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CN-116920747-B - Synthetic device system and synthetic method of methylethylamine

CN116920747BCN 116920747 BCN116920747 BCN 116920747BCN-116920747-B

Abstract

The invention relates to a synthesizing device system and a synthesizing method of methyl ethylamine, wherein the synthesizing device system comprises a formic acid acetamide preparation unit, a reduction unit, a filtering unit and a rectifying unit; the synthesis method corresponds to the synthesis device system, and when the synthesis device system of the methylethylamine is used for synthesizing the methylethylamine, an organic solvent is not required to be added when the preparation of the methylacetamide is carried out, after the synthesis is finished, other complex post-treatment processes are not required, and the methylethylamine product can be efficiently obtained only by simple rectification, so that the production efficiency of the synthesis device system of the methylethylamine can be greatly improved, and the preparation cost of the methylethylamine is reduced.

Inventors

  • ZHANG DONGYANG
  • DONG YUCHENG
  • CHEN JIANYONG
  • SUN QINGYE

Assignees

  • 天津绿菱气体有限公司

Dates

Publication Date
20260505
Application Date
20230728

Claims (16)

  1. 1. A synthesis device system of methylethylamine, which is characterized by comprising a formate acetamide preparation unit, a reduction unit, a filtration unit and a rectification unit; The preparation unit of the formic acid acetamide comprises an ethylamine supply device, a methyl formate supply device, a first reaction device and a formic acid acetamide storage device, wherein the discharge ports of the methyl formate supply device and the ethylamine supply device are respectively connected with the feed inlet of the first reaction device; The reducing unit comprises a reducing agent supply device, an acid liquid supply device, an organic solvent supply device and a second reaction device, wherein the discharge port of the formate-acetamide storage device is connected with the feed port of the second reaction device; The filtering unit comprises a reaction liquid storage device, an alkali liquor supply device, a filtering device and a filtrate storage device, wherein a discharge hole of the second reaction device and a discharge hole of the alkali liquor supply device are respectively connected with a feed hole of the reaction liquid storage device; The rectification unit comprises a first rectification device, a second rectification device, a methyl ethylamine storage tank, a rectification liquid storage tank, a waste liquid storage tank and a solvent recovery tank, wherein the filtrate storage device is connected with a feed inlet of the first rectification device, a light phase outlet of the first rectification device is connected with the methyl ethylamine storage tank, a heavy phase outlet of the first rectification device is connected with the feed inlet of the rectification liquid storage tank, a discharge outlet of the rectification liquid storage tank is connected with the feed inlet of the second rectification device, a heavy phase outlet of the second rectification device is connected with the waste liquid storage tank, and a light phase outlet of the second rectification device is connected with the solvent recovery tank.
  2. 2. The synthesis apparatus system of claim 1, wherein the acetamide formate preparation unit further comprises a condensing means and a condensate storage means connected in sequence; The feed inlet of the condensing device is connected with the gas outlet of the first reaction device; the outlet of the condensate storage device is connected with a methyl formate supply device.
  3. 3. The synthesis plant system of claim 1, wherein the solvent recovery tank is connected to an organic solvent supply via a pipeline.
  4. 4. The synthesis device system of claim 1, wherein the filtration device comprises at least two filters connected in parallel.
  5. 5. A method for synthesizing methylethylamine, wherein the method for synthesizing methylethylamine is performed in the system of the apparatus for synthesizing methylethylamine according to any one of claims 1 to 4, the method comprising the steps of: (1) Mixing ethylamine and methyl formate, heating and refluxing to react, and separating redundant methyl formate after the reaction is finished to obtain acetamide formate; (2) Mixing a reducing agent solution, an acid solution and the formic acid acetamide obtained in the step (1), and heating and refluxing for reaction to obtain a reaction solution; the reducing agent solution is obtained by mixing a reducing agent and an organic solvent; The acid liquor is mixed acid liquor of organic acid and organic solvent; (3) And regulating the pH value of the reaction solution to be more than or equal to 10, then carrying out solid-liquid separation, and carrying out first rectification on the obtained filtrate, wherein the light phase component obtained by the first rectification is the methylethylamine.
  6. 6. The synthesis method according to claim 5, wherein the material ratio of the ethylamine to the methyl formate in the step (1) is as follows: 80-120g of ethylamine was added per 1L of methyl formate.
  7. 7. The method of claim 5, wherein the reducing agent in the reducing agent solution of step (2) is sodium borohydride.
  8. 8. The method of claim 7, wherein the molar ratio of sodium borohydride to ethylamine is 1 (0.8-1.2).
  9. 9. The method according to claim 5, wherein the organic acid in the acid solution is acetic acid.
  10. 10. The method according to claim 5, wherein the concentration of the organic acid in the acid solution is 8 to 12mol/L.
  11. 11. The method of claim 9, wherein the molar ratio of acetic acid to ethylamine is 1 (0.8-1.2).
  12. 12. The method according to claim 5, wherein the organic solvent is tetrahydrofuran.
  13. 13. The method of claim 12, wherein the reducing agent solution is used in an amount of 0.45 to 0.55L of tetrahydrofuran per 100g of ethylamine.
  14. 14. The method of synthesis according to claim 5, further comprising, after step (3): (4) And (3) carrying out second rectification on the heavy phase component obtained by the first rectification, wherein the light component obtained by the second rectification is an organic solvent.
  15. 15. The method of claim 14, wherein the light fraction from the second rectification is recycled to the reducing agent solution and the acid solution.
  16. 16. The method according to claim 5, wherein the methyl formate separated in the step (1) is reused for the reaction of ethylamine with methyl formate.

Description

Synthetic device system and synthetic method of methylethylamine Technical Field The invention relates to the technical field of organic synthesis, relates to a synthesis device system and a synthesis method, and in particular relates to a synthesis device system and a synthesis method of methylethylamine. Background Semiconductor precursors refer to chemicals used in the manufacture of semiconductor crystals during the manufacture of semiconductor devices, which are the basis for the manufacture of semiconductor devices and have a critical impact on the performance and quality of the semiconductor devices. Semiconductor precursor materials are represented by compounds of transition metals zirconium and hafnium, which constitute a series of precursor materials, wherein zirconium oxide and hafnium oxide are the most important materials among the precursor materials with high dielectric constants and thermodynamic stability, but the synthesis of zirconium oxide and hafnium oxide generally needs to be completed at extremely low temperatures, and the process of forming the deposit is irreversible and self-limiting, in order to make up for the shortages of zirconium oxide and hafnium oxide, researchers have developed zirconium tetramine. Compared with the semiconductor precursor material in the form of oxide, the tetramethyl ethylamino zirconium has the advantages of simple and convenient synthesis conditions, purification and post-treatment processes in the liquid state, repeatability in the gasification deposition process and no dust or powder pollution to the substrate. And methylethylamine (N-ethylmethylamine, EMA) is one of the important ligands for the formation of zirconium tetramethylethylamide. The Eschweiler-clsanark reaction is to react carbonyl compounds such as aldehyde or ketone with amine, and take formic acid as reducing agent to heat and obtain an alkylation product of the amine. The amine can react with aldehyde or ketone to generate Schiff base, ni or Pd is used as a catalyst under the condition of pressurization, and carbon-nitrogen double bonds can be reduced through hydrogenation reaction, so that monoalkyl substituted secondary amine can be generated efficiently, but the stability of Schiff base generated by simple amine and aldehyde ketone is poor, and the stable product of Schiff base generated by ethylamine and formaldehyde is not easy to obtain. The primary amine is introduced with the benzyl protecting group and is subjected to methylation, and finally the benzyl protecting group is removed by Pd/C catalysis, so that the primary amine can be effectively prevented from being polysubstituted to generate tertiary amine, the product has better singleness, but the steps are more involved in mass production, and the methylation reagent has higher toxicity and is easy to pollute the environment, so that the method is contrary to the ideas of enterprise cost reduction, efficiency enhancement and environmental protection. Disclosure of Invention Aiming at the defects of the prior art, the invention aims to provide a synthesis device system and a synthesis method of methyl ethylamine, wherein the synthesis method is matched with the synthesis device system, an organic solvent is not required to be added in the initial stage of preparing the methyl ethylamine, and a complex post-treatment process is not required after the reaction, so that the system has higher production efficiency, and the production cost in the production process is reduced. In order to achieve the aim of the invention, the invention adopts the following technical scheme: in a first aspect, the present invention provides a synthesis apparatus system for methylethylamine comprising an acetamide formate preparation unit, a reduction unit, a filtration unit, and a rectification unit; The preparation unit of the formic acid acetamide comprises an ethylamine supply device, a methyl formate supply device, a first reaction device and a formic acid acetamide storage device, wherein the discharge ports of the methyl formate supply device and the ethylamine supply device are respectively connected with the feed inlet of the first reaction device; The reducing unit comprises a reducing agent supply device, an acid liquid supply device, an organic solvent supply device and a second reaction device, wherein the discharge port of the formate-acetamide storage device is connected with the feed port of the second reaction device; The filtering unit comprises a reaction liquid storage device, an alkali liquor supply device, a filtering device and a filtrate storage device, wherein a discharge hole of the second reaction device and a discharge hole of the alkali liquor supply device are respectively connected with a feed hole of the reaction liquid storage device; The rectification unit comprises a first rectification device, a second rectification device, a methyl ethylamine storage tank, a rectification liquid storage tank, a waste liquid st