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CN120058866A - Method for recovering cyclosporine A crystallization mother liquor - Google Patents

Method for recovering cyclosporine A crystallization mother liquor Download PDF

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Publication number
CN120058866A
CN120058866A CN202311613655.1A CN202311613655A CN120058866A CN 120058866 A CN120058866 A CN 120058866A CN 202311613655 A CN202311613655 A CN 202311613655A CN 120058866 A CN120058866 A CN 120058866A
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crystallization
cyclosporine
cyclosporin
mother liquor
temperature
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赵军杰
罗佳乐
杨丰
海文智
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Ningxia Taisheng Biotechnology Co ltd
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Ningxia Taisheng Biotechnology Co ltd
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07KPEPTIDES
    • C07K7/00Peptides having 5 to 20 amino acids in a fully defined sequence; Derivatives thereof
    • C07K7/64Cyclic peptides containing only normal peptide links
    • C07K7/645Cyclosporins; Related peptides

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Abstract

The invention relates to a method for recovering cyclosporine A crystallization mother liquor, which comprises the steps of removing impurities from cyclosporine A crystallization mother liquor by previous treatment, crystallizing by a polar solvent for the first time and crystallizing by a nonpolar solvent for the second time, and finally performing crystal transformation and drying by the polar solvent to obtain a cyclosporine A finished product. The invention effectively purifies the residual cyclosporine A in the crystallization mother liquor, avoids the waste of the residual cyclosporine A in the crystallization mother liquor, can obviously reduce the production cost of the cyclosporine A, is suitable for industrial production, and has the product content of more than 98.5 percent and the maximum single impurity content of less than 0.7 percent.

Description

Method for recovering cyclosporine A crystallization mother liquor
Technical Field
The invention belongs to the technical field of biological medicines, and particularly relates to a method for recovering cyclosporine A crystallization mother liquor.
Background
Cyclosporin A is a cyclic polypeptide containing 11 amino acids isolated from a culture of Beauveria bassiana (Beauveria bassiana), and is an immunosuppressant having a strong action, and has more than 20 homologs such as B, C, D in addition to cyclosporin A. Cyclosporin a is used for immunosuppressive treatment of transplantation operations of kidney, liver and heart, and can also be used for treating a variety of autoimmune diseases such as lupus erythematosus, rheumatoid arthritis, idiopathic thrombocytopenic purpura, ulcerative colitis, myasthenia gravis, chronic nephritis, chronic active hepatitis and nephrotic syndrome, and the cyclosporin a has the following information:
Chinese name cyclosporine A, cyclosporine A
English name of Ciclosporin A
CAS registry number 59865-13-3
The chemical structural formula of cyclosporin A is as follows:
The main impurities in the cyclosporin A fermentation product are cyclosporin A homologs with similar structures, including B, C, D and the like, and the main process route for extracting and purifying the cyclosporin A in the prior art is to extract the cyclosporin A by using an organic solvent, and then separate and purify the cyclosporin A homologs by using different types of column chromatography. The initial content of the cyclosporin A intermediate obtained by a fermentation method is only about 15%, and the crude cyclosporin A product is obtained by extraction, purification, macroporous adsorption resin chromatography and silica gel column chromatography in the later period. The crude cyclosporine A is recrystallized or prepared by liquid phase technology, and finally the pharmaceutical standard cyclosporine A can be obtained. Whether recrystallization or high performance liquid chromatography technology, a certain amount of mother liquor is generated in the processes of refining, purifying and crystal transformation of cyclosporine A, the content of the mother liquor is usually 35% -80%, the maximum single impurity is 1% -3%, and the yield is 10% -40% of the total product. How to fully utilize the mother liquor, improve the product yield and reduce the production cost becomes a problem to be solved urgently for each production enterprise.
Patent US597638 discloses a method for obtaining cyclosporin a by silica gel column chromatography by using high-pressure carbon dioxide as a flow carrier, but the method has high requirements on equipment, has small sample processing capacity, and cannot realize large-scale production.
Patent US2002/0162789A1 discloses a multi-step silica gel chromatographic separation of toluene and ethyl acetate as mobile phases, which has the main disadvantages of high toluene toxicity, multiple chromatographic steps and high solvent consumption.
WO01/64935A1 describes a process for the isolation and purification of cyclosporin A using organic solvent extraction, gel filtration and silica gel column chromatography, which has the major disadvantages of expensive gel filtration packing and the need to remove the solvent from the previous step between the various steps, which is labor intensive and solvent consuming.
WO20010064935 discloses that after the fermentation broth is extracted with methanol, alum is added into the concentrated solution and stirred for 3 hours, the mixture is filtered, the filter cake is dissolved with cyclohexane, and after concentration, a crude cyclosporin a product with the purity of 59.8% is obtained, and then the crude cyclosporin a product is obtained through gel filtration, column chromatography and crystallization purification.
The above patent documents have studied on the separation and purification of cyclosporin a, but none of the above technical solutions relates to the recovery of residual cyclosporin a in a secondary crystallization mother liquor. Therefore, there is a need to develop an effective method for recovering cyclosporine a crystallization mother liquor, which will greatly reduce the production cost of cyclosporine a, and simultaneously reduce the waste and environmental pollution in the production process.
Disclosure of Invention
The invention aims to provide a method for recycling cyclosporine A crystallization mother liquor, which solves the technical problem of waste of residual cyclosporine A in the cyclosporine A crystallization mother liquor by carrying out previous treatment and impurity removal on the cyclosporine A crystallization mother liquor and combining a twice crystallization method and a crystal transformation method, effectively purifies the residual cyclosporine A in the crystallization mother liquor and obviously reduces the production cost of the cyclosporine A.
The technical scheme adopted to realize the aim of the invention is as follows:
1. A method for recovering cyclosporin a crystallization mother liquor, comprising the steps of:
1) Removing solvent from cyclosporine A crystallization mother liquor, adding acetonitrile for dissolution, and carrying out solid-liquid separation to obtain filtrate;
2) Decolorizing the filtrate obtained in the step 1) by using active carbon to obtain decolorized solution;
3) Recovering the solvent from the decolorized solution obtained in the step 2), adding a polar solvent for primary crystallization, and carrying out solid-liquid separation to obtain a crystal I;
4) Adding nonpolar solvent into the crystal I obtained in the step 3) for secondary crystallization, and carrying out solid-liquid separation to obtain crystal II;
5) And (3) adding a polar solvent into the crystal II obtained in the step (4) to perform crystal transformation, performing solid-liquid separation, and performing vacuum drying to obtain a cyclosporine A finished product.
Wherein the ratio of the addition volume of acetonitrile to the amount of the product in the mother liquor in the step 1) is 10-20:1 (w/v).
Wherein the decolorizing temperature of the activated carbon in the step 2) is 40-50 ℃, and the adding amount of the activated carbon is 1-3% (w/w) of the weight of the cyclosporine A.
Wherein, the recycling solvent in the step 3) is decompressed and concentrated under the conditions that the temperature is 50 ℃ to 60 ℃ and the vacuum degree is minus 0.09 to minus 0.1 Mpa.
Wherein, the step 3) further comprises adding purified water with 15-20% of the volume of the crystallization system before one crystallization.
Wherein, the primary crystallization condition in the step 3) is that the crystallization temperature is-5 ℃ to 0 ℃, the crystallization heat preservation time is 2 hours, and the filtration temperature is-15 ℃ to-10 ℃.
The nonpolar solvent in the step 4) is at least one of ethyl acetate, hexane and petroleum ether, and the addition amount of the nonpolar solvent is 10-50 times (w/v) of the product amount.
Wherein, the secondary crystallization condition in the step 4) is that the crystallization temperature is-10 ℃ to-5 ℃ during purification, the crystallization heat preservation time is 2 hours, and the filtration temperature is-20 ℃ to-15 ℃.
The crystallization condition in the step 5) is that the concentration of cyclosporine A is 2% -5%, the crystallization temperature during purification is-5 ℃ to 0 ℃, the heat preservation time is 2 hours, and the filtration temperature is-10 ℃ to-5 ℃.
Wherein, the drying condition in the step 5) is that the temperature is 40-70 ℃, the vacuum degree is-0.09 MPa to-0.1 MPa, and the drying time is 40h.
Wherein the polar solvent in the step 3) and the step 5) is at least one of ethanol, methanol and acetone, and the polar solvent is 10-50 times (w/v) of the product amount.
The technical scheme of the invention has at least the following beneficial technical effects:
1. The method for recovering the cyclosporine A crystallization mother liquor has the advantages of short process route, less investment, recoverable and reusable solvent, improved cyclosporine A yield and obviously reduced cyclosporine A production cost.
2. The process of the invention effectively purifies the residual cyclosporine A in the crystallization mother liquor, avoids the waste of the residual cyclosporine A in the crystallization mother liquor, can obviously reduce the production cost of the cyclosporine A, is suitable for industrial production, and has the product content of more than 98.5 percent and the maximum single impurity content of less than 0.7 percent.
Detailed Description
Embodiments of the present invention will now be described more fully hereinafter with reference to the accompanying examples, in which it is shown, however, that the examples are shown, and in which the invention is practiced. The following description of at least one exemplary embodiment is merely exemplary in nature and is in no way intended to limit the invention, its application, or uses. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The cyclosporine A crystallization mother liquor can be mother liquor obtained by primary crystallization treatment of cyclosporine A fermentation liquor, mother liquor obtained by secondary crystallization and tertiary crystallization or mixed liquor thereof. Such crystallization treatment may be a method generally employed in the art.
The HPLC detection method of the following example and comparative example comprises the steps of using octadecylsilane chemically bonded silica as a filler (stainless steel tube with phi 0.25mm multiplied by 1000mm is connected in front of the column), acetonitrile-water-tert-butyl methyl ether-phosphoric acid (430:520:50:1) as a mobile phase, the temperature of the stainless steel tube and the column is 70 ℃, the detection wavelength is 210nm, and the sample injection volume is 20 mu l. Calculated by a peak area normalization method.
Example 1
Taking 500L (concentration 2.1 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 2.8kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 38 percent, and the maximum single impurity is 2.0 percent. 45L of acetonitrile was added to the concentrate, the mixture was stirred to dissolve the product completely, the solution was stirred for 2 hours at-15℃and filtered. To the filtrate, 80g of activated carbon was added, and the mixture was heated to 45℃with stirring, decolorized for 1 hour, and filtered. Concentrating the filtrate to dryness at 55 deg.C-0.09 Mpa, adding 40L acetone into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear transparent solution. And (3) performing acetone crystallization, adding purified water accounting for 15% of the volume of a crystallization system into the system at 5 ℃, crystallizing at 0 ℃ and preserving heat for 2 hours, filtering at-15 ℃, and collecting crystals. After cyclosporin A crystals were completely dissolved by heating with a mixture of 20L of ethyl acetate and n-hexane (80:20) to 40 ℃, recrystallization was performed, crystallization was started at-3 ℃, and the temperature was kept for 2h at-20 ℃, and the crystals were collected by filtration. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at 0 ℃ for 2h, filtering at-10 ℃, collecting crystals, and drying at 70 ℃ and vacuum degree of-0.09 MPa to-0.1 MPa for 40h to obtain 380g of cyclosporine A product with the yield of 36.2%. The experiment is carried out once by refining acetone, crystallizing ethyl acetate-n-hexane mixed solution once, and carrying out acetone crystal transformation to obtain the cyclosporin A with the maximum single impurity content of 0.52% and the content of 98.9% meeting the medicinal standard.
Example 2
Taking 500L (concentration 1.6 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.15kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 70 percent, and the maximum single impurity is 1.9 percent. To the concentrate was added 25L of acetonitrile, stirred to dissolve the product completely, the solution was left to stand at-15℃for 2h with stirring, and filtered. 100g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 60 deg.C-0.09 Mpa, adding 40L ethanol into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear and transparent solution. Ethanol crystallization is carried out, 8L of purified water with the volume of 20% of the crystallization system is added into the system at the temperature of 5 ℃, crystallization and heat preservation are carried out for 2 hours at the temperature of 0 ℃, filtration is carried out at the temperature of minus 15 ℃, and crystals are collected. After cyclosporin A crystals were completely dissolved by heating with a mixture of 20L of ethyl acetate and petroleum ether (80:20) to 40 ℃, recrystallization was performed, crystallization was started at-5 ℃, and the temperature was kept for 2h at-18 ℃, and the crystals were collected by filtration. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at-2 ℃ for 2h at-10 ℃ for filtering, collecting crystals, and drying at-70 ℃ under the vacuum degree of-0.09 MPa to-0.1 MPa for 40h to obtain 336g of cyclosporine A product with the yield of 42.0%. The experiment is carried out once by refining ethanol, crystallizing ethyl acetate petroleum ether mixed solution once, and carrying out acetone crystal transformation to obtain the cyclosporin A with the maximum single impurity content of 0.60 percent and the content of 98.6 percent, which accords with the medicinal standard.
Example 3
Taking 500L (concentration 1.8 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.15kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 78 percent, and the maximum single impurity is 1.5 percent. To the concentrate was added 21L of acetonitrile, stirred to dissolve the product completely, the solution was left to stand at-20℃for 2 hours with stirring, and filtered. 100g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 55 deg.C-0.09 Mpa, adding 40L acetone into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear transparent solution. And (3) performing acetone crystallization, adding purified water accounting for 15% of the volume of the crystallization system into the system at 3 ℃, crystallizing at-1 ℃ for 2 hours, filtering at-15 ℃, and collecting crystals. After cyclosporin A crystals were completely dissolved by heating with a mixture of 20L of ethyl acetate and n-hexane (80:20) to 40 ℃, recrystallization was performed, crystallization was started at-2 ℃, the temperature was kept for 2h, and the crystals were collected by filtration at-15 ℃. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at 0 ℃ for 2h, filtering at-10 ℃, collecting crystals, and drying at 70 ℃ and vacuum degree of-0.09 MPa to-0.1 MPa for 40h to obtain 370g of cyclosporine A product with the yield of 41.1%. The experiment is carried out once for refining acetone, ethyl acetate is crystallized once for n-hexane, and the maximum single impurity of 0.55 percent can be obtained after acetone is transferred to crystal, and the content of cyclosporin A which accords with the medicinal standard is 98.7 percent.
Example 4
Taking 500L (concentration 2.0 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.8kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 58 percent, and the maximum single impurity is 1.8 percent. 36L of acetonitrile was added to the concentrate, the mixture was stirred to dissolve the product completely, the solution was stirred at-15℃for 2 hours, and filtered. 72g of active carbon was added to the filtrate, heated to 45℃with stirring, decolorized for 1h, and filtered. Concentrating the filtrate to dryness at 55 deg.C-0.09 Mpa, adding 40L ethanol into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear and transparent solution. Ethanol crystallization is carried out, purified water accounting for 15 percent of the volume of the crystallization system is added into the system for 6L at 5 ℃, crystallization and heat preservation are carried out for 2 hours at 0 ℃, filtration is carried out at-15 ℃, and crystals are collected. After the cyclosporine A crystals were completely dissolved by heating with 20L petroleum ether to 40 ℃, recrystallization was performed, crystallization was started at 10 ℃, heat preservation was performed for 2h, -10 ℃ filtration, and crystals were collected. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at 0 ℃ for 2h, filtering at-10 ℃, collecting crystals, performing vacuum degree of-0.09 MPa to-0.1 MPa, and drying for 40h to obtain 318g of cyclosporine A product, wherein the yield is 31.8%. The experiment shows that once acetone is refined, petroleum ether is crystallized once, and the maximum single impurity of 0.68 percent can be obtained after acetone is subjected to crystal transformation, and the content of cyclosporin A which accords with the medicinal standard is 98.5 percent.
Example 5
Taking 500L (concentration 1.7 g/L) of cyclosporin A acetone mother solution, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.55kg of concentrate, wherein the content of cyclosporin A in the mother solution is about 55% and the maximum single impurity is 1.9%. 31L of acetonitrile was added to the concentrate, the product was completely dissolved by stirring, the solution was left to stand at-15℃for 2 hours with stirring, and filtration was carried out. 90g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 60 deg.C-0.09 Mpa, adding 40L methanol into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear transparent solution. Methanol crystallization is carried out, 8L of purified water with the volume of 20% of the crystallization system is added into the system at the temperature of 5 ℃, crystallization and heat preservation are carried out for 2 hours at the temperature of 0 ℃, filtration is carried out at the temperature of minus 17 ℃, and crystals are collected. After the cyclosporine A crystals were completely dissolved by heating with 20L of n-hexane to 40 ℃, recrystallization was performed, crystallization was started at-5 ℃, the temperature was maintained for 2 hours, filtration was performed at-15 ℃, and the crystals were collected. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at-2 ℃ for 2h at-10 ℃ for filtering, collecting crystals, and drying at-70 ℃ under the vacuum degree of-0.09 MPa to-0.1 MPa for 40h to obtain 256g of cyclosporine A product with the yield of 30.1%. The experiment is carried out once ethanol refining, normal hexane crystallization is carried out once, and acetone crystal transformation can be carried out to obtain the cyclosporin A with the maximum single impurity of 0.69 percent and the content of 98.6 percent, which accords with the medicinal standard.
Example 6
Taking 500L (concentration 1.7 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.25kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 68 percent, and the maximum single impurity is 1.5 percent. To the concentrate was added 25L of acetonitrile, stirred to dissolve the product completely, the solution was left to stand at-20℃for 2h with stirring, and filtered. 50g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 55 deg.C-0.09 Mpa, adding 40L acetone into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear transparent solution. And (3) performing acetone crystallization, adding purified water accounting for 15% of the volume of the crystallization system into the system at 3 ℃, crystallizing at-1 ℃ for 2 hours, filtering at-15 ℃, and collecting crystals. After the cyclosporine A crystals were completely dissolved by heating with 20L of ethyl acetate to 40 ℃, recrystallization was performed, crystallization was started at-10 ℃, the temperature was maintained for 2 hours, filtration was performed at-25 ℃, and the crystals were collected. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at 0 ℃ for 2h, filtering at-10 ℃, collecting crystals, performing vacuum degree of-0.09 MPa to-0.1 MPa, and drying for 40h to obtain 236g of cyclosporine A product, wherein the yield is 27.8%. The experiment is carried out once acetone is refined, ethyl acetate is crystallized once, and the maximum single impurity of 0.58 percent is obtained after acetone is subjected to crystal transformation, and the content of cyclosporin A which accords with the medicinal standard is 98.7 percent.
Comparative example 1
Taking 500L (concentration 1.7 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness under 60 ℃ and minus 0.09Mpa to obtain 1.30kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 69% and the maximum single impurity is 1.5%. 26L of acetonitrile was added to the concentrate, the mixture was stirred to dissolve the product completely, the solution was stirred at-20℃for 2 hours, and filtered. 50g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 55 ℃ and minus 0.09Mpa, adding 20L of ethyl acetate petroleum ether (80:20) mixture into the concentrate, heating to 40 ℃ for complete dissolution, recrystallizing, crystallizing at minus 10 ℃, preserving heat for 2 hours, filtering at minus 25 ℃, and collecting crystals. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at-5 ℃ for 2h, filtering at-15 ℃, collecting crystals, and drying at-70 ℃ under the vacuum degree of-0.09 MPa to-0.1 MPa for 40h to obtain 367g of cyclosporine A product with the yield of 43.2%. The mixed solution of ethyl acetate and petroleum ether is crystallized once in the experiment, and the maximum single impurity of 0.75 percent and the cyclosporin A with the content of 98.0 percent can be obtained through acetone crystal transformation.
Comparative example 2
Taking 500L (concentration 1.6 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.15kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 70 percent, and the maximum single impurity is 1.9 percent. To the concentrate was added 23L acetonitrile, stirred to dissolve the product completely, the solution was left to stand at-15℃for 2h with stirring, and filtered. 60g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 60 deg.C-0.09 Mpa, adding 40L acetone into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear transparent solution. And (3) performing acetone crystallization, adding 8L of purified water accounting for 20% of the volume of a crystallization system into the system at 5 ℃, crystallizing at 0 ℃ and preserving heat for 2 hours, filtering at-15 ℃, and collecting crystals. The cyclosporine A crystals were added to 40L of acetone and stirred at 40℃with heating to dissolve the crystals completely, giving a clear and transparent solution. Performing acetone crystallization, crystallizing at-3 ℃ for 2h at-12 ℃ for filtering, collecting crystals, and drying at-70 ℃ under the vacuum degree of-0.09 MPa to-0.1 MPa for 40h to obtain 348g of cyclosporine A product with the yield of 43.5%. The experiment shows that once acetone is refined, the maximum single impurity of 0.88 percent and the cyclosporin A with 96.6 percent can be obtained through acetone crystal transformation.
Comparative example 3
Taking 500L (concentration 1.7 g/L) of cyclosporin A acetone mother liquor, vacuum concentrating, concentrating to dryness at 60 ℃ and minus 0.09Mpa to obtain 1.25kg of concentrate, wherein the content of cyclosporin A in the mother liquor is about 68 percent, and the maximum single impurity is 1.7 percent. To the concentrate was added 25L of acetonitrile, stirred to dissolve the product completely, the solution was left to stand at-20℃for 2h with stirring, and filtered. 100g of active carbon is added into the filtrate, the mixture is stirred and heated to 45 ℃, decolorized for 1h and filtered. Concentrating the filtrate to dryness at 55 deg.C-0.09 Mpa, adding 40L acetone into the concentrate, heating and stirring at 40 deg.C to dissolve completely to obtain clear transparent solution. And (3) performing acetone crystallization, adding purified water accounting for 15% of the volume of the crystallization system into the system at 3 ℃, crystallizing at-1 ℃ for 2 hours, filtering at-15 ℃, and collecting crystals. Heating the cyclosporine A crystal to 40 ℃ with 20L of ethyl acetate-n-hexane (80:20) mixed solution to be completely dissolved, then recrystallizing, starting crystallization at-2 ℃, preserving heat for 2 hours at-15 ℃, filtering, collecting the crystal at 70 ℃, carrying out vacuum degree of-0.09 MPa to-0.1 MPa, and drying for 40 hours to obtain 384g of cyclosporine A product, wherein the yield is 45.2%. The acetone is refined once in the experiment, and the maximum single impurity of 0.71 percent and the cyclosporin A with the content of 98.1 percent can be obtained once by crystallizing ethyl acetate and n-hexane.

Claims (10)

1.一种环孢菌素A结晶母液的回收方法,包括以下步骤:1. A method for recovering cyclosporin A crystallization mother liquor, comprising the following steps: 1)环孢菌素A结晶母液去溶剂,加乙腈溶解,固液分离得滤液;1) removing the solvent from the cyclosporin A crystal mother liquor, adding acetonitrile to dissolve it, and separating the solid and liquid to obtain a filtrate; 2)将步骤1)得到的滤液活性炭脱色处理,得脱色液;2) decolorizing the filtrate obtained in step 1) with activated carbon to obtain a decolorized liquid; 3)将步骤2)得到的脱色液回收溶剂,加极性溶剂一次结晶,固液分离得结晶I;3) recovering the solvent from the decolorized solution obtained in step 2), adding a polar solvent for primary crystallization, and performing solid-liquid separation to obtain crystal I; 4)将步骤3)得到的结晶I加非极性溶剂二次结晶,固液分离得结晶II;4) adding a non-polar solvent to the crystal I obtained in step 3) for secondary crystallization, and separating the solid and liquid to obtain crystal II; 5)将步骤4)得到的结晶II加极性溶剂转晶,固液分离,真空干燥,得环孢菌素A成品。5) adding a polar solvent to the crystal II obtained in step 4) to transform the crystal, separate the solid and liquid, and vacuum dry to obtain the cyclosporin A product. 2.按照权利要求1所述的纯化方法,其特征在于步骤2)所述活性炭脱色条件:脱色温度为40℃—50℃,所述活性炭加入量为环孢菌素A重量的1%~3%(w/w)。2. The purification method according to claim 1, characterized in that the activated carbon decolorization conditions in step 2) are: the decolorization temperature is 40°C-50°C, and the amount of activated carbon added is 1% to 3% (w/w) of the weight of cyclosporin A. 3.按照权利要求1所述的纯化方法,其特征在于步骤3)所述回收溶剂是在温度为50℃~60℃和真空度为-0.09~-0.1Mpa条件下减压浓缩。3. The purification method according to claim 1 is characterized in that the recovery solvent in step 3) is concentrated under reduced pressure at a temperature of 50°C to 60°C and a vacuum degree of -0.09 to -0.1 MPa. 4.按照权利要求1所述的纯化方法,其特征在于步骤3)进一步包括一次结晶前加入结晶体系体积15%~20%的纯化水。4. The purification method according to claim 1, characterized in that step 3) further comprises adding 15% to 20% of the volume of the crystallization system of purified water before the primary crystallization. 5.按照权利要求4所述的纯化方法,其特征在于所述一次结晶条件:析晶温度为-5℃~0℃,析晶保温时间为2h,过滤温度为-15℃~-10℃。5. The purification method according to claim 4 is characterized in that the primary crystallization conditions are: crystallization temperature is -5°C to 0°C, crystallization insulation time is 2h, and filtration temperature is -15°C to -10°C. 6.按照权利要求1所述的纯化方法,其特征在于步骤4)所述非极性溶剂选自乙酸乙酯、己烷和石油醚中的至少一种,所述非极性溶剂加入量为产品量10~50倍(w/v)。6. The purification method according to claim 1, characterized in that the non-polar solvent in step 4) is selected from at least one of ethyl acetate, hexane and petroleum ether, and the amount of the non-polar solvent added is 10 to 50 times the amount of the product (w/v). 7.按照权利要求1所述的纯化方法,其特征在于步骤4)所述二次结晶条件:纯化时析晶温度为-10℃~-5℃,析晶保温时间为2h,过滤温度为-20℃~-15℃。7. The purification method according to claim 1 is characterized in that the secondary crystallization conditions in step 4) are as follows: the crystallization temperature during purification is -10°C to -5°C, the crystallization insulation time is 2 hours, and the filtration temperature is -20°C to -15°C. 8.按照权利要求1所述的纯化方法,其特征在于步骤5)所述转晶条件:环孢菌素A浓度为2%~5%,纯化时析晶温度为-5℃~0℃,保温时间为2h,过滤温度为-10℃~-5℃。8. The purification method according to claim 1, characterized in that the crystallization conditions in step 5) are: cyclosporin A concentration is 2% to 5%, the crystallization temperature during purification is -5°C to 0°C, the insulation time is 2 hours, and the filtration temperature is -10°C to -5°C. 9.按照权利要求1所述的纯化方法,其特征在于步骤5)所述干燥条件:温度40~70℃,真空度-0.09MPa~-0.1Mpa,干燥时间40h。9. The purification method according to claim 1, characterized in that the drying conditions in step 5) are: temperature 40-70°C, vacuum degree -0.09MPa to -0.1Mpa, and drying time 40h. 10.按照权利要求1所述的纯化方法,其特征在于步骤3)和步骤5)所述极性溶剂为乙醇、甲醇和丙酮中的至少一种,所述极性溶剂为产品量10~50倍(w/v)。10. The purification method according to claim 1, characterized in that the polar solvent in step 3) and step 5) is at least one of ethanol, methanol and acetone, and the amount of the polar solvent is 10 to 50 times (w/v) the amount of the product.
CN202311613655.1A 2023-11-29 2023-11-29 Method for recovering cyclosporine A crystallization mother liquor Pending CN120058866A (en)

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