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CN111087400A - Synthetic method of sitagliptin - Google Patents

Synthetic method of sitagliptin Download PDF

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Publication number
CN111087400A
CN111087400A CN202010029573.2A CN202010029573A CN111087400A CN 111087400 A CN111087400 A CN 111087400A CN 202010029573 A CN202010029573 A CN 202010029573A CN 111087400 A CN111087400 A CN 111087400A
Authority
CN
China
Prior art keywords
sitagliptin
hydroxy
piperazine hydrochloride
dioxane
dimethyl
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
CN202010029573.2A
Other languages
Chinese (zh)
Inventor
刘万里
李彬
薛洪泽
侯伟宏
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Tianjin Minxiang Biomedical Co ltd
Original Assignee
Tianjin Minxiang Biomedical Co ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Tianjin Minxiang Biomedical Co ltd filed Critical Tianjin Minxiang Biomedical Co ltd
Priority to CN202010029573.2A priority Critical patent/CN111087400A/en
Publication of CN111087400A publication Critical patent/CN111087400A/en
Pending legal-status Critical Current

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D487/00Heterocyclic compounds containing nitrogen atoms as the only ring hetero atoms in the condensed system, not provided for by groups C07D451/00 - C07D477/00
    • C07D487/02Heterocyclic compounds containing nitrogen atoms as the only ring hetero atoms in the condensed system, not provided for by groups C07D451/00 - C07D477/00 in which the condensed system contains two hetero rings
    • C07D487/04Ortho-condensed systems

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)

Abstract

The invention discloses a synthesis method of sitagliptin, which comprises the following steps: reacting 2,4, 5-trifluoro-phenylacetic acid serving as a raw material with pivaloyl chloride to convert the trichloroacetic acid into acyl chloride, condensing the acyl chloride with 2, 2-dimethyl-1, 3-dioxane-4, 6-diketone under the combined action of N, N-diisopropylethylamine and 4-dimethylaminopyridine to obtain 5- [ 1-hydroxy-2- (2, 4, 5-trifluorophenyl) ethylidene ] -2, 2-dimethyl-1, 3-dioxane-4, 6-diketone, refluxing in a methanol solution for ring opening and decarbonylation to obtain keto ester, and reacting with an intermediate 3-trifluoromethyl- [1, 2, 4] triazolo [4, 3, a ] piperazine hydrochloride at 0 ℃ to obtain amino-protected sitagliptin. The catalyst has less consumption, the reaction conditions in China in the route are mild, the operation of each step of reaction is simple, the feasibility is relatively high, and the method is suitable for industrial production.

Description

Synthetic method of sitagliptin
Technical Field
The invention relates to the field of sitagliptin preparation, in particular to a synthetic method of sitagliptin.
Background
Sitagliptin is a dipeptidyl peptidase-IV inhibitor drug used for treating type II diabetes, which controls the blood sugar level of a diabetic patient by improving the insulin production capacity of the pancreatic islets β cells of the diabetic patient, increasing the secretion of insulin when the blood sugar is increased, and has good tolerance, no weight gain and no risk of hypoglycemia.The 10M Merck company announces that sitagliptin phosphate (sitagliptin phosphate) is approved by the U.S. food and drug administration in 2006.
At present, most methods for synthesizing sitagliptin at home and abroad relate to chiral induction and asymmetric hydrogenation: the steps are different in length, four or five steps are less, and ten steps are more. The optical purity ee% of the chiral induction and asymmetric hydrogenation is lower, and the ee% needs to be improved by further purification, so that the resource waste exists. And half of isomers in the chemical resolution method cannot be utilized, so that the yield is low and the cost is high.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides a sitagliptin synthesis method, which is low in catalyst consumption, mild in reaction conditions in the route, simple in reaction operation in each step, relatively high in feasibility and suitable for industrial production.
In order to achieve the aim of the invention, the invention adopts the specific scheme that:
a process for synthesizing sitagliptin includes such steps as using 2,4, 5-trifluoro-phenylacetic acid as raw material, reacting with pivaloyl chloride to convert it to acyl chloride, condensing with 2, 2-dimethyl-1, 3-dioxane-4, 6-diketone under the action of N, N-diisopropyl ethylamine and 4-dimethylamino pyridine to obtain 5- [ 1-hydroxy-2- (2, 4, 5-trifluorophenyl) ethylidene ] -2, 2-dimethyl-1, 3-dioxane-4, 6-diketone, reflux ring-opening decarbonylation in methanol solution to obtain keto ester, catalytic asymmetric hydrogenation of keto ester at 80 deg.C in methanol solution with (S) -dinaphthalene diphenyl phosphate and anhydrous ruthenium sodium, hydrolysis with hydroxide to obtain β -hydroxy acid, condensation of β -hydroxy acid with N-ethyl-N-dimethylamino-propylamine carbodiimide, condensation with O-benzyl amine, dehydration of condensation compound in triphenyl phosphine and diisopropyl azodicarboxylate to obtain β -lactam compound, hydrolysis of its amide in N-ethyl-N-dimethylamino-propylamine under the condition of reaction with morpholine hydrochloride, hydrolysis of L-methyl ester at 3-hydroxy acid to obtain morpholine hydrochloride, hydrolysis of 3-methyl ester at 0-hydroxy amide compound and hydrolysis of morpholine-3-amino-methyl ester.
Further, the amount of the (S) -binaphthyl diphenyl phosphate and anhydrous ruthenium trichloride catalyst was 0.2m 01% of the reactants.
The invention has the beneficial effects that:
the catalyst has less consumption, the reaction conditions in China in the route are mild, the operation of each step of reaction is simple, the feasibility is relatively high, and the method is suitable for industrial production.
Detailed Description
The present invention is further described below by way of specific examples, but the present invention is not limited to only the following examples. Variations, combinations, or substitutions of the invention, which are within the scope of the invention or the spirit, scope of the invention, will be apparent to those of skill in the art and are within the scope of the invention.
A process for synthesizing sitagliptin includes such steps as using 2,4, 5-trifluoro-phenylacetic acid as raw material, reacting with pivaloyl chloride to convert it to acyl chloride, condensing with 2, 2-dimethyl-1, 3-dioxane-4, 6-diketone under the action of N, N-diisopropyl ethylamine and 4-dimethylamino pyridine to obtain 5- [ 1-hydroxy-2- (2, 4, 5-trifluorophenyl) ethylidene ] -2, 2-dimethyl-1, 3-dioxane-4, 6-diketone, reflux ring-opening decarbonylation in methanol solution to obtain keto ester, catalytic asymmetric hydrogenation of keto ester at 80 deg.C in methanol solution with (S) -dinaphthalene diphenyl phosphate and anhydrous ruthenium sodium, hydrolysis with hydroxide to obtain β -hydroxy acid, condensation of β -hydroxy acid with N-ethyl-N-dimethylamino-propylamine carbodiimide, condensation with O-benzyl amine, dehydration of condensation compound in triphenyl phosphine and diisopropyl azodicarboxylate to obtain β -lactam compound, hydrolysis of its amide in N-ethyl-N-dimethylamino-propylamine under the condition of reaction with morpholine hydrochloride, hydrolysis of L-methyl ester at 3-hydroxy acid to obtain morpholine hydrochloride, hydrolysis of 3-methyl ester at 0-hydroxy amide compound and hydrolysis of morpholine-3-amino-methyl ester.
The dosage of the (S) -binaphthyl diphenyl phosphate and the anhydrous ruthenium trichloride catalyst is 0.2m 01% of the reactants.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the present invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention should be included in the scope of the present invention.

Claims (2)

1. A synthetic method of sitagliptin is characterized in that 2,4, 5-trifluoro phenylacetic acid is used as a raw material, reacts with pivaloyl chloride to be converted into acyl chloride, then is condensed with 2, 2-dimethyl-1, 3-dioxane-4, 6-diketone under the combined action of N, N-diisopropyl ethylamine and 4-dimethylamino pyridine to obtain 5- [ 1-hydroxy-2- (2, 4, 5-trifluoro phenyl) ethylidene ] -2, 2-dimethyl-1, 3-dioxane-4, 6-diketone in a methanol solution, then reflux ring opening and decarbonylation are carried out in the methanol solution to obtain ketone ester, asymmetric hydrogenation is catalyzed by (S) -binaphthyl diphenyl phosphate and anhydrous ruthenium trichloride in the methanol solution at the temperature of 80 ℃, then sodium hydroxide is used for hydrolysis to obtain β -hydroxy acid, β -hydroxy acid is condensed with O-benzyl in the presence of N-ethyl-N-dimethylamino carbodiimide, condensation compound is dehydrated and cyclized in triphenyl phosphine and diisopropyl azodicarboxylate to obtain a condensation compound, then the condensation compound is hydrolyzed with N-ethyl-N-dimethylamino-carbodiimide to obtain a ring opening reaction methyl piperazine hydrochloride, and a reaction product of piperazine hydrochloride under the temperature of 0-hydroxy amide type (S-methyl chloride) and the reaction product of EDC type piperazine hydrochloride to obtain the intermediate of L-methyl piperazine hydrochloride.
2. The method for synthesizing sitagliptin according to claim 1, characterized in that the amount of the (S) -binaphthyl diphenyl phosphate and anhydrous ruthenium trichloride catalyst is 0.2m 01% of the reactants.
CN202010029573.2A 2020-01-13 2020-01-13 Synthetic method of sitagliptin Pending CN111087400A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202010029573.2A CN111087400A (en) 2020-01-13 2020-01-13 Synthetic method of sitagliptin

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202010029573.2A CN111087400A (en) 2020-01-13 2020-01-13 Synthetic method of sitagliptin

Publications (1)

Publication Number Publication Date
CN111087400A true CN111087400A (en) 2020-05-01

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Family Applications (1)

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CN202010029573.2A Pending CN111087400A (en) 2020-01-13 2020-01-13 Synthetic method of sitagliptin

Country Status (1)

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CN (1) CN111087400A (en)

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2004087650A2 (en) * 2003-03-27 2004-10-14 Merck & Co. Inc. Process and intermediates for the preparation of beta-amino acid amide dipeptidyl peptidase-iv inhibitors

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2004087650A2 (en) * 2003-03-27 2004-10-14 Merck & Co. Inc. Process and intermediates for the preparation of beta-amino acid amide dipeptidyl peptidase-iv inhibitors

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
KARL B. HANSEN等: "First Generation Process for the Preparation of the DPP-IV Inhibitor Sitagliptin" *

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Application publication date: 20200501