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CN111039811A - Process for preparing nonane diacyl amino acid salt - Google Patents

Process for preparing nonane diacyl amino acid salt Download PDF

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Publication number
CN111039811A
CN111039811A CN201911336658.9A CN201911336658A CN111039811A CN 111039811 A CN111039811 A CN 111039811A CN 201911336658 A CN201911336658 A CN 201911336658A CN 111039811 A CN111039811 A CN 111039811A
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azelaic acid
reaction
acid salt
amino acid
producing
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范有君
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Sichuan Xinmeijia Biomedicine Co ltd
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C231/00Preparation of carboxylic acid amides
    • C07C231/02Preparation of carboxylic acid amides from carboxylic acids or from esters, anhydrides, or halides thereof by reaction with ammonia or amines
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C51/00Preparation of carboxylic acids or their salts, halides or anhydrides
    • C07C51/58Preparation of carboxylic acid halides
    • C07C51/60Preparation of carboxylic acid halides by conversion of carboxylic acids or their anhydrides or esters, lactones, salts into halides with the same carboxylic acid part

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Abstract

The invention relates to the technical field of preparation of azelaic acid salt, in particular to a preparation method of azelaic acid salt. The preparation method of the azelaic acid salt comprises the steps of reacting azelaic acid compound with amino acid in a protic solvent, and adjusting the pH of a reaction mixed solution formed by the reaction to 1-3 after the reaction is finished. The method not only improves the conversion rate of raw materials, but also improves the purity of the yield of the final product, and simultaneously, the method also saves the production cost, simplifies the operation steps and reduces the energy consumption.

Description

Process for preparing nonane diacyl amino acid salt
Technical Field
The invention relates to the technical field of preparation of azelaic acid salt, in particular to a preparation method of azelaic acid salt.
Background
Azelaic acid is a raw material for whitening and removing acnes, but is greatly limited in application due to water insolubility, high melting point, large using amount, easy color change and poor compatibility. Therefore, a azelaic acid salt has been developed to reduce the amount of use thereof and to ensure a better whitening effect, for example, potassium azelaic acid diglycolate, which is a newly developed azelaic acid derivative, is soluble in water, is used in a small amount, has a good effect of regulating oil secretion, and has a stronger whitening effect. However, the method for preparing the azelaic acid salt in the prior art has many problems, such as high energy consumption, low raw material conversion rate, large pollution, dark product color, complex reaction process, high cost, difficult refining and the like.
In view of this, the invention is particularly proposed.
Disclosure of Invention
The invention aims to provide a preparation method of a azelaic acid salt. The method has the advantages of high product yield and purity, simple operation and low cost.
The invention is realized by the following steps:
in a first aspect, embodiments provide a method for preparing a azelaic acid salt, comprising reacting a azelaic acid compound with an amino acid in a protic solvent to form a azelaic acid salt, and adjusting the pH of a reaction mixture formed by the reaction to 1-3 after the reaction is completed.
In an alternative embodiment, the reaction comprises: dissolving the amino acid in a protic solvent, adjusting the pH value to 11-14, and then adding the azelaic acid compound for reaction, wherein the reaction time is preferably 2-3 hours.
In an alternative embodiment, the reaction comprises: dissolving the amino acid in a protic solvent and then adjusting the pH to 11-14 using an alkali metal hydroxide;
then reducing the temperature of the solution to below 15 ℃, and then dropwise adding the azelaic acid compound and the alkali metal hydroxide to keep the pH of the reaction system at 11-14;
after the dropwise addition of the azelaic acid compound is completed, the temperature of the solution is raised to 18-25 ℃, and the reaction is carried out for 2-3 hours.
In an alternative embodiment, the alkali metal hydroxide is added in the form of an aqueous alkali metal hydroxide solution; preferably, the mass concentration of the aqueous alkali metal hydroxide solution is less than 40%, preferably 20-30%;
preferably, the alkali metal hydroxide is sodium hydroxide or potassium hydroxide.
In an alternative embodiment, the mass ratio of the azelaic acid compound to the amino acid is 1: 0.7-0.9.
In alternative embodiments, the azelaic acid based compound comprises a azelaic acid halide compound; preferably azelaic acid dichloride;
preferably, the amino acid is a natural amino acid, preferably a water-soluble natural amino acid, more preferably glycine;
preferably, the protic solvent is water.
In alternative embodiments, the method of making further comprises making the azelaic acid compound;
preferably, the step of preparing the azelaic acid compound comprises: carrying out acylation reaction on azelaic acid and an acylation reagent;
preferably, the conditions of the acylation reaction are: the reaction temperature is 18-25 ℃, the reaction time is 10-15 hours, and the mass ratio of the azelaic acid to the acylating reagent is 1: 0.6-0.9;
preferably, the acylating agent is a halogen element-containing acylating agent, preferably thionyl chloride.
In an alternative embodiment, the pH of the reaction mixture is adjusted to 1-2.
In an alternative embodiment, the method of making further comprises: carrying out post-treatment on the reaction mixed liquid after the pH value is adjusted;
preferably, the post-treatment comprises performing solid-liquid separation on the reaction mixed solution after the pH is adjusted to obtain a crude product, and then washing the crude product.
In an alternative embodiment, the method of making further comprises: refining the crude product;
preferably, the refining comprises: decolorizing and crystallizing the crude product;
preferably, the refining comprises: mixing the crude product with water at 75-85 ℃ to dissolve the crude product, adding active carbon, uniformly stirring for 30-60 minutes, filtering while hot, and cooling the filtrate to form a refined product of the azelaic acid salt.
The invention has the following beneficial effects: according to the invention, the amino acid and the azelaic acid compound are reacted in the protic solvent, and the pH of the reaction mixed solution formed after the reaction is adjusted to 1-3, so that the conversion rate of the raw materials is improved, the purity of the yield of the final product is improved, meanwhile, the production cost is saved, the operation steps are simplified, and the energy consumption is reduced.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below. The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer. The reagents or instruments used are not indicated by the manufacturer, and are all conventional products available commercially.
The features and properties of the present invention are described in further detail below with reference to examples.
The embodiment of the invention provides a preparation method of a azelaic acid salt, which comprises the following steps:
s1, preparing a azelaic acid compound;
carrying out acylation reaction on azelaic acid and an acylation reagent, wherein the conditions of the acylation reaction are as follows: the reaction temperature may be 18 to 25 ℃, for example, any one of 18 ℃, 19 ℃, 20 ℃, 21 ℃, 22 ℃, 23 ℃, 24 ℃ and 25 ℃ or a range of any two values may be selected; the reaction time may be 10 to 15 hours, for example, any one of 10 hours, 11 hours, 12 hours, 13 hours, 14 hours and 15 hours, or a range of any two of them may be selected; the mass ratio of the azelaic acid to the acylating reagent is 1: 0.6-0.9; for example, the mass ratio may be 1:0.6, 1:0.65, 1:0.7,1:0.75,1:0.8,1:0.85,1: any one of the values of 0.9, or a range of values formed by any two of the values; the reaction can be ensured to be carried out smoothly by adopting the conditions. Preferably, the acylating agent is a halogen element-containing acylating agent, preferably thionyl chloride.
Specifically, when the acylating reagent is thionyl chloride, the vacuum degree in the reaction vessel can be adjusted, and then the thionyl chloride is recovered, so that resources are saved, the production cost is reduced, and the environmental pollution caused by the thionyl chloride is avoided. The vacuum degree is more than or equal to 0.08MPa, and the temperature depends on the source of the raw materials.
S2, synthesizing a azelaic acid amino acid salt;
first, a azelaic acid compound is reacted with an amino acid in a protic solvent to form a azelaic acid salt. The adoption of the protic solvent can not only promote the reaction, but also reduce the production cost.
Specifically, the amino acid is dissolved in a protic solvent, the pH is adjusted to 11-14, and then the azelaic acid compound is added for reaction, preferably, the reaction time is 2-3 hours. The pH can be any one value of 11, 11.5, 12, 12.5, 13, 13.5 and 14, or a range of any two values; the reaction time may be any one of 2 hours, 2.5 hours, and 3 hours, or a range of any two values. By adopting the steps and the conditions, the yield of the product can be ensured, the formed product has less impurities and is easier to refine, the difficulty of subsequent purification is simplified, and the purity of the product is favorably improved.
More specifically, the amino acid is dissolved in a protic solvent, and then the pH is adjusted to 11 to 14 using an alkali metal hydroxide; then reducing the temperature of the solution to below 15 ℃, and then dropwise adding the azelaic acid compound and the alkali metal hydroxide to keep the pH of the reaction system at 11-14; after the dropwise addition of the azelaic acid compound is completed, the temperature of the solution is raised to 18-25 ℃, and the reaction is carried out for 2-3 hours. The temperature in the process of dropwise adding the azelaic acid compound is lower than the reaction temperature, so that the decomposition of the azelaic acid compound caused by high temperature is avoided, and then the reaction is promoted by properly heating, but the heating temperature is not too high, so that the decomposition of the azelaic acid compound is avoided, and the yield of the product is further ensured. Meanwhile, alkali metal hydroxide is added in the process of dropwise adding the azelaic acid compound, so that the pH value of a reaction system is not changed, and the subsequent reaction is smoothly carried out. The alkali metal hydroxide added twice is the same alkali metal hydroxide, and the formation of impurities is reduced.
Further, the alkali metal hydroxide is added in the form of an aqueous alkali metal hydroxide solution; preferably, the mass concentration of the aqueous alkali metal hydroxide solution is less than 40%, preferably 20-30%; the addition of the alkali metal hydroxide aqueous solution is more beneficial to controlling the pH of a reaction system, ensuring the smooth reaction and reducing the formation of impurities, and the alkali metal hydroxide with the mass concentration of less than 40 percent is adopted, so that the purity and the yield of the product can be further improved, and the formation of impurities is reduced.
Further, the alkali metal hydroxide is sodium hydroxide or potassium hydroxide. The azelaic acid compound comprises azelaic acid halide compound; preferably azelaic acid dichloride; preferably, the amino acid is a natural amino acid, preferably a water-soluble natural amino acid, more preferably glycine; preferably, the protic solvent is water. By adopting the raw materials, the formation of impurities can be further reduced, the conversion rate of the raw materials is improved, the purity and the yield of the product are improved, particularly when the protic solvent selects water, the reaction is promoted, and the production cost can be saved.
Although the examples of the present invention provide examples in which the amino acid is glycine, it is understood that natural water-soluble amino acids such as alanine, proline, arginine, and serine that can react with azelaic acid compound are also within the scope of the present invention.
Further, after the completion of the reaction, the pH of the reaction mixture formed by the reaction is adjusted to 1 to 3, preferably 1 to 2. For example, the pH of the reaction mixture may be any one of 1, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, 2, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, 2.7, 2.8, 2.9, and 3, or a range of any two thereof. In the prior art, the pH of a reaction mixed solution is basically adjusted to be neutral or close to neutral, and the inventors unexpectedly found that after the pH is adjusted to be acidic, particularly 1-3, the yield of the product is greatly improved, impurities in the product are less, and the purity of the product is higher.
Specifically, the pH of the reaction mixture is adjusted by concentrated hydrochloric acid, and after 1 to 1.5 hours, the temperature is reduced to about 15 ℃. The pH value is adjusted and then kept for 1 to 1.5 hours, which is beneficial to the precipitation of the product, improves the yield of the product, and then reduces the temperature to further promote the precipitation of the product. It should be noted that the concentrated hydrochloric acid used in the examples of the present invention is hydrochloric acid having a mass fraction of more than 20%.
Then carrying out post-treatment on the reaction mixed liquid after the pH value is adjusted; specifically, the post-treatment comprises the steps of carrying out solid-liquid separation on the reaction mixed solution after the pH is adjusted to obtain a crude product, washing the crude product until the pH is 3-4, washing to remove unreacted reactants or residual other impurities dissolved in the protic solvent from the crude product, and then improving the purity of the crude product.
And then the crude product is refined, so that impurities in the crude product are reduced, the color of the crude product is reduced, the purity, the color and the like of the product are improved, and the quality of the product is improved.
Specifically, the refining includes: decolorizing and crystallizing the crude product; preferably, the refining comprises: mixing the crude product with water at 75-85 ℃ to dissolve the crude product, adding active carbon, uniformly stirring for 30-60 minutes, filtering while hot, and cooling the filtrate to form a refined product of the azelaic acid salt. The refining by the method can effectively reduce the content of impurities in the finished product, improve the color and the glossiness of the finished product and further improve the quality of the finished product.
Example 1
This example provides a method for preparing potassium nonanoylglycine salt, comprising:
s1, synthesizing azelaic acid dichloride;
synthesis of Nonoyl dichloride with reference to the following formula
Figure BDA0002331139390000071
Specifically, stirring is started, thionyl chloride is added into a reaction kettle, then azelaic acid is added, the temperature in the reaction kettle is controlled to be 20 ℃, and the reaction is completed after heat preservation is carried out for 12 hours. And (3) recovering excessive thionyl chloride in vacuum until the vacuum degree is more than or equal to 0.08MPa, wherein the mass ratio of azelaic acid to thionyl chloride is 1: 0.6.
s2, synthesizing potassium nonanoylglycine;
synthesizing potassium nonanoylglycine according to the following formula;
Figure BDA0002331139390000081
h is to be255kg of O (distilled water) and 4.2kg of glycine are put into a reaction kettle, the stirring is started, and then the reaction kettle is usedKOH with a mass concentration of 30%(aq)Adjusting the pH value of the reaction liquid in the kettle to 11, then utilizing brine to reduce the temperature of the reaction liquid to 15 ℃, then beginning to dropwise add the azelaic acid dichloride and simultaneously adding 30 percent KOH(aq)The pH of the reaction liquid in the kettle is ensured to be 11, and the temperature is controlled not to exceed 15 ℃ in the feeding process. After the addition was complete, the reaction solution was warmed to 20 ℃ and held for 2.5 h. After the reaction is finished, the pH value of the reaction mixed solution is adjusted to 2 by using concentrated hydrochloric acid, the temperature of the reaction mixed solution is reduced to about 15 ℃ after 1 hour, then solid-liquid separation is carried out by using a three-legged centrifuge, and then washing is carried out for 2 times by using distilled water until the pH value is 3, so as to obtain a crude product.
Next, the crude product was reacted with 20kgH2Mixing O (distilled water) at 80 ℃, adding activated carbon, keeping the temperature, stirring for 30 minutes, filtering while the mixture is hot, cooling the filtrate to about 15 ℃, performing solid-liquid separation by using a three-legged centrifuge to obtain a wet refined product, and drying to obtain a finished product of the potassium nonanedioyl glycinate, wherein the conversion rate is as follows: 95 percent; the yield was 93% and the purity was 99.3% (melting point. + -. 170 ℃ C.).
Example 2
This example provides a method for preparing azelaic acid sodium salt, comprising:
synthesis of Nonoyl dichloride Using the Synthesis of example 1 to obtain Nonoyl Glycine sodium salt, specifically, H255kg of O (distilled water) and 4.8kg of glycine are put into a reaction kettle, the stirring is started, and then NaOH with the mass concentration of 20 percent is used(aq)Adjusting the pH value of the reaction liquid in the kettle to 12, then utilizing brine to reduce the temperature of the reaction liquid to 10 ℃, then beginning to dropwise add the azelaic acid dichloride, and simultaneously adding 20 percent NaOH(aq)The pH of the reaction liquid in the kettle is ensured to be 12, and the temperature is controlled not to exceed 15 ℃ in the feeding process. After the addition was complete, the reaction solution was warmed to 25 ℃ and held for 2 h. After the reaction is finished, the pH value of the reaction mixed solution is adjusted to 3 by using concentrated hydrochloric acid, the temperature of the reaction mixed solution is reduced to about 15 ℃ after 1.5h, then solid-liquid separation is carried out by using a three-legged centrifuge, and then washing is carried out for 3 times by using distilled water until the pH value is 4, so as to obtain a crude product.
Next, the crude product was reacted with 20kgH2O (distilled water) at 75 deg.CMixing, adding active carbon, keeping the temperature, stirring for 60 minutes, filtering while the mixture is hot, cooling the filtrate to about 15 ℃, performing solid-liquid separation by using a three-legged centrifuge to obtain a wet refined product, and drying to obtain a finished product of the potassium nonanedioyl glycinate with the yield of 94% and the purity of 99.5% (the melting point is +/-170 ℃).
Example 3
This example provides a method for preparing potassium nonanoylglycine salt, comprising:
synthesis of Nonoyl dichloride Using the Synthesis of example 1 to obtain Nonoyl Glycine sodium salt, specifically, H255kg of O (distilled water) and 5.4kg of glycine are put into a reaction kettle, the stirring is started, and then KOH with the mass concentration of 25 percent is used(aq)Adjusting the pH value of the reaction liquid in the kettle to 13-14, then utilizing brine to reduce the temperature of the reaction liquid to 5 ℃, then beginning to dropwise add the azelaic acid dichloride, and simultaneously adding 25 percent KOH(aq)The pH of the reaction liquid in the kettle is ensured to be 14, and the temperature is controlled not to exceed 15 ℃ in the feeding process. After the addition was complete, the reaction solution was warmed to 18 ℃ and held for 3 h. After the reaction is finished, the pH value of the reaction mixed solution is adjusted to 1 by using concentrated hydrochloric acid, the temperature of the reaction mixed solution is reduced to about 15 ℃ after 1.2h, then solid-liquid separation is carried out by using a three-legged centrifuge, and then washing is carried out for 3 times by using distilled water until the pH value is 3.5, so as to obtain a crude product.
Next, the crude product was reacted with 20kgH2Mixing O (distilled water) at 85 ℃, adding active carbon, keeping the temperature, stirring for 45 minutes, filtering while hot, cooling the filtrate to about 15 ℃, performing solid-liquid separation by using a three-foot centrifuge to obtain a wet refined product, and drying to obtain the finished product of the nonanedioyl glycine potassium salt, wherein the yield is 93.5%, and the purity is 99.6% (melting point +/-170 ℃).
Example 4-example 5
Example 4-example 5 azelaic acid compounds were synthesized following the procedure provided in example 1, except that example 4: the mass ratio of the azelaic acid to the thionyl chloride is 1: 0.9, the reaction temperature is 18 ℃, and the reaction time is 15 hours; example 5: the mass ratio of the azelaic acid to the thionyl chloride is 1:0.7, the reaction temperature is 225 ℃, and the reaction time is 10 hours.
Example 6-example 7
Examples 6-7 potassium nonanoylamino acid was synthesized according to the procedure provided in example 1, except that the amino acid of example 6 was lysine and the amino acid of example 7 was serine.
Comparative example 1: potassium azeloylglycine was synthesized following the procedure provided in example 1, with the exception that: after the reaction, the pH of the reaction mixture was adjusted to 7, and the product yield was 85.5% and the purity was 90.8%.
Comparative example 2: potassium azeloylglycine was synthesized following the procedure provided in example 1, with the exception that: the reaction solvent is diethyl ether, the yield of the product is 80.5%, and the purity is 89.5%.
In conclusion, the azelaic acid compound and the amino acid are reacted in the protic solvent to generate the azelaic acid salt, the pH of the reaction mixed solution formed by the reaction is adjusted to 1-3 after the reaction is finished, the yield and the purity of the product can be improved, the yield can basically reach more than 90 percent, the purity can also reach more than 99 percent, and the production cost can be reduced.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (10)

1. A preparation method of a azelaic acid salt is characterized in that a azelaic acid compound and amino acid react in a protic solvent to generate the azelaic acid salt, and the pH of a reaction mixed solution formed by the reaction is adjusted to 1-3 after the reaction is finished.
2. The method for producing a azelaic acid salt according to claim 1, wherein the reaction comprises: dissolving the amino acid in a protic solvent, adjusting the pH value to 11-14, and then adding the azelaic acid compound for reaction, wherein the reaction time is preferably 2-3 hours.
3. The method for producing a azelaic acid salt according to claim 1, wherein the reaction comprises: dissolving the amino acid in a protic solvent and then adjusting the pH to 11-14 using an alkali metal hydroxide;
then reducing the temperature of the solution to below 15 ℃, and then dropwise adding the azelaic acid compound and the alkali metal hydroxide to keep the pH of the reaction system at 11-14;
after the dropwise addition of the azelaic acid compound is completed, the temperature of the solution is raised to 18-25 ℃, and the reaction is carried out for 2-3 hours.
4. The method for producing a azelaic acid salt according to claim 3, wherein the alkali metal hydroxide is added in the form of an aqueous alkali metal hydroxide solution; preferably, the mass concentration of the aqueous alkali metal hydroxide solution is less than 40%, preferably 20-30%;
preferably, the alkali metal hydroxide is sodium hydroxide or potassium hydroxide.
5. The method for producing a azelaic acid salt according to claim 1,
the mass ratio of the azelaic acid compound to the amino acid is 1: 0.7-0.9.
6. The method for producing a azelaic acid salt according to any one of claims 1 to 5, wherein the azelaic acid compound comprises a azelaic acid halide compound; preferably azelaic acid dichloride;
preferably, the amino acid is a natural amino acid, preferably a water-soluble natural amino acid, more preferably glycine;
preferably, the protic solvent is water.
7. The method of producing a azelaic acid salt according to claim 6, further comprising producing the azelaic acid compound;
preferably, the step of preparing the azelaic acid compound comprises: carrying out acylation reaction on azelaic acid and an acylation reagent;
preferably, the conditions of the acylation reaction are: the reaction temperature is 18-25 ℃, the reaction time is 10-15 hours, and the mass ratio of the azelaic acid to the acylating reagent is 1: 0.6-0.9;
preferably, the acylating agent is a halogen element-containing acylating agent, preferably thionyl chloride.
8. The method for producing a azelaic acid salt according to any one of claims 1 to 5, wherein the pH of the reaction mixture is adjusted to 1 to 2.
9. The method for producing a azelaic acid salt according to any one of claims 1-5, wherein the method further comprises: carrying out post-treatment on the reaction mixed liquid after the pH value is adjusted;
preferably, the post-treatment comprises performing solid-liquid separation on the reaction mixed solution after the pH is adjusted to obtain a crude product, and then washing the crude product.
10. The method of claim 9, further comprising: refining the crude product;
preferably, the refining comprises: decolorizing and crystallizing the crude product;
preferably, the refining comprises: mixing the crude product with water at 75-85 ℃ to dissolve the crude product, adding active carbon, uniformly stirring for 30-60 minutes, filtering while hot, and cooling the filtrate to form a refined product of the azelaic acid salt.
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CN117105798A (en) * 2023-08-10 2023-11-24 妆莱(广州)生物研究有限公司 A kind of preparation method of azelaic acid amide MEA

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Application publication date: 20200421