a nitrogen tank. Valves No. 39, valve No. 34, valve No. 1, valve No. 4, and valve No. 7 are respectively arranged on the pipelines connecting the n-hexane / tetrahydrofuran storage tank, the n-butyllithium storage tank, the DMSO storage tank, the solid feeder, and the distillation kettle / liquid separation kettle to the nitrogen tank.

[0009] Preferably, the n-hexane / tetrahydrofuran storage tank and the n-butyllithium storage tank share a pipeline 1 to connect to the reaction kettle. A valve No. 38 is arranged at one end of pipeline 1 close to the reaction kettle. The n-hexane / tetrahydrofuran storage tank and the n-butyllithium storage tank are respectively connected to pipeline 1 through pipeline 2 and pipeline 3. Valves No. 41 and valve No. 37 are respectively arranged at both ends of pipeline 2. Valves No. 35 and valve No. 36 are respectively arranged at both ends of pipeline 2;

[0010] Valves No. 2 and valve No. 3 are respectively arranged at both ends of the pipeline connecting the DMSO storage tank to the reaction kettle.

[0011] Preferably, a valve No. 5 is arranged on the pipeline connecting the solid feeder to the reaction kettle;

[0012] Valves No. 11 and valve No. 12 are respectively arranged at both ends of the pipeline connecting the reaction kettle to the cylinder-cone type three-in-one filter;

[0013] Valves No. 14 and valve No. 16 are respectively arranged at both ends of the pipeline connecting the cylinder-cone type three-in-one filter to the distillation kettle / liquid separation kettle. A pipeline sight glass 1 is arranged on the pipeline between valve No. 14 and valve No. 16;

[0014] The bottom of the cylinder-cone type three-in-one filter is connected to the filter residue quenching treatment device through a pipeline, and a valve thirteen is arranged on the pipeline connecting the cylinder-cone type three-in-one filter and the filter residue quenching treatment device.

[0015] Preferably, the reaction kettle and the rectification tower share a pipeline four to connect to the distillation kettle / liquid separation kettle. Valves seventeen and nineteen are respectively arranged at both ends of the pipeline four. A pipeline sight glass two is arranged between the valve seventeen and the valve nineteen on the pipeline four. The pipeline four is connected to the solid feeding device through a pipeline between the valve nineteen and the pipeline sight glass two, and a valve forty-three is arranged on the pipeline connecting the solid feeding device and the pipeline four;

[0016] The reaction kettle and the rectification tower are respectively connected to the pipeline four through a pipeline five and a pipeline six. Valves twenty-one and twenty-two are respectively arranged at both ends of the pipeline five, and a valve forty-four is arranged on the pipeline six;

[0017] A valve twenty-three is arranged on the pipeline connecting the distillation kettle / liquid separation kettle and the distillation condenser. A pipeline seven is connected to the bottom of the distillation condenser. A pipeline sight glass three is arranged on the pipeline seven. The pipeline seven is respectively connected to the DMSO / n-hexane recovery tank and the substituted cyclopentadiene recovery tank through a pipeline eight and a pipeline nine. A valve twenty-six is arranged on the pipeline eight, and a valve twenty-five is arranged on the pipeline nine;

[0018] The distillation condenser is connected to a vacuum pump through a pipeline, and a valve twenty-seven is arranged on the pipeline connecting the distillation condenser and the vacuum pump.

[0019] Preferably, the bottom of the DMSO / n-hexane recovery tank is connected to a pipeline ten, and a valve twenty-eight is arranged on the pipeline ten. The pipeline ten is respectively connected to the n-hexane / tetrahydrofuran storage tank and the DMSO storage tank through a pipeline eleven and a pipeline twelve. Valves forty and forty-two are respectively arranged at both ends of the pipeline eleven, and valves thirty-one and thirty are respectively arranged at both ends of the pipeline twelve;

[0020] The bottom of the substituted cyclopentadiene recovery tank is connected to a pipeline thirteen. Valves twenty-nine and thirty-two are respectively arranged at both ends of the pipeline thirteen. The pipeline thirteen is connected to a pipeline fourteen, and the pipeline fourteen is connected to the cyclopentadiene / substituted cyclopentadiene dropping tank. A valve thirty-three is arranged on the pipeline fourteen. The pipeline fourteen is connected to a cracking to produce cyclopentadiene device through a pipeline fifteen, and a valve six is arranged on the pipeline fifteen;

[0021] Valves ten, eight and nine are respectively arranged on the pipelines connecting the hydrochloric acid aqueous solution dropping tank, the cyclopentadiene / substituted cyclopentadiene dropping tank, and the bromopropane / liquefied dimethylamine dropping tank to the feeding port of the reaction kettle.

[0022] Preferably, the reaction kettle, the cylinder-cone type three-in-one filter and the distillation kettle / liquid separation kettle are respectively provided with a stirrer one, a stirrer two and a stirrer three.

[0023] Advantages of the present invention: The present invention conducts reactions through a reaction kettle, which is connected to a n-hexane / tetrahydrofuran storage tank, a n-butyllithium storage tank, a DMSO storage tank, a hydrochloric acid aqueous solution dropping tank, a cyclopentadiene / substituted cyclopentadiene dropping tank, a bromopropane / liquefied dimethylamine dropping tank, and a solid feeder for adding raw materials. The reaction kettle is connected to a cylinder-cone type three-in-one filter for filtration. The cylinder-cone type three-in-one filter is connected to a distillation kettle / liquid separation kettle for distillation or liquid separation. The distillation kettle / liquid separation kettle is connected to a rectifying column for rectification. The distillation kettle / liquid separation kettle is connected to the reaction kettle for recycling; the distillation kettle / liquid separation kettle is connected to a distillation condenser for distillation condensation to recover raw materials. The present invention can first prepare n-propylcyclopentadiene by using DMSO, sodium hydroxide solid, cyclopentadiene, bromopropane, acid aqueous solution drop, and anhydrous sodium sulfate, and then prepare n-propylcyclopentadienyl zirconium trichloride by using n-propylcyclopentadiene, n-butyllithium, n-hexane, tetrahydrofuran, and zirconium tetrachloride; finally, prepare n-propylcyclopentadienyl tris(dimethylamino)zirconium by using n-propylcyclopentadienyl zirconium trichloride, n-hexane, and liquefied dimethylamine. Description of the Drawings

[0024] In order to more clearly illustrate the technical solutions in the present invention or the prior art, the following will briefly introduce the drawings required for the description of the embodiments or the prior art. Obviously, the following drawings are only those of the present invention. For those of ordinary skill in the art, without creative efforts, other drawings can also be obtained based on these drawings.

[0025] Figure 1 It is a schematic diagram of the overall device of the present invention;

[0026] The marks in the figure are:

[0027] 1. Valve 1; 2. Valve 2; 3. Valve 3; 4. Valve 4; 5. Valve 5; 6. Valve 6; 7. Valve 7; 8. Valve 8; 9. Valve 9; 10. Valve 10; 11. Valve 11; 12. Valve 12; 13. Valve 13; 14. Valve 14; 15. Pipe sight glass 1; 16. Valve 16; 17. Valve 17; 18. Pipe sight glass 2; 19. Valve 19; 20. Vacuum pump; 21. Valve 21; 22. Valve 22; 23. Valve 23; 24. Pipe sight glass 3; 25. Valve 25; 26. Valve 26; 27. Valve 27; 28. Valve 28; 29. Valve 29; 30. Valve 30; 31. Valve 31; 32. Valve 32; 33. Valve 33; 34. Valve 34; 35. Valve 35; 36. Valve 36; 37. Valve 37; 38. Valve 38; 39. Valve 39; 40. Valve 40; 41. Valve 41; 42. Valve 42; 43. Valve 43; 44. Valve 44; 45. Reactor; 46. n-Hexane / Tetrahydrofuran storage tank; 47. n-Butyllithium storage tank; 48. DMSO storage tank; 49. Hydrochloric acid aqueous solution dropping tank; 50. Cyclopentadiene / Substituted cyclopentadiene dropping tank; 51. Propyl bromide / Liquid dimethylamine dropping tank; 52. Solid feeder; 53. Cylindrical-conical three-in-one filter; 54. Distillation kettle / liquid separation kettle; 55. Agitator 3; 56. Rectifying column; 57. Distillation condenser; 58. DMSO / n-Hexane recovery tank; 59. Substituted cyclopentadiene recovery tank; 60. Cracking device for preparing cyclopentadiene; 61. Nitrogen tank; 62. Agitator 1; 63. Agitator 2; 64. Solid feeding device; 65. Filter residue quenching treatment device. Detailed implementation manners

[0028] To make the objectives, technical solutions and advantages of the present invention clearer and more understandable, the present invention will be further described in detail below in conjunction with specific embodiments.

[0029] It should be noted that unless otherwise defined, the technical terms or scientific terms used in the present invention should have the ordinary meanings understood by those with ordinary skills in the field to which the present invention belongs. The "first", "second" and similar terms used in the present invention do not represent any order, quantity or importance, but are only used to distinguish different components. The terms such as "including" or "comprising" mean that the elements or objects appearing before this term cover the elements or objects listed after this term and their equivalents, without excluding other elements or objects. The terms such as "connected" or "coupled" are not limited to physical or mechanical connections, but may include electrical connections, whether direct or indirect. The terms such as "upper", "lower", "left" and "right" are only used to represent relative positional relationships, and when the absolute position of the object being described changes, the relative positional relationship may also change accordingly.

[0030] As Figure 1 shown, this embodiment provides a synthesis device for a high-purity metal complex precursor, including a reaction kettle 45. A plurality of feeding ports are arranged at the top of the reaction kettle 45. The plurality of feeding ports are respectively connected to a n-hexane / tetrahydrofuran storage tank 46, a n-butyllithium storage tank 47, a DMSO storage tank 48, a hydrochloric acid aqueous solution dropping tank 49, a cyclopentadiene / substituted cyclopentadiene dropping tank 50, a bromopropane / liquefied dimethylamine dropping tank 51, and a solid feeder 52 through pipelines;

[0031] The n-hexane / tetrahydrofuran storage tank 46 and the n-butyllithium storage tank 47 share a pipeline one to connect to the reaction kettle 45. A valve thirty-eight 38 is arranged at one end of the pipeline one close to the reaction kettle 45. The n-hexane / tetrahydrofuran storage tank 46 and the n-butyllithium storage tank 47 are respectively connected to the pipeline one through a pipeline two and a pipeline three. A valve forty-one 41 and a valve thirty-seven 37 are respectively arranged at both ends of the pipeline two. A valve thirty-five 35 and a valve thirty-six 36 are respectively arranged at both ends of the pipeline two;

[0032] Valves two 2 and three 3 are respectively arranged at both ends of the pipeline connecting the DMSO storage tank 48 to the reaction kettle 45. A valve five 5 is arranged on the pipeline connecting the solid feeder 52 to the reaction kettle 45.

[0033] The bottom discharge port of the reaction kettle 45 is connected to a cylinder-cone type three-in-one filter 53 through a pipeline. The bottom of the cylinder-cone type three-in-one filter 53 is connected to a distillation kettle / liquid separation kettle 54 through a pipeline. The bottom of the distillation kettle / liquid separation kettle 54 is connected to the reaction kettle 45 through a pipeline. Valves eleven 11 and twelve 12 are respectively arranged at both ends of the pipeline connecting the reaction kettle 45 to the cylinder-cone type three-in-one filter 53;

[0034] Valves fourteen 14 and sixteen 16 are respectively arranged at both ends of the pipeline connecting the cylinder-cone type three-in-one filter 53 to the distillation kettle / liquid separation kettle 54. A pipeline sight glass one 15 is arranged on the pipeline between the valve fourteen 14 and the valve sixteen 16;

[0035] The bottom of the cylinder-cone type three-in-one filter 53 is connected to a filter residue quenching treatment device 65 through a pipeline. A valve thirteen 13 is arranged on the pipeline connecting the cylinder-cone type three-in-one filter 53 to the filter residue quenching treatment device 65.

[0036] The bottom of the distillation kettle / liquid separation kettle 54 is connected to a rectifying column 56 through a pipeline. The bottom of the distillation kettle / liquid separation kettle 54 is also connected to a solid feeding device 64 through a pipeline. The top of the distillation kettle / liquid separation kettle 54 is connected to a distillation condenser 57 through a pipeline. The bottom of the distillation condenser 57 is connected to a DMSO / n-hexane recovery tank 58 and a substituted cyclopentadiene recovery tank 59 respectively through two pipelines. The bottom of the DMSO / n-hexane recovery tank 58 is connected to a n-hexane / tetrahydrofuran storage tank 46 and a DMSO storage tank 48 respectively through two pipelines. The substituted cyclopentadiene recovery tank 59 is connected to a cyclopentadiene / substituted cyclopentadiene dropping tank 50 through a pipeline. The top of the cyclopentadiene / substituted cyclopentadiene dropping tank 50 is also connected to a cracking device for producing cyclopentadiene 60 through a pipeline;

[0037] The reaction kettle 45 and the rectifying column 56 share a pipeline four to connect to the distillation kettle / liquid separation kettle 54. Valves seventeen 17 and nineteen 19 are respectively arranged at both ends of the pipeline four. A pipeline sight glass two 18 is arranged between the valve seventeen 17 and the valve nineteen 19 on the pipeline four. The pipeline four is connected to the solid feeding device 64 through a pipeline between the valve nineteen 19 and the pipeline sight glass two 18. A valve forty-three 43 is arranged on the pipeline connecting the solid feeding device 64 to the pipeline four;

[0038] The reaction kettle 45 and the rectifying column 56 are respectively connected to the pipeline four through a pipeline five and a pipeline six. Valves twenty-one 21 and twenty-two 22 are respectively arranged at both ends of the pipeline five. A valve forty-four 44 is arranged on the pipeline six;

[0039] A valve twenty-three 23 is arranged on the pipeline connecting the distillation kettle / liquid separation kettle 54 to the distillation condenser 57,

[0040] The bottom of the distillation condenser 57 is connected to a pipeline seven. A pipeline sight glass three 24 is arranged on the pipeline seven. The pipeline seven is respectively connected to the DMSO / n-hexane recovery tank 58 and the substituted cyclopentadiene recovery tank 59 through a pipeline eight and a pipeline nine. A valve twenty-six 26 is arranged on the pipeline eight. A valve twenty-five 25 is arranged on the pipeline nine;

[0041] The distillation condenser 57 is connected to a vacuum pump 20 through a pipeline. A valve twenty-seven 27 is arranged on the pipeline connecting the distillation condenser 57 to the vacuum pump 20;

[0042] The bottom of the DMSO / n-hexane recovery tank 58 is connected to a pipeline ten. A valve twenty-eight 28 is arranged on the pipeline ten. The pipeline ten is respectively connected to the n-hexane / tetrahydrofuran storage tank 46 and the DMSO storage tank 48 through a pipeline eleven and a pipeline twelve. Valves forty 40 and forty-two 42 are respectively arranged at both ends of the pipeline eleven. Valves thirty-one 31 and thirty 30 are respectively arranged at both ends of the pipeline twelve;

[0043] The bottom of the substituted cyclopentadiene recovery tank 59 is connected to pipeline thirteen. Valve twenty-nine 29 and valve thirty-two 32 are respectively arranged at both ends of pipeline thirteen. Pipeline thirteen is connected to pipeline fourteen, and pipeline fourteen is connected to the cyclopentadiene / substituted cyclopentadiene dropping tank 50. Valve thirty-three 33 is arranged on pipeline fourteen. Pipeline fourteen is connected to the cracking unit for producing cyclopentadiene 60 through pipeline fifteen, and valve six 6 is arranged on pipeline fifteen;

[0044] On the pipelines connecting the hydrochloric acid aqueous solution dropping tank 49, the cyclopentadiene / substituted cyclopentadiene dropping tank 50, and the bromopropane / liquefied dimethylamine dropping tank 51 to the feeding port of the reaction kettle 45, valves ten 10, valve eight 8, and valve nine 9 are respectively arranged.

[0045] The top of the n-hexane / tetrahydrofuran storage tank 46, the n-butyllithium storage tank 47, the DMSO storage tank 48, the solid feeder 52, and the distillation kettle / separating kettle 54 are all connected to the nitrogen tank 61 through pipelines. Valves thirty-nine 39, valve thirty-four 34, valve one 1, valve four 4, and valve seven 7 are respectively arranged on the pipelines connecting the n-hexane / tetrahydrofuran storage tank 46, the n-butyllithium storage tank 47, the DMSO storage tank 48, the solid feeder 52, and the distillation kettle / separating kettle 54 to the nitrogen tank 61. The n-hexane / tetrahydrofuran storage tank 46 and the n-butyllithium storage tank 47 share a pipeline one to connect to the reaction kettle 45. Valve thirty-eight 38 is arranged at one end of pipeline one close to the reaction kettle 45. The n-hexane / tetrahydrofuran storage tank 46 and the n-butyllithium storage tank 47 are respectively connected to pipeline one through pipeline two and pipeline three. Valves forty-one 41 and valve thirty-seven 37 are respectively arranged at both ends of pipeline two. Valves thirty-five 35 and valve thirty-six 36 are respectively arranged at both ends of pipeline two;

[0046] The reaction kettle 45, the cylinder-cone type three-in-one filter 53, and the distillation kettle / separating kettle 54 are respectively provided with stirrer one 62, stirrer two 63, and stirrer three 55.

[0047] Open Valve 1, Valve 2, and Valve 3, and use nitrogen pressure to quantitatively transfer 6 L of DMSO in the DMSO storage tank 48 to the reaction kettle 45. Open Valve 5, and quantitatively transfer 416 g of sodium hydroxide solid in the solid feeder 52 to the reaction kettle 45. Start the stirrer 62 of the reaction kettle 45, and at the same time cool the materials in the reaction kettle 45 to 0 °C. Then open Valve 8, and slowly add 767 g of cyclopentadiene in the cyclopentadiene / substituted cyclopentadiene dropping tank 50 dropwise to the reaction kettle 45. After the dropping is completed, slowly return to room temperature and continue stirring for 3 h. Then open Valve 9, and slowly add 1230 g of 1-bromopropane in the 1-bromopropane / dimethylamine solution dropping tank 51 dropwise to the reaction kettle 45. After the dropping is completed, continue stirring for 12 h. Then open Valve 10, and add a mixed solution of 120 mL of HCl and 1600 mL of water in the hydrochloric acid aqueous solution dropping tank 49 dropwise to the reaction kettle 45. After the dropping is completed, open Valve 11, Valve 12, Valve 14, and Valve 16 in sequence, and transfer the materials in the reaction kettle 45 to the cylinder-cone type three-in-one filter 53 for filtration. The filtrate enters the distillation kettle / liquid separation kettle 54. After confirming the liquid separation through the bottom pipeline sight glass 2 of the distillation kettle / liquid separation kettle 54, open Valve 17, Valve 19, Valve 21, and Valve 22 in sequence, and transfer the lower organic phase to the synthesis kettle 45. Confirm the liquid level of the organic phase and the aqueous phase through the pipeline sight glass 2. Then add anhydrous sodium sulfate to the reaction kettle 45 through the solid feeder 52 to dry and remove water from the organic phase. After the water removal is completed, transfer the mixed material of the organic phase and anhydrous sodium sulfate to the cylinder-cone type three-in-one filter 53 for filtration. The filtrate enters the distillation kettle / liquid separation kettle 54. Open Valve 23 and Valve 25, and use vacuum distillation to separate DMSO into the DMSO / n-hexane recovery tank 58. Then close Valve 25, open Valve 26, and use vacuum distillation to control the vacuum degree at 13 - 15 torr, and collect 681.5 g of the fraction with an internal temperature of 26 °C into the substituted cyclopentadiene recovery tank 59. Use gas chromatography to detect the purity of n-propylcyclopentadiene to be 97% and the yield to be 63%.

[0048] Open valves thirty-four (34), thirty-five (35), thirty-six (36), and thirty-eight (38), and quantitatively transfer 1680 mL of n-butyllithium in the n-butyllithium storage tank (47) to the reaction kettle (45) by nitrogen pressure feeding. Then close valves thirty-four (34), thirty-five (35), and thirty-six (36), open valves thirty-nine (39), forty-one (41), and thirty-seven (37), and quantitatively transfer 2 L of n-hexane in the n-hexane / tetrahydrofuran storage tank (46) to the reaction kettle (45) by nitrogen pressure feeding. Then cool the reaction kettle (45) to 0 °C, open valves twenty-nine (29), thirty-two (32), and thirty-three (33), and transfer the n-propylcyclopentadiene in the substituted cyclopentadiene recovery tank (59) to the cyclopentadiene / substituted cyclopentadiene dropping tank (50) by nitrogen pressure feeding. Then slowly and quantitatively drop 433 g of n-propylcyclopentadiene in the cyclopentadiene / substituted cyclopentadiene dropping tank (50) into the reaction (45). After the dropping is completed, continue the reaction for 2 h. Then successively open valves thirty-nine (39), forty-one (41), thirty-seven (37), and thirty-eight (38), and quantitatively transfer 0.8 L of tetrahydrofuran in the n-hexane / tetrahydrofuran storage tank (46) to the reaction kettle (45) by nitrogen pressure feeding. Then add 886 g of zirconium tetrachloride in the solid feeder (52) to the reaction kettle (45) in two batches, then slowly return to room temperature, and continue stirring and reacting for 12 h. Then transfer the materials in the reaction kettle (45) to the cylinder-cone type three-in-one filter (53) for filtration. The filtrate enters the distillation kettle / liquid separation kettle (54). After the solvent is drained, open valves seventeen (17) and forty-three (43) to obtain 868.4 g of n-propylcyclopentadiene zirconium trichloride, with a yield of 75%.

[0049] Transfer 487.6 g of n-propylcyclopentadienyl zirconium trichloride to the solid feeder (52) through the solid feeding device (64).

[0050] Open valves 34, 35, 36, and 38, and quantitatively transfer 1985 mL of n-butyllithium in the n-butyllithium storage tank 47 to the reaction kettle 45 by means of nitrogen gas pressure feeding. Then close valves 34, 35, and 36, open valves 39, 41, and 37, and quantitatively transfer 2 L of n-hexane in the n-hexane / tetrahydrofuran storage tank 46 to the reaction kettle 45 by means of nitrogen gas pressure feeding. Then cool the reaction kettle 45 to -10 °C, and then quantitatively add 252.8 g of liquefied dimethylamine in the bromopropane / liquefied dimethylamine dropping tank 51 dropwise to the reaction kettle 45. After the dropping is completed, continue the reaction for 2 h. Then add 487.6 g of n-propylcyclopentadienylzirconium trichloride in the solid feeder 52 to the reaction kettle 45 in two batches. Then slowly restore to room temperature and react for 12 hours. Then transfer the material in the reaction kettle 45 to the cylinder-cone type three-in-one filter 53 for filtration. The filtrate enters the distillation kettle / liquid separation kettle 54 to drain the solvent. Then open valves 17, 19, and 44, and transfer the material in the distillation kettle / liquid separation kettle 54 into the rectification column 56 for vacuum rectification to obtain 439 g of n-propylcyclopentadienyltris(dimethylamino)zirconium with a yield of 83%.

[0051] Those of ordinary skill in the art should understand that the discussion of any of the above embodiments is only exemplary and is not intended to imply that the scope of the present invention is limited to these examples; under the concept of the present invention, the technical features in the above embodiments or different embodiments can also be combined, the steps can be implemented in any order, and there are many other variations in different aspects of the present invention as described above, which are not provided in detail for the sake of brevity. Any omission, modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention shall be included within the protection scope of the present invention.

Claims

1. A synthesis device for a high-purity metal complex precursor, comprising a reaction vessel (45), characterized in that: The top of the reactor (45) is provided with a plurality of feeding ports, which are respectively connected to an n-hexane / tetrahydrofuran storage tank (46), an n-butyl lithium storage tank (47), a DMSO storage tank (48), a hydrochloric acid aqueous solution dropping tank (49), a cyclopentadiene / substituted cyclopentadiene dropping tank (50), a bromopropane / liquefied dimethylamine dropping tank (51) and a solid feeder (52) through pipelines; the bottom discharge port of the reactor (45) is connected to a cylindrical-conical three-in-one filter (53) through a pipeline, the bottom of the cylindrical-conical three-in-one filter (53) is connected to a distillation kettle / liquid separator (54) through a pipeline, the bottom of the distillation kettle / liquid separator (54) is connected to the reactor (45) through a pipeline, and the bottom of the distillation kettle / liquid separator (54) is connected to a rectification tower through a pipeline. (56), the bottom of the distillation kettle / liquid separator (54) is also connected to the solid feeding device (64) through a pipeline, the top of the distillation kettle / liquid separator (54) is connected to the distillation condenser (57) through a pipeline, the bottom of the distillation condenser (57) is respectively connected to the DMSO / n-hexane recovery tank (58) and the substituted cyclopentadiene recovery tank (59) through two pipelines, the bottom of the DMSO / n-hexane recovery tank (58) is respectively connected to the n-hexane / tetrahydrofuran storage tank (46) and the DMSO storage tank (48) through two pipelines, the substituted cyclopentadiene recovery tank (59) is connected to the cyclopentadiene / substituted cyclopentadiene dropping tank (50) through a pipeline, and the top of the cyclopentadiene / substituted cyclopentadiene dropping tank (50) is also connected to the cracking cyclopentadiene device (60) through a pipeline.

2. The synthesis device of the high-purity metal complex precursor according to claim 1, characterized in that: The tops of the n-hexane / tetrahydrofuran storage tank (46), the n-butyl lithium storage tank (47), the DMSO storage tank (48), the solid feeder (52) and the distillation kettle / liquid separator (54) are all connected to the nitrogen tank (61) via pipelines. The pipelines connecting the n-hexane / tetrahydrofuran storage tank (46), the n-butyl lithium storage tank (47), the DMSO storage tank (48), the solid feeder (52) and the distillation kettle / liquid separator (54) to the nitrogen tank (61) are respectively provided with valve thirty-nine (39), valve thirty-four (34), valve one (1), valve four (4) and valve seven (7).

3. The synthesis device of the high-purity metal complex precursor according to claim 2, characterized in that: The n-hexane / tetrahydrofuran storage tank (46) and the n-butyl lithium storage tank (47) are connected to the reactor (45) through a common pipeline 1. A valve 38 (38) is provided at one end of the pipeline 1 close to the reactor (45). The n-hexane / tetrahydrofuran storage tank (46) and the n-butyl lithium storage tank (47) are connected to the pipeline 1 through pipeline 2 and pipeline 3 respectively. A valve 41 (41) and a valve 37 (37) are provided at both ends of the pipeline 2 respectively. A valve 35 (35) and a valve 36 (36) are provided at both ends of the pipeline 2 respectively. A valve 2 (2) and a valve 3 (3) are provided at both ends of the pipeline connecting the DMSO storage tank (48) to the reactor (45). A valve 5 (5) is provided on the pipeline connecting the solid feeder (52) to the reactor (45).

4. The synthesis device of the high-purity metal complex precursor according to claim 3, characterized in that: The two ends of the pipeline connecting the reaction kettle (45) to the cylindrical-conical three-in-one filter (53) are respectively provided with valve eleven (11) and valve twelve (12); the two ends of the pipeline connecting the cylindrical-conical three-in-one filter (53) to the distillation kettle / liquid separation kettle (54) are respectively provided with valve fourteen (14) and valve sixteen (16), and a pipeline sight glass one (15) is provided on the pipeline between valve fourteen (14) and valve sixteen (16); the bottom of the cylindrical-conical three-in-one filter (53) is connected to the filter residue quenching treatment device (65) through a pipeline, and a valve thirteen (13) is provided on the pipeline connecting the cylindrical-conical three-in-one filter (53) to the filter residue quenching treatment device (65).

5. The synthesis device of the high-purity metal complex precursor according to claim 4, characterized in that: The reaction kettle (45) and the distillation tower (56) are connected to the distillation kettle / liquid separation kettle (54) through a common pipeline 4, and valve 17 (17) and valve 19 (19) are respectively provided at both ends of the pipeline 4. A pipeline sight glass 2 (18) is provided on the pipeline 4 between valve 17 (17) and valve 19 (19). The pipeline 4 is connected to the solid feeding device (64) through a pipeline between valve 19 (19) and pipeline sight glass 2 (18). A valve 43 (43) is provided on the pipeline connecting the solid feeding device (64) to the pipeline 4. The reaction kettle (45) and the distillation tower (56) are connected to the pipeline 4 through pipeline 5 and pipeline 6 respectively. Valve 21 (21) and valve 22 (43) are respectively provided at both ends of the pipeline 5. 22), a valve forty-four (44) is provided on the pipeline six; a valve twenty-three (23) is provided on the pipeline connecting the distillation kettle / liquid separation kettle (54) to the distillation condenser (57); the bottom of the distillation condenser (57) is connected to a pipeline seven, a pipeline sight glass three (24) is provided on the pipeline seven, the pipeline seven is connected to the DMSO / n-hexane recovery tank (58) and the substituted cyclopentadiene recovery tank (59) through pipeline eight and pipeline nine respectively, a valve twenty-six (26) is provided on the pipeline eight, and a valve twenty-five (25) is provided on the pipeline nine; the distillation condenser (57) is connected to the vacuum pump (20) through a pipeline, and a valve twenty-seven (27) is provided on the pipeline connecting the distillation condenser (57) to the vacuum pump (20).

6. The synthesis device of the high-purity metal complex precursor according to claim 5, characterized in that: The bottom of the DMSO / n-hexane recovery tank (58) is connected to pipeline 10, on which a valve 28 (28) is provided. Pipeline 10 is connected to the n-hexane / tetrahydrofuran storage tank (46) and the DMSO storage tank (48) through pipeline 11 and pipeline 12, respectively. Both ends of pipeline 11 are provided with valve 40 (40) and valve 42 (42), and both ends of pipeline 12 are provided with valve 31 (31) and valve 30 (30). The bottom of the substituted cyclopentadiene recovery tank (59) is connected to pipeline 13, and both ends of pipeline 13 are provided with valve 29 (29) and valve 30. 2 (32), pipeline thirteen is connected to pipeline fourteen, pipeline fourteen is connected to the cyclopentadiene / substituted cyclopentadiene dropping tank (50), pipeline fourteen is provided with valve thirty-three (33), pipeline fourteen is connected to the cracking cyclopentadiene production device (60) through pipeline fifteen, and pipeline fifteen is provided with valve six (6); the pipelines connecting the hydrochloric acid aqueous solution dropping tank (49), the cyclopentadiene / substituted cyclopentadiene dropping tank (50), and the bromopropane / liquefied dimethylamine dropping tank (51) to the feed port of the reaction kettle (45) are respectively provided with valve ten (10), valve eight (8) and valve nine (9).

7. The synthesis device of the high-purity metal complex precursor according to claim 1, characterized in that: The reaction kettle (45), the cylindrical-conical three-in-one filter (53) and the distillation kettle / liquid separation kettle (54) are respectively provided with a stirrer 1 (62), a stirrer 2 (63) and a stirrer 3 (55).

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