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Process for the preparation of nebivolol

By using fungal esterase from Xinyu Shekou Shell for enzymatic hydrolysis and acid-alkali extraction and separation, the problems of multiple steps and low yield in the existing nebivolol synthesis were solved, and efficient and simplified nebivolol preparation was achieved. Improved overall yield and stereoselectivity.

Active Publication Date: 2013-07-31
MENARINI INT OPERATIN S LUXEMBORG SA
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0039] As for the separation of enantiomers at the level of 6-fluoro-chroman-2-carboxylic acid, it is known to employ amide formation of (+)-dehydroabietamine followed by fractional crystallization and amide hydrolysis to recover the acid (EP0334429 ) method is laborious and provides rather low yields
[0040] Regarding the enzymatic resolution of carboxylate esters, this is a method known in the literature, but it has never been used for esters of fluoroderivatives of chroman-2-carboxylic acid, and thus also for nebivolol synthesis

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0098] As described in EP-0687305, recombinant E. coli strains containing the esterase originally expressed in Ulmus chinensis were grown according to techniques well known to those skilled in the art. The cell fraction was lysed by sonication and the lysate was centrifuged to obtain a cell-free supernatant. Mix 1.6 mL of a solution (6800 units / mL) containing esterase (lipase) obtained from Ulmus chinensis (6800 units / mL) and about 25 g of ethyl 6-fluorochroman-2-carboxylate (1) in 25 mL of deionized water with Add 100 μL of the suspension in Tween 80 to 500 mL of 0.1N NaHCO 3 buffer solution (pH 9.7), optionally with 2N NaOH to adjust the pH to 9.7. The mixture thus obtained was stirred slowly.

[0099] The pH was automatically maintained at 9.7 with a controlled addition of 2N NaOH solution.

[0100] The progress of the reaction was controlled by HPLC.

[0101] At the end of the hydrolysis reaction, the mixture was extracted with dichloromethane to obtain the ester in th...

Embodiment 2

[0110] Example 2 Preparation of Acyl Meldrum Derivatives

[0111]

[0112] 28 g of the resolved (R) acid were dissolved in 250 mL of anhydrous dichloromethane; 1.4 equivalents of oxalyl chloride and DMF were added dropwise to the resulting solution. The solution was kept under stirring at room temperature under N 2 Atmospheric conditions; after 1.5 hours, the solvent was evaporated to give an oil which was redissolved in 200 mL of anhydrous dichloromethane. Separately, medrum's acid (1.05 equivalents) and pyridine (2 equivalents) were dissolved in anhydrous dichloromethane (150 mL), and stirred at 0°C for 15 minutes. To this solution was added the previously formed acid chloride. At the end of the addition, the mixture was stirred at 0 °C for 1 hour and at room temperature for an additional 45 minutes. Then, it was diluted with another 500 mL of dichloromethane and washed with H 2 O (2×200mL), 2N HCl (100mL), water and brine washed the organic phase, and 2 SO 4 Dry ...

Embodiment 3

[0113] Example 3 Preparation of β-ketoesters

[0114]

[0115] 40 g of crude acyl medrum derivative (R) were placed under stirring with 110 mL of tert-butanol; the resulting mixture was heated to 80° C. for 1 hour until the control by HPLC showed marked disappearance of the starting product. At the end of the reaction, tert-butanol was evaporated under reduced pressure; it was treated with 500 ml ethyl acetate and washed with saturated NaHCO 3 solution, neutral H 2 O, brine washes organic phase, and it is in Na 2 SO 4 Dry on top. The solvent was then evaporated to obtain 28 g of crude β-ketoester as an oil (HPLC purity = 69%, λ = 280 nm), which was used in subsequent reactions without further purification.

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PUM

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Abstract

The present invention relates to a novel process for the synthesis of the Nebivolol product depicted in Scheme 1, comprised of a reduced number of high-yield steps, and characterized by the enzymatic resolution of the chroman ester precursor.

Description

technical field [0001] The present invention relates to a new method for the synthesis of nebivolol. Background technique [0002] Nebivolol is two enantiomers [2S[2R[R[R]]]]α,α'-[imino-bis(methylene)]bis[6-fluoro-chroman-2 -Methanol] and a racemic mixture of [2R[2S[S[S]]]]α,α'-[imino-bis(methylene)]bis[6-fluoro-chroman-2-methanol] (Structure 1). [0003] [0004] Nebivolol [0005] Structural Formula 1 [0006] In particular, it was reported that the enzymatic resolution of the starting chromanyl ester (1) was treated with a stereoselective enzyme belonging to the family of esterases, existing in native or recombinant form, and capable of deriving from Microorganisms obtained from Ophiostoma novoulmi. [0007] The esters and acids thus obtained can be converted into the corresponding "semichiral" epoxides, the (RR+RS,4) pairs and (SS+SR , 5) Right. [0008] Next, each pair of components can be separated by exploiting their different reactivity with benzylamine in ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C07D311/58
CPCC12P17/162C07D311/58C07D407/12
Owner MENARINI INT OPERATIN S LUXEMBORG SA