IL44646A - Pharmaceutical tablet comporising penicillins or cephalosporins - Google Patents

Pharmaceutical tablet comporising penicillins or cephalosporins

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Publication number
IL44646A
IL44646A IL44646A IL4464674A IL44646A IL 44646 A IL44646 A IL 44646A IL 44646 A IL44646 A IL 44646A IL 4464674 A IL4464674 A IL 4464674A IL 44646 A IL44646 A IL 44646A
Authority
IL
Israel
Prior art keywords
tablet
penicillin
magnesium carbonate
heavy magnesium
penicillins
Prior art date
Application number
IL44646A
Other versions
IL44646A0 (en
Original Assignee
Beecham Group 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 Beecham Group Ltd filed Critical Beecham Group Ltd
Publication of IL44646A0 publication Critical patent/IL44646A0/en
Publication of IL44646A publication Critical patent/IL44646A/en

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Classifications

    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K9/00Medicinal preparations characterised by special physical form
    • A61K9/20Pills, tablets, discs, rods
    • A61K9/2072Pills, tablets, discs, rods characterised by shape, structure or size; Tablets with holes, special break lines or identification marks; Partially coated tablets; Disintegrating flat shaped forms
    • A61K9/2077Tablets comprising drug-containing microparticles in a substantial amount of supporting matrix; Multiparticulate tablets
    • A61K9/2081Tablets comprising drug-containing microparticles in a substantial amount of supporting matrix; Multiparticulate tablets with microcapsules or coated microparticles according to A61K9/50
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K31/00Medicinal preparations containing organic active ingredients
    • A61K31/33Heterocyclic compounds
    • A61K31/395Heterocyclic compounds having nitrogen as a ring hetero atom, e.g. guanethidine or rifamycins
    • A61K31/41Heterocyclic compounds having nitrogen as a ring hetero atom, e.g. guanethidine or rifamycins having five-membered rings with two or more ring hetero atoms, at least one of which being nitrogen, e.g. tetrazole
    • A61K31/425Thiazoles
    • A61K31/429Thiazoles condensed with heterocyclic ring systems
    • A61K31/43Compounds containing 4-thia-1-azabicyclo [3.2.0] heptane ring systems, i.e. compounds containing a ring system of the formula, e.g. penicillins, penems
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K9/00Medicinal preparations characterised by special physical form
    • A61K9/20Pills, tablets, discs, rods
    • A61K9/2004Excipients; Inactive ingredients
    • A61K9/2009Inorganic compounds
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61PSPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
    • A61P31/00Antiinfectives, i.e. antibiotics, antiseptics, chemotherapeutics
    • A61P31/04Antibacterial agents

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  • Health & Medical Sciences (AREA)
  • Chemical & Material Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Pharmacology & Pharmacy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Animal Behavior & Ethology (AREA)
  • General Health & Medical Sciences (AREA)
  • Public Health (AREA)
  • Veterinary Medicine (AREA)
  • Epidemiology (AREA)
  • Inorganic Chemistry (AREA)
  • Communicable Diseases (AREA)
  • Oncology (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Nuclear Medicine, Radiotherapy & Molecular Imaging (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Bioinformatics & Cheminformatics (AREA)
  • Medicinal Preparation (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)

Description

D'i'^'S'JB ηι"?»3ΐοη nwn mnpn m' ao Novel pharmaceutical tablets comprising penicillins or cephalosporins BEECEAM GROUP LIMITED C, 42798 This invention relates to pharmaceut cal tablets. More specifically, this invention relates to pharmaceutical tablets containing high proportions of heavy magnesium carbonate. Such novel tablets may be prepared by direct compression.
The dissolution rate of water soluble, sparingly acid soluble medicaments may be increased at low pH by the addition of an agent capable of increasing the pH of the medium. For example, attempts to formulate benzyl enicil lin in tablets containing calcium carbonate have been made in the hone that the partial neutralisation of stomach acids brought about by action of the calcium carbonate would increase the dissolution rate of benzyl-penicillin. Unfortunately, it has not been possible to form a tablet with various other penicillins such as the isoxazolyl-penicillins together with substantial quantities of calcium carbonate without either (a) using a wet granulation process which may result in possible stability problems; (b) including considerable quantities of tab letting aids or (c) reducing the proportion of the penicillin to an unacceptable amount.
We have n∞ found that if heavy mannesium carbonate BP is used as exci ient, then hard tablets of a penicillin or other medicament may be produced that contain a high proportion of penicillin and further, such tablets disperse in stomach acids in a short period. It has also been discovered that these tablets may be prepared by direct compression without the need for inclusion of large amounts of tablettin! aids. This is particularly surprising in view of the comments by Jaffe and Foss, [J. Amer. Pharm. Assoc., Sci. fid., XLVIII, 26 (1959)] that "Those substances containing the carbonate radical show a poor tendency to form tablets upon direct compression". 44646/2 Direct compression which consists essentially of only mixing and compaction stages offers great economies in terms of time, labour, space, equipment and power when compared to the usual methods of tabletting such as wet granulatio or double compression. Magnesium carbonate appears to be unique in that it is a pH modifying agent that is suitable for inclusion in tablets formed by direc compression. Conventional pH modifiers such as sodium citrate, sodium acetate, sodium carbonate, potassium carbonate, calcium citrate or calcium carbonate are not directly compressible.
The discovery that heavy magnesium carbonat BP is a directly compressible buffer, allows for the simplified manufacture of medicament tablets which benefit from the presence of an acidity reducing or disintegration enhancing substance.
Heavy magnesium carbonate is also known as Magnesii Subcarbonas Ponderosus and is a hydrated basic magnesium carbonate of varying composition corresponding approximately to the formula 3MgC03, Mg(OH)2, H20.
Magnesium carbonate per se (i.e. MgCO^] is not sufficiently compressible for use as sole buffer in the compositions of this invention and light magnesium carbonate BP [i.e. 3MgC03, Mg (OH) 21 3H20] hasr.disadvantageous flow characteristics which prevent it from being used as sole buffer in compositions of this invention.
Accordingly the present i invention provides a pharmaceutical tablet which comprises 10-70% of heavy magnesium carbonate, 44646/2 All percentages used herein are on a weight/weight basis.
When used herein the term "penicillin or cephalosporin" means a semi-synthetic penicillin or cephalosporin which is suitable for oral administration.
Suitable conventional tabletting ingredients for use in the tablets of this invention include lubricants, preservatives, dyes, flavours, fillers, binders, solid organic acids and other conventional agents. In mos applications, fillers and binders are no necessary to form acceptable tablets.
Preservatives and dyes are generally present only in very small quantities, for example, usually less tha 1% in total. The quantities of binders, fillers, flavours and the like, depend upon the nature of the medicament, for example, high potency medicaments frequently require the presence of more fillers and the like than do low potency medicaments. Typical fillers include calcium phosphate, sodium sulphate, starch, silica, lactose, dextrose and the like. Typical binders include natural and synthetic resins such as polyvinylpyrollidone, starches and gums such as acacia and tragacanth.
Most suitably, the penicillin or cephalosporin (which may be in th form of a salt or ester) , is sparingly soluble by which it is meant that it is less than 3% soluble in aqueous hydrochloric acid at pH 1.3 at 37°C.
Preferably, such taHets contain 40-60% of a sparingly soluble penicillin or cephalosporin or a salt of ester thereof, 30-60% of heavy magnesium carbonate and 2-10% of conventional tabletting agents. 44646/2 However, if two or more penicillins or cephalosporins are used in the same tablet, it is frequently advantageous to use higher total quantities of antibiotics and lower total quantities of other materials. For example, especially suitable tablets of this sort comprises 60-85% of penicillin or cephalosporin, 10-20% of heavy magnesium carbonate acid and 2-15% of conventional tabletting agents.
One group of useful penicillins suitable for inclusion in the tablets of the invention are the isoxazolyl penicillins and their salts, for example, cloxacillin, flucloxacillin , dicloxacillin and their alkali and alkaline earth metal salts. Tablets containing carbenicillin esters and ticarcillin esters also benefit from the inclusion of heavy magnesium carbonate.
Heavy magnesium carbonate may be advantageously used when an isoxazolyl or other sparingly soluble penicillin is combined in a tablet with another more soluble penicillin.
Suitable penicillins for inclusion in the tablets of this invention include those of the formulae I and II) : (I) 44646/2 wherein R. is a hydrogen, floorine or chlorine atom, R« is a ■ : 1 . ' . · '■ ' £ phenyl or thienyl group and R- is a hydrocarboyl group such as r * phenyl, tola/1 or indanyl; and their alkali and alkaline earth metal salts.
Such compositions may be present together with other penicillins such as ampicillin or amoxycillin or their pivaloyloxymethyl or phthalyl esters.
Other penicillins and cephalosporins which may be included in the tablets of this invention include phenethicillin, propacillin, azldocillin, hetacillin (a form of ampicillin) , metampicillin (a form of ampicillin), cyclacillin, epicillin, pivampicillin, talampicillin, cephalexihnand cephradine.
If desired, the heavy magnesium carbonate may be replaced by a mixture of heavy magnesium carbonate plus other carbonate in which mixture the heavy magnesium carbonate comprises at least half the ingredients present. Suitable other carbonates include CaCO^, NajGO-j, NaHCO^, MgCO^ and the like. Hie preferred other carbonate to be present is CaCO . This preference exists because the presence of Ca 2+ ions counteracts the light laxative properties of the Mg 2+ ions in the, composition. However, there should be at least 8% of heavy magnesium carbonate present in the tablet.
Thus, another aspect of this invention of great usefulness comprises a tablet containing 30-85% of a penicillin or cephalosporin, 10-70% of heavy magnesium carbonate, 2-35% of calcium carbonate and 0-40% of conventional tabletting agents; the weight of heavy magnesium carbonate present in the tablet being The medicament may be microencapsulated or dispersed in a filler prior to inclusion in the tablet.
In some instances, fillers may be added in addition to the heavy magnesium carbonate. Suitable fillers for such tablets include 3tarch, cellulose, urea (as in Belgian patent specification No. 817515) , glycine, calcium phosphate, sodium sulphate and the like. Glycine, urea and calcium carbonate are particularly useful fillers to be used if it is intended to use more than 10% of fillers in addition to the heavy magnesium carbonate.
The tablets of the present invention nay be prepared by blending together, ingredients in conventional manner and compressing the resulting mixture in a tablet press.
Conventional single or multiple punch presses may be used and generally at conventional pressures.
In one of its broadest process aspect, this invention provides a process for the preparation of a pharmaceutical tablet which comprises 10-35% of heavy magnesium carbonate, 5-85% of penicillin or cephalosporin and 0-40% of conventional tablet ingredients and which process comprises the direc 'compression of a mixture of the blended tablet ingredients.
It will be appreciated that the benefits resulting from the use of a direct compression process are very great in tern>3 of saving on labour, time and equipment so that the process of this invention is of considerable commercial usefulness.
Within the scope of this invention is included the preparation of any of the aforesaid tablets by conventional means and particularly by means of direct compression.
The following Examples Illustrate the Invention :- EXAMPLE 1 Sodium CloxacHHn Microencapsulated with 1% Plasdone K29/33 ["Plasdone" (a Registered Trade Hark) 1s comprised of polyvlnyl-py roll done], showed adequate compresslonal characteristics when mixed with 1/2% aerosll (as flow aid), 1 1/2% magnesium stearnte (as lubricant), 4% primojel (as dlslntegrant) and 15% avicel (as compression aid) but the resulting tablets containing 250 mgs. sodium cloxacllUn failed to dissolve at a satisfactory rate at pH * 1.3 [See Table].
However, using heavy magnesium carbonate, the following formulation :- % Sodium CloxacilUn Microcapsules Heavy Magnesium Carbonate Sodium Lauryl Sulphate 1.7 Magnesium Stearate 0.7 Primojel 4.0 was directly compressed at 1200 kg/cm to give tablets of short dissolution time [See Table] and good hardness qualities [14 on Erweka Scale].
Dissolution Rates of 250 mg. Tablets of Example 1 at pH = Ί.3 and 37°C Uhen Measured by a Flask and Stirrer Method at 60 r.p.m.
EXAMPLE 2 Phenethicniin microencapsulated with 1% Plasdone K29/33 was formed into tablets by direct compression at 820 kg/cm . The formulation used was :- % Phenethicillin Microcapsules 49 (= 250 mg. Phenethicillin) Heavy Magnesium Carbonate BP 39 Magnesium Stearate 2 Primojel 8 Sodium Lauryl Sulphate 2 - - S The time for 50% dissolution of the tablets at pH 1. , 3 an 60 r.p.m. stirring was 7 1/2 minutes. In equivalent tablets 1n which the pheneth1c1H1n and magnesium carbonate were replaced by 88% of microencapsulated phenethici llin, the dissolution time under the same conditions was 12 1/2 minutes. The direct compressibility of the two systems was the same.
EXAMPLE 3 Calcium flucloxacilUn was formulated as follows :- % Calcium Flucl oxacillin 52.2 Heavy Magnesium Carbonate 40.8 Sodium Lauryl Sulphate 1.6 Magnesium S tear ate 0.4 Primojel 5.0 This formulation was directly compressible giving hard tablets with a dissolution efficiency (as defined by K.A. Khan and C.T. Rhodes, Pharm. Acta Helv. 47, nage 5941972) of 31%, using a conventional flask and stirrer method at 60 r.p.m., pH 1.2 and 37°C.
[If other buffers e.g. sodium citrate, glycine or calcium carbonate were used In place of the heavy magnesium carbonate, the mixture was no longer directly, compressible. The following formulation was made into tablets using a double compression procedure :- % Calcium FlucloxacilUn 52.1 Sodium Citrate 10.4 Glycine 31.3 Sodium Starch Glycol ate 3.7 Sodium Lauryl Sulphate 1.9 Ma n sium S If a conventional direct compression excipient-di calcium phosphate dihydrate (unir.illed) was used, tablets could be compressed directly . but even with a conventional buffer - sodium citrate, present the · dissolution was still poor e.g. a formulation :- % Calcium FlucloxacllUn ^ 61.8 Sodium Citrate 12.3 Dicaldum Phosphate 18.6 Sodium Lauryl Sulphate 2.2 Prirnojel 4.4 Mannesium Stearate 0.7 had a dissolution efficiency of 3.9% at 100 r.p.m. ].
EXAMPLE 4 Heavy magnesium carbonate BP may be advantageously used in formulations where two penicillins, one sparingly soluble in acid one more soluble, are combined. The presence of heavy magnesium carbonate both greatly improves the tabletting properties of the formulation and increases the dissolution rate of the total penicillin. An example of such a formulation 1s :- Calcium Flucl oxacillin 32 % Amoxycillin 32 % Heavy Magnesium Carbonate 31 % Magnesium Stearate 1 Prirnojel 4 .1' 44646/2 This formulation 1s directly compressible. Any other salt of flucloxacillln, e.g. the sodium, potassium, magnesium or aluminium salt, could replace the calcium salt 1n this formulation, however, the calcium salt is easiest to compress.
EXAMPLE 5 ' In certain combination tablets, the total tablet weight may limit the amount of heavy magnesium carbonate that can be used 1n the formulation. However, In such formulations, the incorporation of 5-20% heavy magnesium carbonate will greatly Improve the tab letting properties and the disintegration/dissolution rates of the formulation.
Examples of such tablets are :- A% B P Sodium CI oxacillin 40 30 33 Ampi ci 11 i n Tri hydrate 40 42 33 Heavy Magnesium Carbonate 12 20 14 Primojel 4 5 4 Sodium Lauryl Sulphate 2 1 2 Magnesium Stearate 2 2 2 Calcium Carbonate 0 0 8 EXAMPLE 6.
The following tablets could be prepared by direct compression : A¾ B¾ Carbenicillin Phenyl Ester Sodium Salt 59 79 Microcrystalline Cellulose 0 15 Λ Heavy Magnesium Carbonate BP 35 0 Magnesium Stearate 1 1 Sodium Lauryl Sulphate 1 1 Primojel 4 Λ Although both formulations produced tablets with acceptable hardnesses, friabilities, etc., tablet Λ had a much faster dissolution rate than tablet B. Increasing the level f microcrystal line cellulose did not improve the dissolution ratr; of tablet B. '.'hen the tablets were given to hyman volunteers, the tablets containing heavy magnesium carbonate produced almost douMe the cumulative urinary nxcretion of penicillins over the first six hours than did tablet B.
The inclusion of other buffers, e.g. glycine, at sufficient concentrations to attain the same cumulative urinary excrstion of penicillins as tablet A, prevented the tablets being made by direct compression. Very friable, capped tablets were produced after a single compression.
These results clearly show the unique properties of heavy magnesium carbonate In being both a pH modifying agent, increasing the bioavailability of sparingly acid soluble drugs and of also being a directly compressible tablotting excipient.
Example 7 The following tablet was prepared by direct compression % Calcium CI oxacil in 50 (= 250 mg. CI oxacillin) Calcium Carbonate 18.5 Heavy Magnesium Carbonate 25 Magnesium Stearate 0.5 Primojel 5.0 Sodium Lauryl Sulphate 1.0 44646

Claims (17)

1. A pharmaceutical tablet which comprises 10-70$ of heavy magnesium carbonate, 30-85$ of penicillin or cephalosporin as hereinbefore defined and 0-40$ of conventional tabletting ingredients.
2. A tablet as in Claim 1 which comprises 40-60$ of a sparingly soluble penicillin or cephalosporin as hereinbefore defined, 30-60$ of heavy magnesium carbonate and 0-10$ of conventional tabletting ingredients.
3. A tablet as in Claims 1 or 2 which comprises 30-85$ of penicillin or cephalosporin, 10-68$ of heavy magnesium carbonate, 2-35$ of calcium carbonate and 0-40$ of conventional tabletting ingredients; the weight of heavy magnesium carbonate present in the tablet being at least as great as the weight of calcium carbonate present.
4. A tablet as in Claim 2 or 3 wherein the penicillin is cloxacillin, flucloxacillin, dicloxacillin or an alkali metal or alkaline earth metal salt thereof.
5. A tablet as in Claim 2 or 3 wherein the penicillin is an a ester of carbenicillin or ticarcillin or an alkali metal or alkaline earth metal salt thereof.
6. A tablet as in Claim 2 or 3 wherein the penicillin or cephalosporin is phenethicillin, propacillin, azidocillin, hetacillin, metampicillin, 44646/3 cyclacillin, epicillin, pivampicillin , talampicillin, cephalexin and cephradine.
7. A tablet as in Claim 2 or 3 in vhich tvo penicillins are present.
8. A tablet as in Claim 7 vhich comprises 60-85 of penicillin, 10-20$ of heavy magnesium carbonate, 2-10$ "of calcium carbonate and 2-15$ of conventional tabletting ingredients.
9. A tablet as. in Claims 7 or 8 vherein one of the penicillins is cloxacillin, flucloxacillin, dicloxacillin or an alkali metal or alkaline earth metal salt, thereof and the other penicillin is ampicillin, amoxycillin, arapicillin pivaloyloxymethyl ester, or a salt thereof or ampicillin phthalyl ester or a salt thereof.
10. A tablet as in Claim 9 vherein one of the penicillins is an alkaline earth metal salt of cloxacillin or flucloxacillin.
11. A tablet as in Claim 10 vherein the second penicillin is ampicillin or amoxycillin.
12. A tablet as in Claim 9 vherein one penicillin is sodium cloxacillin and the other penicillin is -ampicillin.
13. A tablet as in Claim 9 vherein one penicillin is calcium flucloxa-cillin and the other penicillin is amoxycillin. 44646
14. A process for the preparation of a tablet as in any of Claims 1-13 which process comprises the blending of the ingredients followed by compression.
15. A process as in Claim 14 which comprises direct compression.
16. A tablet as in any of Claims 1-13 and substantially as described in any of the Examples herein.
17. A tablet as in any of Claims 1-13 whenever prepared by direct compression.
IL44646A 1973-05-05 1974-04-16 Pharmaceutical tablet comporising penicillins or cephalosporins IL44646A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB2150273A GB1422176A (en) 1973-05-05 1973-05-05 Pharmaceutical tablets
GB5685873 1973-12-07

Publications (2)

Publication Number Publication Date
IL44646A0 IL44646A0 (en) 1974-06-30
IL44646A true IL44646A (en) 1977-04-29

Family

ID=26255363

Family Applications (1)

Application Number Title Priority Date Filing Date
IL44646A IL44646A (en) 1973-05-05 1974-04-16 Pharmaceutical tablet comporising penicillins or cephalosporins

Country Status (10)

Country Link
JP (1) JPS5714649B2 (en)
CA (1) CA1018890A (en)
DE (1) DE2421273A1 (en)
DK (1) DK145712C (en)
FR (1) FR2227856B1 (en)
GB (1) GB1422176A (en)
IE (1) IE39216B1 (en)
IL (1) IL44646A (en)
NL (1) NL7406023A (en)
SE (1) SE402405B (en)

Families Citing this family (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CH647676A5 (en) * 1978-12-22 1985-02-15 Donald E Panoz ORAL, PROGRAM RELEASED GALENIC FORMS AND METHODS OF PREPARING THE SAME.
DE3239592C2 (en) * 1982-10-26 1986-10-30 Institut organičeskogo sinteza Akademii Nauk Latvijskoj SSR, Riga Antibacterial drug
ES2019583B3 (en) * 1985-10-19 1991-07-01 Beecham Group Plc COMPOSITION FOR THE TREATMENT OF INFECTIONS.
US6749864B2 (en) 1986-02-13 2004-06-15 Takeda Chemical Industries, Ltd. Stabilized pharmaceutical composition
CA1327010C (en) * 1986-02-13 1994-02-15 Tadashi Makino Stabilized solid pharmaceutical composition containing antiulcer benzimidazole compound and its production
US5433959A (en) * 1986-02-13 1995-07-18 Takeda Chemical Industries, Ltd. Stabilized pharmaceutical composition
US4743450A (en) * 1987-02-24 1988-05-10 Warner-Lambert Company Stabilized compositions
GB9613470D0 (en) 1996-06-27 1996-08-28 Ciba Geigy Ag Small solid oral dosage form
IS7724A (en) * 2005-03-02 2006-09-03 Actavis Group Composition of tablets with rapid decomposition containing heavy magnesium carbonate
EP1728511A1 (en) * 2005-05-31 2006-12-06 Faust Pharmaceuticals New use of phenethicillin and salts thereof.
WO2011095269A2 (en) * 2010-02-03 2011-08-11 Merck Patent Gmbh Directly compressible magnesium hydroxide carbonate
US20140065220A1 (en) * 2011-03-17 2014-03-06 Kyowa Chemical Industry Co., Ltd. Binder for forming tablets

Also Published As

Publication number Publication date
FR2227856B1 (en) 1978-02-03
DK145712B (en) 1983-02-07
NL7406023A (en) 1974-11-07
SE402405B (en) 1978-07-03
GB1422176A (en) 1976-01-21
IE39216L (en) 1974-11-05
JPS5029732A (en) 1975-03-25
IL44646A0 (en) 1974-06-30
IE39216B1 (en) 1978-08-30
DK145712C (en) 1983-07-25
AU6853574A (en) 1975-11-06
FR2227856A1 (en) 1974-11-29
CA1018890A (en) 1977-10-11
JPS5714649B2 (en) 1982-03-25
DE2421273A1 (en) 1974-11-14

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