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Process for preparing optic pure 2-fluoro-alphar-methyl-[1,1'-diphenyl]-4-acetic acid

A diphenyl and methyl technology, applied to optically pure 2-fluoro-α-methyl-[1, can solve the problems of only 90-95% optical purity, not allowing optically pure compounds, and severe reaction conditions, etc. Achieve the effect of high yield, low cost and high optical purity of the product

Inactive Publication Date: 2004-12-22
SHANGHAI INST OF ORGANIC CHEM CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0006] U.S. Pat. No. 4,209,638 (The Boots Company Limited) by heating the racemate of 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid and nitrogen-containing organic Salts of bases (such as α-methylbenzylamine) can increase the ratio of the desired enantiomer from the racemate, but in some embodiments, the reaction conditions are very severe, such as heating at reflux temperature for several days, and do not Allows obtaining optically pure compounds from racemates
[0007] U.S.Pat.No.4,973,745 (Medice Chem.-Pharm.Fabrik Putter GmbH & Co.KG) uses optically pure threo-1-p-nitrophenyl-2-aminopropane-1,3-diol as resolving agent , the (S)-enantiomer was prepared from the racemate of 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid, but its optical purity was only 90-95%
[0008] U.S.Pat.No.4,983,765 (PAZ Arzneimittel-Entwicklungsgesellschaft mbH) uses phenethylamine as resolving agent from the racemate of 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid or The (S)-enantiomer was prepared from a mixture of (S)- and (R)-enantiomers with an optical purity greater than 99%, but in low yields (less than 50%)

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] Example 1: Preparation of (S)-(+)-2-fluoro-α-methyl-[1,1'-diphenyl]-4-acetic acid

[0025] Take 100 g (409 mmol) of the racemate of 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid and (-)-1-deoxy-1-n-octylamino-D- Put 60 g (204.5 mmol) of glucitol into a reaction flask, add 1500 ml of isopropanol, and heat to reflux in an oil bath for 15 minutes. After the reaction was finished, stand at room temperature for more than 10 hours to crystallize, filter to obtain 95g (177mmol) of white solid ([α] D 20 =-17.8° (c=1, MeOH)), yield 86.4%.

[0026] The above white solid was recrystallized twice, the salt / isopropanol ratio was 1g / 13.5ml, and 80g (149mmol) of white solid was obtained ([α] D 20 =-19.0° (c=1, MeOH)), yield 72.7%.

[0027] Take 80 g (149 mmol) of the solid obtained in the third crystallization, put it into a round bottom flask, add 900 ml of 2N sulfuric acid aqueous solution and 600 ml of ethyl acetate, stir to dissolve the solid, perform liquid-liquid exchange...

Embodiment 2

[0029] Example 2: Racemization

[0030] The filtrate obtained by combining the reaction and recrystallization of Example 1 was concentrated under reduced pressure to obtain 80 g of a light yellow solid, which was put into a reaction flask, 400 ml of 4N sodium hydroxide solution was added, and the mixture was heated to reflux in an oil bath for 6 hours. After the reaction, cool to room temperature, add 140ml concentrated hydrochloric acid and 300ml ethyl acetate, stir to dissolve the solid, perform liquid-liquid exchange, extract the aqueous solution with ethyl acetate, combine the ethyl acetate extracts, wash with water, and dry over anhydrous sodium sulfate , filtered, and the filtrate was concentrated under reduced pressure to obtain 59.7 g of the racemate ([α] D 20 =0° (c=1, MeOH)), yield 93.8%.

Embodiment 3

[0031] Example 3: Preparation of (S)-(+)-2-fluoro-α-methyl-[1,1'-diphenyl]-4-acetic acid

[0032] Take 100 g (409 mmol) of the racemate of 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid and (-)-1-deoxy-1-n-octylamino-D- Put 60 g (204.5 mmol) of glucitol into a reaction flask, add 1400 ml of absolute ethanol, and heat to reflux in an oil bath for 15 minutes. After the reaction was finished, stand at room temperature for more than 10 hours to crystallize, filter to obtain 59.2 g (110 mmol) of white solid ([α] D 20 =-18.3° (c=1, MeOH)), yield 53.6%.

[0033] Put 59.2g (110mmol) of the obtained white solid into a round-bottomed flask, add 670ml of 2N sulfuric acid aqueous solution, stir for 2 hours, filter, wash the solid with a small amount of water, and dry to obtain (S)-(+)-2-fluoro-α-methyl -[1,1'-diphenyl]-4-acetic acid 25.2g (103mmol) ([α] D 20 =+42.6° (c=1, EtOH)), ee value 0.95, yield 50.4% (based on (S)-enantiomer), chemical purity greater than 98%.

[0034] Add co...

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Abstract

The present invention prepares optically pure 2-fluoro-alpha-methyl-[1,1'-diphenyl]-4-acetic acid from 2-fluoro-alpha-methyl-[1,1-diphenyl]-4-acetic acid racemic body and through chemical resolution process. The said method has not only simple process, high yield and low cost but also complete resolution, so that it is suitable for industrial production.

Description

technical field [0001] The invention relates to a method for preparing optically pure 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid racemate from 2-fluoro-α-methyl-[1,1′- Diphenyl]-4-acetic acid method. Furthermore, it is a kind of diastereomeric salt formed by reacting 2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid racemate with optically pure amine, and then purified by crystallization. Acid treatment or hydrolysis converts (S)-(+)-2-fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid and (R)-(-)-2-fluoro- A convenient method for α-methyl-[1,1'-diphenyl]-4-acetic acid. Background technique [0002] 2-Fluoro-α-methyl-[1,1′-diphenyl]-4-acetic acid is a non-steroidal anti-inflammatory drug, its mechanism of action is to inhibit the cyclooxygenase system, which can reduce inflammation and relieve pain. For the treatment of rheumatic diseases, the racemate is currently marketed and clinically applied. [0003] The racemate contains a pair of enantiomers of 2-fluoro-α-methyl-[1...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C07B57/00C07C57/58
CPCY02P20/582
Inventor 林国强雷新胜张爱民俞晓明刘汉泉骆宏丰夏立钧
Owner SHANGHAI INST OF ORGANIC CHEM CHINESE ACAD OF SCI