[go: up one dir, main page]

EP1891010A2 - A process for the preparation of an injectable solution of (2s)-n-(2;6-dimethyl-phenyl)-1-propyl-2-piperidincarboxamide - Google Patents

A process for the preparation of an injectable solution of (2s)-n-(2;6-dimethyl-phenyl)-1-propyl-2-piperidincarboxamide

Info

Publication number
EP1891010A2
EP1891010A2 EP06754189A EP06754189A EP1891010A2 EP 1891010 A2 EP1891010 A2 EP 1891010A2 EP 06754189 A EP06754189 A EP 06754189A EP 06754189 A EP06754189 A EP 06754189A EP 1891010 A2 EP1891010 A2 EP 1891010A2
Authority
EP
European Patent Office
Prior art keywords
ropivacaine
preparation
propyl
piperidincarboxamide
water
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.)
Withdrawn
Application number
EP06754189A
Other languages
German (de)
French (fr)
Inventor
Roberto Angeli
Marco Possenti
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.)
L Molteni and C dei Fratelli Alitti Societa di Esercizio SpA
Molteni and C SpA
Original Assignee
L Molteni and C dei Fratelli Alitti Societa di Esercizio SpA
Molteni and C SpA
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 L Molteni and C dei Fratelli Alitti Societa di Esercizio SpA, Molteni and C SpA filed Critical L Molteni and C dei Fratelli Alitti Societa di Esercizio SpA
Publication of EP1891010A2 publication Critical patent/EP1891010A2/en
Withdrawn legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D211/00Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings
    • C07D211/04Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom
    • C07D211/06Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having no double bonds between ring members or between ring members and non-ring members
    • C07D211/36Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having no double bonds between ring members or between ring members and non-ring members with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
    • C07D211/60Carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61PSPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
    • A61P23/00Anaesthetics
    • A61P23/02Local anaesthetics

Definitions

  • the present invention relates to a process for the preparation of an injectable solution of (2S)-(-)-N-(2;6-dimethyl-phenyl)-l-propyl-2- piperidincarboxamide (I)
  • Compound (I) is an active ingredient effective as local anesthetic, cited in the Merck Index, XIII Edition, page 1483, # 8339, Ropivacaine. Its preparation is disclosed in EP 0 151 110, expired on August 1 st , 2003, starting from (S)-pipecolic acid 2,6-xylidide and n-propyl bromide.
  • the commercially available formulation is a completely clear solution, which contains Ropivacaine neutralized with hydrochloric acid.
  • "Sodium hydroxide” as well as “hydrochloric acid” axe cited among the excipients: this is clearly mistaken, as any skilled chemist knows that the presence of sodium hydroxide excludes that of hydrochloric acid and vice versa.
  • the commercially available solution has to be slightly acidic (pH is in fact4.0-6.0) as Ropivacaine is water-insoluble, and would therefore precipitate in an alkali medium.
  • Ropivacaine injectable aqueous solutions can be easily prepared starting from the free base, prepared from the same intermediates as in EP O 151 110, but using tetrahydrofuran as the solvent, followed by repeated washings with diisopropyl ether, which completely remove the undesired enantiomer.
  • the resulting Ropivacaine base which is perfectly measurable as it is not hygroscopic (contrary to the anhydrous hydrochloride), is directly transformed in situ by addition to the hydrochloric acid solution in water for injectables; after complete dissolution, pH is adjusted to the desired range (5.6-5.8) by addition of sodium hydroxide After the steam sterilization the pH of solution decreases
  • Ropivacaine injectable formulations are thereby obtained in a remarkably simpler mode than disclosed in EP 0 239 710.
  • the complex preparation of the hydrochloride monohydrate described in such Patent is in fact avoided, and the desired result is directly obtained from Ropivacaine base, without involving other intermediates.
  • Ropivacaine is prepared starting from the intermediate (S) pipecolic acid 2,6-xylidide (145 g; 0.624 mols) and n-propyl bromide (766 g; 6.24 mols) in tetrahydrofuran (2.5 L) under reflux for approx. 20-24 hours. Inorganic salts are filtered off and the solvent is evaporated to dryness to obtain a dry- solid, consisting of crude Ropivacaine base. The solid is taken up into the minimum amount of diisopropyl ether (200 ml) and filtered under vacuum.
  • the resulting product is a non-hygroscopic solid, that is stable in time and can be used for the formation of the hydrochloride in situ during the preparation of the pharmaceutical product.
  • a suitable 10 liters two-necked round-bottom flask (fitted with a stirring shaft and pH meter, placed on a 25.0 kg technique balance) is loaded with about 9.0 kg of water for injectables, 71.1988 g of sodium chloride are dissolved and acidified by addition of 321.7 ml of 1 N hydrochloric acid (equivalent to the theoretical amount to form the hydrochloride, starting from Ropivacaine base), stirring at about 350 rpm, under nitrogen. 88.2684 g of Ropivacaine base are added under the same conditions, stirring is increased to 1000 rpm and kept for approx. 2 hours 30 minutes.
  • pH pH is adjusted to 5.5.6-5.8 with 1 N sodium hydroxide under stirring. Afterwards, the solution is adjusted to 10.00 kg with water for injectables, keeping stirring for a further 60 minutes.
  • the solution is clear and colorless, pH ranges from 5.5.6 to 5.8and osmolarity is equivalent to that of the reference product.
  • the solution is then distributed in polypropylene vials, according to the blow-fill-seal technique, with pre-filtration through 1-0.2 ⁇ m filters and filtration through 0.22 ⁇ m absolute filters, immediately upstream the filling machine. Afterwards, the resulting vials are individually sealed, under high vacuum, with the selected plastic material and steam sterilized at 121°Cfor 15 minutues b) Preparation of Ropivacaine HCl solution bulk 7.5 mg/ml starting from Ropivacaine base by acidification
  • Example 2 a The procedure of Example 2 a) is repeated, using 241.3. ml of 1 N hydrochloric acid (equivalent to the theoretical amount to form the hydrochloride from Ropivacaine base), 75.8985 g of sodium chloride and 66.2013 g of Ropivacaine base.
  • the procedure of Example 2 a) is repeated, using 64.3 ml of 1 hydrochloric acid (equivalent to the theoretical amount to form the hydrochloride from Ropivacaine base), 86.2378 g of sodium chloride +and 17.6537 g of Ropivacaine base.
  • This concentration could be distributed in polypropylene vials, as described in Example 2, and in polypropylene bags with pre-filtration through 1-0.2 ⁇ m filters and filtration through 0.22 ⁇ m absolute filters, immediately upstream the filling machine. Afterwards, the resulting bags are individually sealed, under high vacuum, with the selected plastic material and steam sterilized at 121 0 C for 15 minutes.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Anesthesiology (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Nuclear Medicine, Radiotherapy & Molecular Imaging (AREA)
  • Pharmacology & Pharmacy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Animal Behavior & Ethology (AREA)
  • General Health & Medical Sciences (AREA)
  • Public Health (AREA)
  • Veterinary Medicine (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Medicinal Preparation (AREA)

Abstract

A process for the preparation of an injectable solution of (2S)-(-)-N- (2;6-dimethyl-phenyl)-l-propyl-2-piperidincarboxamide (Ropivacaine) starting from Ropivacaine base substantially free from the dextro enantiomer, by dissolution of the same in water for injectables containing hydrochloric acid in stoichiometric amounts.

Description

A PROCESS FOR THE PREPARATION OF AN INJECTABLE SOLUTION OF (25VN-(2:6-DIMETHYL-PHENYL)-l-PROPYL-2- PIPERIDINCARBOXAMIDE
The present invention relates to a process for the preparation of an injectable solution of (2S)-(-)-N-(2;6-dimethyl-phenyl)-l-propyl-2- piperidincarboxamide (I)
Compound (I) is an active ingredient effective as local anesthetic, cited in the Merck Index, XIII Edition, page 1483, # 8339, Ropivacaine. Its preparation is disclosed in EP 0 151 110, expired on August 1st, 2003, starting from (S)-pipecolic acid 2,6-xylidide and n-propyl bromide.
The presently commercially available specialty (Naropina) is disclosed in "L'Informatore Farmaceutico", Edition 2005. page 852) as follows:
"1 ml of solution contains Ropivacaine hydrochloride monohydrate 2 mg/ml - 7,5 mg/ml - 10 mg/ml. Excipients: sodium chloride, hydrochloric acid, sodium hydroxide, water for injectable preparations " .
It should be noted that the commercially available formulation is a completely clear solution, which contains Ropivacaine neutralized with hydrochloric acid. "Sodium hydroxide" as well as "hydrochloric acid" axe cited among the excipients: this is clearly mistaken, as any skilled chemist knows that the presence of sodium hydroxide excludes that of hydrochloric acid and vice versa. Furthermore, as the commercially available solution is completely clear, it has to be slightly acidic (pH is in fact4.0-6.0) as Ropivacaine is water-insoluble, and would therefore precipitate in an alkali medium. In addition, the expression "contains Ropivacaine hydrochloride monohydrate" is not true, as the definition "monohydrate" is incongruous in case of an aqueous solution: the exact expression should be "prepared from Ropivacaine hydrochloride monohydrate" , as it can be evinced by a subsequent Patent, EP 0 239 710, expiring on December 15. 2006 (protection extended to September 15. 2010 by the Supplementary Protection Certificate n. 572). The latter Patent evidences the drawbacks of previous EP 0 151 110, in particular that: a) the process for the preparation of Ropivacaine anhydrous hydrochloride affords a product containing 10% of the undesired
(R)-(+) enantiomer; b) the anhydrous hydrochloride is "hygroscopic and therefore instable, and contains about 2% water", whereas one mole of crystallization water would involve 5.5% water; c) a product having variable water content requires the determination of such content each time the pharmaceutical formulation is prepared.
According to EP 0 239 710 said drawbacks are avoided through the preparation of the hydrochloride monohydrate. According to claims 4, 5 and 6, said preparation is carried out treating a hydrochloride aqueous solution
(containing the (R)-(+) enantiomer) with acetone at a temperature ranging from 45°C to the acetone boiling point (56°C). It is evident from said Patent
(see particularly column 2, lines 10-37, and Example 1) that the preparation is remarkably troublesome, in that it requires carefully monitoring water to acetone ratios, as well as acetone temperature; moreover, the operation has to be repeated to obtain an optically pure compound.
It has now been found that Ropivacaine injectable aqueous solutions can be easily prepared starting from the free base, prepared from the same intermediates as in EP O 151 110, but using tetrahydrofuran as the solvent, followed by repeated washings with diisopropyl ether, which completely remove the undesired enantiomer. According to the invention, the resulting Ropivacaine base, which is perfectly measurable as it is not hygroscopic (contrary to the anhydrous hydrochloride), is directly transformed in situ by addition to the hydrochloric acid solution in water for injectables; after complete dissolution, pH is adjusted to the desired range (5.6-5.8) by addition of sodium hydroxide After the steam sterilization the pH of solution decreases
Ropivacaine injectable formulations are thereby obtained in a remarkably simpler mode than disclosed in EP 0 239 710. The complex preparation of the hydrochloride monohydrate described in such Patent is in fact avoided, and the desired result is directly obtained from Ropivacaine base, without involving other intermediates.
The following examples illustrate the process according to the invention.
Example 1. Preparation of Ropivacaine base
Ropivacaine is prepared starting from the intermediate (S) pipecolic acid 2,6-xylidide (145 g; 0.624 mols) and n-propyl bromide (766 g; 6.24 mols) in tetrahydrofuran (2.5 L) under reflux for approx. 20-24 hours. Inorganic salts are filtered off and the solvent is evaporated to dryness to obtain a dry- solid, consisting of crude Ropivacaine base. The solid is taken up into the minimum amount of diisopropyl ether (200 ml) and filtered under vacuum. The residue is washed on the filter with the same solvent (3 x 150 ml) and dried at 55°C under vacuum to obtain 161 g of Ropivacaine base in a 94% molar yield on the xylidide; HPLC purity = 99.75%; HPLC enantiomeric purity = 99.54%, concentration = 99.5%; loss on drying: 0.3%. The resulting product is a non-hygroscopic solid, that is stable in time and can be used for the formation of the hydrochloride in situ during the preparation of the pharmaceutical product.
Example 2. Preparation of pharmaceutical formulations a) Preparation of the Ropivacaine HCl bulk solution 10 mg/ml starting from Ropivacaine base by acidification
A suitable 10 liters two-necked round-bottom flask (fitted with a stirring shaft and pH meter, placed on a 25.0 kg technique balance) is loaded with about 9.0 kg of water for injectables, 71.1988 g of sodium chloride are dissolved and acidified by addition of 321.7 ml of 1 N hydrochloric acid (equivalent to the theoretical amount to form the hydrochloride, starting from Ropivacaine base), stirring at about 350 rpm, under nitrogen. 88.2684 g of Ropivacaine base are added under the same conditions, stirring is increased to 1000 rpm and kept for approx. 2 hours 30 minutes. When the solution is completely clear (pH 3.6-3.7), pH is adjusted to 5.5.6-5.8 with 1 N sodium hydroxide under stirring. Afterwards, the solution is adjusted to 10.00 kg with water for injectables, keeping stirring for a further 60 minutes.
The solution is clear and colorless, pH ranges from 5.5.6 to 5.8and osmolarity is equivalent to that of the reference product. The solution is then distributed in polypropylene vials, according to the blow-fill-seal technique, with pre-filtration through 1-0.2 μm filters and filtration through 0.22 μm absolute filters, immediately upstream the filling machine. Afterwards, the resulting vials are individually sealed, under high vacuum, with the selected plastic material and steam sterilized at 121°Cfor 15 minutues b) Preparation of Ropivacaine HCl solution bulk 7.5 mg/ml starting from Ropivacaine base by acidification
The procedure of Example 2 a) is repeated, using 241.3. ml of 1 N hydrochloric acid (equivalent to the theoretical amount to form the hydrochloride from Ropivacaine base), 75.8985 g of sodium chloride and 66.2013 g of Ropivacaine base. c) Preparation of Ropivacaine HCI solution bulk 2.0 mg/ml starting from Ropivacaine base by acidification The procedure of Example 2 a) is repeated, using 64.3 ml of 1 hydrochloric acid (equivalent to the theoretical amount to form the hydrochloride from Ropivacaine base), 86.2378 g of sodium chloride +and 17.6537 g of Ropivacaine base. This concentration could be distributed in polypropylene vials, as described in Example 2, and in polypropylene bags with pre-filtration through 1-0.2 μm filters and filtration through 0.22 μm absolute filters, immediately upstream the filling machine. Afterwards, the resulting bags are individually sealed, under high vacuum, with the selected plastic material and steam sterilized at 1210C for 15 minutes.

Claims

1. A process for the preparation of (2S)-(-)-N-(2;6-dimethyl-phenyl)-l- propyl-2-piperidincarboxamide (Ropivacaine) injectable solutions, in which Ropivacaine base, containing the R enantiomer in no more than 0.5% by weight, is dissolved in water for injectables containing hydrochloric acid in the stoichiometric amount, and the resulting solutions are then distributed in single-dose containers according to conventional methods.
2. A process as claimed in claim 1, characterized in that the amount of water for injectable preparations is added to obtain injectable solutions containing the desired amount of Ropivacaine hydrochloride.
3. A process as claimed in claims 1 and 2, in which the final single-dose injectable solutions contain 2 to 10 mg/ml of Ropivacaine hydrochloride.
4. A process according to the above claims, in which Ropivacaine containing the R enantiomer in no more than 0.5% is prepared by reaction of
(S) pipecolic acid 2,6-xylidide with n-propyl bromide in tetrahydrofuran, and the resulting crude Ropivacaine is subjected to repeated washings with diisopropyl ether.
EP06754189A 2005-06-17 2006-06-07 A process for the preparation of an injectable solution of (2s)-n-(2;6-dimethyl-phenyl)-1-propyl-2-piperidincarboxamide Withdrawn EP1891010A2 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
IT001144A ITMI20051144A1 (en) 2005-06-17 2005-06-17 "PROCEDURE FOR THE PREPARATION OF AN INJECTABLE SOLUTION OF (2S) -N- (2; 6-DIMETHYL-FENYL) -1-PROPYL-2-PIPERIDINCARBOSSAMIDE"
PCT/EP2006/005431 WO2006133837A2 (en) 2005-06-17 2006-06-07 A process for the preparation of an injectable solution of (2s)-n-(2;6-dimethyl-phenyl)-1-propyl-2-piperidincarboxamide

Publications (1)

Publication Number Publication Date
EP1891010A2 true EP1891010A2 (en) 2008-02-27

Family

ID=37496886

Family Applications (1)

Application Number Title Priority Date Filing Date
EP06754189A Withdrawn EP1891010A2 (en) 2005-06-17 2006-06-07 A process for the preparation of an injectable solution of (2s)-n-(2;6-dimethyl-phenyl)-1-propyl-2-piperidincarboxamide

Country Status (3)

Country Link
EP (1) EP1891010A2 (en)
IT (1) ITMI20051144A1 (en)
WO (1) WO2006133837A2 (en)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102697708A (en) * 2012-04-17 2012-10-03 上海禾丰制药有限公司 Ropivacaine hydrochloride injection and preparation process thereof

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2797241A (en) 1953-08-28 1957-06-25 Brown Charles Leslie Meredith Diethyl-glycinexylidide and process
GB790762A (en) 1953-08-28 1958-02-19 Arthur Poole A hydrate of lignocaine hydrochloride and process for making it
WO2006127639A2 (en) * 2005-05-25 2006-11-30 Navinta Llc Process for preparation of isotonic aqueous injection of ropivacaine

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0151110B1 (en) * 1983-08-01 1989-03-01 Astra Läkemedel Aktiebolag L-n-n-propylpipecolic acid-2,6-xylidide and method for preparing the same

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2797241A (en) 1953-08-28 1957-06-25 Brown Charles Leslie Meredith Diethyl-glycinexylidide and process
GB790762A (en) 1953-08-28 1958-02-19 Arthur Poole A hydrate of lignocaine hydrochloride and process for making it
WO2006127639A2 (en) * 2005-05-25 2006-11-30 Navinta Llc Process for preparation of isotonic aqueous injection of ropivacaine

Also Published As

Publication number Publication date
ITMI20051144A1 (en) 2006-12-18
WO2006133837A3 (en) 2007-04-19
WO2006133837A2 (en) 2006-12-21

Similar Documents

Publication Publication Date Title
EP1373207B1 (en) Novel amlodipine camsylate and method for preparing thereof
AU2002243069A1 (en) Novel amlodipine camsylate and method for preparing thereof
EP0239710B1 (en) (s)-(-)-1-propyl-2',6'-pipecoloxylidide hydrochloride monohydrate, process for its preparation and pharmaceutical preparation containing it
WO2003043989A1 (en) Hydrophilic (s)-amlodipine salts or their hydrates and pharmaceutical compositions
WO2008060093A1 (en) Crystalline s-(-)-amlodipine maleic acid salt anhydride and preparation method thereof
KR100878698B1 (en) Crystalline bepotastine metal salt hydrate, preparation method thereof and pharmaceutical composition comprising the same
WO2006133837A2 (en) A process for the preparation of an injectable solution of (2s)-n-(2;6-dimethyl-phenyl)-1-propyl-2-piperidincarboxamide
CA2653333C (en) Zofenopril calcium
JP4319491B2 (en) Amlodipine organic acid salt
US8362263B2 (en) Crystalline S-(−)-amlodipine adipic acid salt anhydrous and preparation method thereof
WO2004026834A1 (en) Crystalline organic acid salt of amlodipine
WO2008069469A1 (en) Crystalline s-(-)-amlodipine camsylate anhydride and preparation method thereof
AU2006251583A1 (en) Process for preparation of isotonic aqueous injection of ropivacaine
WO2008091085A1 (en) Crystalline s-(-)-amlodipine orotate anhydrous and preparation method thereof
KR20040016837A (en) 3-(3-amidinophenyl)-5-[({[1-(1-iminoethyl)-4-piperidyl}amino)methyl]benzoic acid dihydrochloride and process for preparing the same
KR101307712B1 (en) Crystalline hydrate of bepotastine metal salt, method for preparing same and pharmaceutical composition comprising same
KR20040011751A (en) An organic acid salt of amlodipine
WO1993014068A1 (en) Novel salts of a quinolone-carboxylic acid
HK1139073B (en) 5-(2,4-dihydroxy-5-isopropyl-phenyl)-4-(4-morpholin-4-ylmethyl-phenyl)-isoxazole-3-carboxylic acid ethylamide mesylate, hydrates and polymorphs thereof, and formulations comprising these forms
MXPA03007192A (en) Novel benzoylguanidine salt

Legal Events

Date Code Title Description
PUAI Public reference made under article 153(3) epc to a published international application that has entered the european phase

Free format text: ORIGINAL CODE: 0009012

17P Request for examination filed

Effective date: 20071218

AK Designated contracting states

Kind code of ref document: A2

Designated state(s): AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HU IE IS IT LI LT LU LV MC NL PL PT RO SE SI SK TR

DAX Request for extension of the european patent (deleted)
DAX Request for extension of the european patent (deleted)
TPAC Observations by third parties

Free format text: ORIGINAL CODE: EPIDOSNTIPA

17Q First examination report despatched

Effective date: 20101213

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: THE APPLICATION IS DEEMED TO BE WITHDRAWN

18D Application deemed to be withdrawn

Effective date: 20110427