Crystalline pharmaceutical product

Drug – bio-affecting and body treating compositions – Designated organic active ingredient containing – Heterocyclic carbon compounds containing a hetero ring...

Reexamination Certificate

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C540S513000

Reexamination Certificate

active

06335330

ABSTRACT:

FIELD OF THE INVENTION
This invention relates to a crystalline salt form of (S)-7-[(4,4′-bipiperidin- 1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1 ,4-benzodiazepine-2-acetic acid, its preparation and use as a therapeutic substance.
BACKGROUND
The compound (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, given by formula (I), and procedures
for preparing such compound, its trifluoroacetic acid and sodium salts are disclosed in WO 95/18619 (PCT/U.S. Ser. No. 95/00248, SmithKline Beecham Corp.). Since this compound has both a basic and acidic center, it may exist as either an acid addition salt or basic addition salt. If neither an acid nor a basic addition salt is formed, it may exist as an internal salt or zwitterion. This compound is an inhibitor of the GPIIbIIIa (fibrinogen) receptor on platelets and it acts to inhibit platelet aggregation. Thus, the compound is useful for treating such ailments as stroke, myocardial infarction, thrombosis, embolism, and restenosis following angioplasty. The zwitterion and trifluoroacetate salt prepared according to WO 95/18619 possess undesirable characteristics for preparing pharmaceutical formulations of this compound for commercial sale. The zwitterion is hygroscopic and tends to have a variable water content, equilibrating toward a species which takes up about six molar equivalents of water. This may cause difficulty in milling and mixing to create pharmaceutical compositions. The trifluoroacetate salt is not thermally stable for an extended period which impairs its shelf life.
Accordingly, a stable form of the compound which possesses desirable physical characteristics is needed.
SUMMARY OF THE INVENTION
This invention comprises a stable hydrochloride salt of (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid.
In another aspect, this invention comprises a stable pharmaceutical composition of (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride.
In yet another aspect, this invention comprises a method of antagonizing the fibrinogen receptor for preventing or treating diseases wherein platelet aggregation or the binding of ligand to the fibrinogen receptor is a factor.
DETAILED DESCRIPTION
It has now been found that (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid may be prepared as a hydrochloride salt which is crystalline, stable and possesses a consistent water content. Its preparation and physical properties appear to be consistent and reproducible, which make it particularly useful for use in a commercial product.
The present invention provides (S)-7-[(4,4′-bipiperidin- 1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride, formula (I), as a novel material, and, in particular, as a pharmaceutically acceptable form. The material crystallizes preferably with one mole of HCl, and appears to exist in a generally anhydrous form. Although small amounts of water may be detected by Karl Fischer analysis, this is generally less than 1-2% w/w of the drug substance, and it appears to be consistent irrespective of the storage conditions. The hydrochloride does not appear to exist in polymorphic forms, but in a single microcrystalline aggregate form ranging from 10 to 250 microns. Accordingly, the hydrochloride salt form offers significant advantages for bulk material consistency, handling, and formulation. In addition, the hydrochloride salt form exhibits enhanced dissolution and solubility in water.
In a preferred aspect, this invention provides (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride in substantially pure form.
The present invention also provides a process for preparing (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride which comprises forming a solution of (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride and crystallizing the hydrochloride salt from solution by precipitation or recrystallization. The solution may be prepared in any conventional manner, such as by dissolving the (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, or a suitable salt, in a suitable solvent, and adding hydrogen chloride as a gas, or dissolved in a second solvent to the solution. The second solvent may be the same or different from that used in the original solution. Preferably the second solvent will be miscible with the solvent for the benzodiazepine. Water is a useful solvent. Alcohols, especially methanol, ethanol, and isopropanol, are particularly preferred organic solvents for dissolving the hydrochloric acid and making the hydrochloride salt.
The hydrochloride salt may be precipitated from the solution by adding a solvent in which the salt if less soluble than the solvent in which the salt is prepared or by inducing crystallization, for instance by chilling the solution, adding a co-solvent, adding a seed crystal, or merely allowing the solution to stand. Alternatively, the hydrochloride salt may be precipitated by concentrating the solution of the hydrochloride salt, e.g., removing the solvent(s), such as by evaporation. In another alternative, the solvent may be removed, and the residue may be treated with another solvent, or mixture of solvents, to induce crystallization.
Although the process is preferably carried out starting with a solution of the zwitterionic form of (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, the hydrochloride may be prepared using other salts, for instance an acid addition salt, such as the acetate or trifluoroacetate salt, or a basic addition salt, such as an alkali metal (e.g., lithium, sodium or potassium) or organic amine salt.
In one embodiment, the (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid is suspended in water, and titrated with an aqueous solution of hydrochloric acid to a pH of about 2-3. During the addition of acid, the solid dissolves to give a clear solution. It is important to avoid an excess of the acid, about one equivalent is desired, to produce a stable and readily crystallizable salt. Evaporation of the water yields a crude hydrochloride salt which may be recrystallized from an appropriate solvent, such as ethanol to yield a purified hydrochloride salt.
(S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid as a zwitterion may be prepared according to the procedures set forth in WO 95/18619 and WO 97/24336 (PCT/IB96/01502, SmithKline Beecham) which are incorporated herein by reference as though fully set forth.
This invention further provides a pharmaceutical composition which comprises (S)-7-[(4,4′-bipiperidin-1-yl)carbonyl]-2,3,4,5-tetrahydro-4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride and a pharmaceutically acceptable carrier. Accordingly, (S)-7-[(4,4′-bipiperidin- 1 -yl)carbonyl]-2,3,4,5-tetrahydro4-methyl-3-oxo-1H-1,4-benzodiazepine-2-acetic acid, hydrochloride may be used in the manufacture of a medicament. Pharmaceutical compositions may be formulated as a solution or powder for parenteral administration. Powders may be reconstituted by addition of a suitable diluent or other pharmaceutically acceptable carrier prior to use. The liquid formulation may be a buffered, isotonic, aqueous solution. Examples of suitable diluents are normal pyrogen-free water, isotonic saline solut

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