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IT8921929A1 - COMPLEXES OF 4-HYDROXY-2-METHYL-N - 2-PYRIDINYL-2-H, 2-BENZOTHIAZINE-3 CARBOXYAMIDE-1, 1-DIOXIDE WITH CYLODEXTRIN, HAVING ANTI-INFLAMMATORY ACTION, PROCEDURE FOR THEIR PREPARATION AND RELATED PHARMACEUTICAL COMPOSITIONS. - Google Patents

COMPLEXES OF 4-HYDROXY-2-METHYL-N - 2-PYRIDINYL-2-H, 2-BENZOTHIAZINE-3 CARBOXYAMIDE-1, 1-DIOXIDE WITH CYLODEXTRIN, HAVING ANTI-INFLAMMATORY ACTION, PROCEDURE FOR THEIR PREPARATION AND RELATED PHARMACEUTICAL COMPOSITIONS. Download PDF

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IT8921929A1
IT8921929A1 IT1989A21929A IT2192989A IT8921929A1 IT 8921929 A1 IT8921929 A1 IT 8921929A1 IT 1989A21929 A IT1989A21929 A IT 1989A21929A IT 2192989 A IT2192989 A IT 2192989A IT 8921929 A1 IT8921929 A1 IT 8921929A1
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cyclodextrin
complexes
formula
pharmaceutical compositions
compound
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IT1989A21929A
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IT8921929A0 (en
IT1236834B (en
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Laura Puricelli
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Magis Farm Spa
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Description

Domanda di Brevetto per Invenzione Industriale dal titolo: Patent Application for Industrial Invention entitled:

Complessi del 4-idrossi-2-metil-N-2-piridinil-2-H,2-benzotiazina -3-carbossiammide-l,1-diossido con ciclodestrine, aventi azione anti-infiammatoria, procedimento per la loro preparazione e relative composizioni farmaceutiche Complexes of 4-hydroxy-2-methyl-N-2-pyridinyl-2-H, 2-benzothiazine -3-carboxyamide-1,1-dioxide with cyclodextrins, having anti-inflammatory action, process for their preparation and relative compositions pharmaceuticals

RIASSUNTO SUMMARY

I complessi del 4-idrossi-2-metil-N-2-piridinil-2-H,2-benzotiazina -3-carbossiammide-l,1-diossido con ?, ?, ? dimetil-P, isopropil-? ciclodestrine impiegati nella terapia antiinfiammatoria, vengono assorbiti per via orale e per via rettale in quantit? nettamente superiori rispetto al principio attivo tal quale somministrato per le stesse vie. The 4-hydroxy-2-methyl-N-2-pyridinyl-2-H, 2-benzothiazine -3-carboxyamide-1,1-dioxide complexes with?,?,? dimethyl-P, isopropyl-? cyclodextrins used in anti-inflammatory therapy, are absorbed orally and rectally in quantities? significantly higher than the active ingredient as it is administered by the same routes.

DESCRIZIONE DELL' INVENZIONE DESCRIPTION OF THE INVENTION

La presente invenzione riguarda i complessi del 4-idrossi-2-metil-N-2-piridinil-2-H,2-benzotiazina -3-carbossiammide-l,1-diossido con ?, ?, ? , dimetil-?, idrossipropil-? ciclodestrine, il procedimento per la loro preparazione e loro composizioni farmaceutiche. The present invention relates to the 4-hydroxy-2-methyl-N-2-pyridinyl-2-H, 2-benzothiazine -3-carboxyamide-1,1-dioxide complexes with?,?,? , dimethyl- ?, hydroxypropyl-? cyclodextrins, the process for their preparation and their pharmaceutical compositions.

II 4-idrossi-2-metil-N-2-piridinil-2-H,2-benzotiazina ~3~ carbossiamraide-1,1-diossido avente formula (I) II 4-hydroxy-2-methyl-N-2-pyridinyl-2-H, 2-benzothiazine ~ 3 ~ carboxyiamraide-1,1-dioxide having formula (I)

conosciuto in terapia con il nome di Peroxicam ? un composto avente attivit? antiinfiammatoria. Il suddetto principio attivo presenta per? un inconveniente, se somministrato tal quale per via orale, pu? provocare su soggetti sensibili lesioni sulla mucosa gastrointestinale. known in therapy under the name of Peroxicam? a compound having activity? anti-inflammatory. The aforementioned active ingredient presents for? a drawback, if administered as it is orally, can? to cause lesions on the gastrointestinal mucosa on sensitive subjects.

Oggetto della presente invenzione sono i complessi del composto di formula (I) con una ciclodestrina scelta tra ?, ?, y, dimetil?, idrossipropil-? ciclodestrina, preferibilmente dimetil-?, idrossipropil-? ciclodestrina. Object of the present invention are the complexes of the compound of formula (I) with a cyclodextrin selected from?,?, Y, dimethyl ?, hydroxypropyl-? cyclodextrin, preferably dimethyl- ?, hydroxypropyl-? cyclodextrin.

Nei complessi secondo l'invenzione il principio attivo e le ciclodestrina scelta sono presenti preferibilmente in rapporti molecolari compresi tra 1:1 ad 1:4 , particolarmente tra 1:1 ed 1:3. In the complexes according to the invention, the active principle and the selected cyclodextrin are preferably present in molecular ratios ranging from 1: 1 to 1: 4, particularly between 1: 1 and 1: 3.

E' stato infatti soprendentemente trovato che i complessi oggetto della presente invenzione vengono asssorbiti facilmente per via gastrointestinale e per via rettale e sono cos? in grado di fornire alti livelli serici del principio attivo, inoltre se somministrati per via orale, non presentano gli inconvenienti del principio attivo usato tal quale. It has in fact been surprisingly found that the complexes object of the present invention are easily absorbed by the gastrointestinal and rectal routes and are so? able to provide high serum levels of the active principle, moreover if administered orally, they do not have the drawbacks of the active principle used as it is.

Ulteriore oggetto dellla presente invenzione sono pertanto composizioni farmaceutiche aventi attivit? antiinfiammatoria, contenenti come principio attivo i complessi oggetto della presente invenzione, in combinazione con supporti e/o eccipienti farmacologicamente accettabili. A further object of the present invention are therefore pharmaceutical compositions having activity? anti-inflammatory, containing as the active principle the complexes object of the present invention, in combination with pharmacologically acceptable carriers and / or excipients.

Nel trattamento delle malattie artro-reumatiche i complessi oggetto della presente invenzione possono essere somministrati in in dosi scaglionate 2 o 3 volte al giorno in unit? posologiche contenenti ad esempio da 20 a 50 mg. di principio attivo, in combinazione con adatti supporti o eccipienti fisiologicamente accettabili. In the treatment of arthro-rheumatic diseases, the complexes object of the present invention can be administered in staggered doses 2 or 3 times a day in unit? dosage containing for example from 20 to 50 mg. of active principle, in combination with suitable supports or physiologically acceptable excipients.

Le composizioni farmaceutiche oggetto della presente invenzione sono particolarmente adatte per la somministrazione orale e rettale. The pharmaceutical compositions object of the present invention are particularly suitable for oral and rectal administration.

Le suddette composizioni farmaceutiche possono presentarsi per la somministrazione orale in forma solida, come capsule, compresse, confetti e bustine monodosi, oppure in forma liquida come soluzioni o sospensioni pronte o estemporanee. The aforesaid pharmaceutical compositions can be presented for oral administration in solid form, such as capsules, tablets, sugared almonds and single-dose sachets, or in liquid form as ready or extemporaneous solutions or suspensions.

Ulteriore oggetto della presente invenzione ? costituito dalla preparazione dei complessi dell'invenzione, comprendente: Further object of the present invention? consisting of the preparation of the complexes of the invention, comprising:

1) a - si sospende il composto di formula (I) in una soluzione contenente la ciclodestrina scelta si agita la miscela ottenuta preferibilmente a temperature comprese tra 30 e 70?C fino a completa solubilizzazione della sospensione, 1) a - the compound of formula (I) is suspended in a solution containing the selected cyclodextrin the obtained mixture is stirred preferably at temperatures between 30 and 70 ° C until the suspension is completely dissolved,

oppure or

b -il principio attivo di formula (I) previamente disciolto in un solvente organico insolubile in acqua preferibilmente scelto tra: cloroformio, cloruro di metilene, ed acetato di etile, viene miscelato con una soluzione acquosa della ciclodestrina scelta, b - the active principle of formula (I) previously dissolved in an organic solvent insoluble in water, preferably selected from: chloroform, methylene chloride, and ethyl acetate, is mixed with an aqueous solution of the selected cyclodextrin,

2) a - si separa il complesso ottenuto a bassa temperatura, preferibilmente a temperature comprese tra 0 e 5?C, Oppure 2) a - the obtained complex is separated at low temperature, preferably at temperatures between 0 and 5 ° C, Or

b - si separa il complesso per evaporazione dell'acqua, mediante la tecnica della liofilizzazione, o a caldo con l'aiuto del vuoto. b - the complex is separated by evaporation of water, by means of the freeze-drying technique, or by heat with the help of vacuum.

Preferibilmente il processo oggetto della presente invenzione viene condotto impiegando dei rapporti molari di principio attivo /ciclodestrina rispettivamente 1:1, 1:2, 1:3, 1:4. Preferably the process object of the present invention is carried out using molar ratios of active ingredient / cyclodextrin respectively 1: 1, 1: 2, 1: 3, 1: 4.

Vengono riportati i seguenti esempi a scopo illustrativo,ma non limitativo della presente invenzione. The following examples are reported for illustrative but not limitative purposes of the present invention.

ESEMPIO 1 -Complesso Piroxicam/dimetil-?-ciclodestrina 1-1 13-31 S (0.01 moli) di dimetil-?-ciclodestrina si sciolgono in 2 litri di acqua distillata. EXAMPLE 1 - Piroxicam / dimethyl -? - cyclodextrin complex 1-1 13-31 S (0.01 moles) of dimethyl -? - cyclodextrin are dissolved in 2 liters of distilled water.

Si riscalda a 60?C e si aggiungono 3-31 g (O.O1moli)di Piroxicam. The mixture is heated to 60 ° C and 3-31 g (O.O1mol) of Piroxicam are added.

Si agita la miscela di reazione mantenendo la temperatura a 60?C, fino a completa dissoluzione del principio attivo. The reaction mixture is stirred maintaining the temperature at 60 ° C, until complete dissolution of the active principle.

Si raffredda a circa 2*C e si recupera il complesso sottoforma cristallina. It is cooled to about 2 ° C and the complex is recovered in the crystalline form.

Si ottengono 16 g di prodotto contenenti secondo 1'analisi HPLC circa il 20 % di Peroxicam. 16 g of product are obtained, containing about 20% of Peroxicam according to the HPLC analysis.

ESEMPIO 2 Complesso Piroxicam/dimetil-?-ciclodestrina 1-2 26.62 g (0.02 moli) di dimetil-?-ciclodestrina si sciolgono in 2 litri di acqua distillata. EXAMPLE 2 Piroxicam / dimethyl -? - cyclodextrin 1-2 complex 26.62 g (0.02 moles) of dimethyl -? - cyclodextrin are dissolved in 2 liters of distilled water.

Si riscalda a 60?C e si aggiungono 3-31 g (O.Olmoli)di Piroxicam. Si agita la miscela di reazione mantenendo la temperatura a 60?C, fino a completa dissoluzione del principio attivo. It is heated to 60 ° C and 3-31 g (O.Olmoles) of Piroxicam are added. The reaction mixture is stirred maintaining the temperature at 60 ° C, until complete dissolution of the active principle.

Si raffredda e si recupera il complesso per evaporazione dell'acqua con l'aiuto del vuoto a 50?C. The complex is cooled and recovered by evaporation of the water with the help of a vacuum at 50 ° C.

Si ottengono 20 g di prodotto contenenti secondo l'analisi HPLC circa il 16.5% di Peroxicam. 20 g of product are obtained, containing approximately 16.5% of Peroxicam according to the HPLC analysis.

ESEMPIO 3 Complesso Piroxicam/dimetil-?-ciclodestrina 1-3 39.93 B (0.03 moli) di dimetil-?-ciclodestrina vengono sciolti in 2 litri di acqua distillata . EXAMPLE 3 Piroxicam / dimethyl -? - cyclodextrin 1-3 complex 39.93 B (0.03 moles) of dimethyl -? - cyclodextrin are dissolved in 2 liters of distilled water.

Si aggiungono sotto agitazione alla soluzione soluzione acquosa 100 mi di acetato di etile contenenti 3.31 g{0.01 moli) di Piroxicam. 100 ml of ethyl acetate containing 3.31 g (0.01 moles) of Piroxicam are added under stirring to the aqueous solution.

Si agita energicamente la miscela di reazione per 12 ore. The reaction mixture is vigorously stirred for 12 hours.

Si separa la fase organica dalla fase acquosa, e quest'ultima viene portata a secco con l'aiuto del vuoto.Si ottengono 43-20 g di complesso contenente secondo l'analisi HPLC circa il 7.66 % di principio attivo. The organic phase is separated from the aqueous phase, and the latter is brought to dryness with the help of vacuum. 43-20 g of complex are obtained, according to HPLC analysis containing approximately 7.66% of active principle.

ESEMPIO 4-Complesso Piroxicam/idrossipropil-?-ciclodestrina 1-1 Con un procedimento analogo a quello descritto nell'esempio 1, 15.40 g di idrossipropil-?-ciclodestrina (0.01 moli) vengono vengono fatti reagire con 3.31 g (O.Olmoli) di Piroxicam. EXAMPLE 4 - Piroxicam / hydroxypropyl -? - cyclodextrin complex 1-1 With a procedure similar to that described in example 1, 15.40 g of hydroxypropyl -? - cyclodextrin (0.01 moles) are reacted with 3.31 g (O.Olmoles) by Piroxicam.

In questo modo si ottiene il complesso piroxicam/idrossipropil?-ciclodestrino 1-1. In this way the piroxicam / hydroxypropyl? -Cyclodextrin 1-1 complex is obtained.

ESEMPIO 5- Complesso Piroxicam/idrossipropil-?-ciclodestrina 1-2 Con un procedimento analogo a quello descritto nell'esempio 1, 30.8 g (0.02 moli) di idrossipropil-?-ciclodestrina vengono Fatti reagire con 3.31 g (0.01 moli) di Piroxicam. EXAMPLE 5 - Piroxicam / hydroxypropyl -? - cyclodextrin 1-2 complex With a procedure similar to that described in example 1, 30.8 g (0.02 moles) of hydroxypropyl -? - cyclodextrin are reacted with 3.31 g (0.01 moles) of Piroxicam .

In questo modo si ottengono 31-70 g di un complesso con un contenuto, determinato con HPLC, del 10.4 % in peso di Piroxicam. In this way 31-70 g of a complex are obtained with a content, determined by HPLC, of 10.4% by weight of Piroxicam.

ESEMPIO 6 Complesso piroxicam/idrossipropil-?-ciclodestrina 1-3 Con un procedimento analogo a quello descritto nell'esempio 1, 46.2 g (0.02 moli) di idrossipropil-p-ciclodestrina vengono fatti reagire con 3.31 g (0.01 moli) di Piroxicam. EXAMPLE 6 Piroxicam / hydroxypropyl -? - cyclodextrin 1-3 complex With a process similar to that described in example 1, 46.2 g (0.02 moles) of hydroxypropyl-p-cyclodextrin are reacted with 3.31 g (0.01 moles) of Piroxicam.

In questo modo si ottengono circa 46 g di un complesso con un contenuto, determinato con HPLC, del 7.3 % in peso di Piroxicam. ATTIVIT?' INFIAMMATORIA In this way about 46 g of a complex are obtained with a content, determined by HPLC, of 7.3% by weight of Piroxicam. ACTIVITIES? ' INFLAMMATORY

L'attivit? infiammatoria ? stata provata sui ratti aventi un peso corporeo di 150-170 g e sui quali ? stato provocato l'edema da carragenina. The activity? inflammatory? been tested on rats with a body weight of 150-170 g and on which? carrageenan edema was caused.

I risultati dimostrano che l'attivit? antiinfiammatoria dei complessi di dimetil-p-ciclodestrina ed idrossi propil-?ciclodestrina con Piroxicam ? superiore di circa due volte rispetto a quello del piroxicam somministrato in quantit? equivalenti. The results show that the activity? anti-inflammatory of the complexes of dimethyl-p-cyclodextrin and hydroxy propyl-? cyclodextrin with Piroxicam? higher than about twice that of piroxicam administered in quantities? equivalents.

BIODISPONIBILITA' DEI COMPLESSI RISPETTO A QUANTIT? EQUIVALENTI DI PIROXICAM BIOAVAILABILITY OF THE COMPLEX COMPARED TO THE QUANTITY? EQUIVALENTS OF PIROXICAM

La prova viene effettuata sui conigli bianchi del ceppo New Zealand aventi un peso corporeo di 2.5-3 kg. per somministrazione orale di 10 mg/kg di principio attivo. The test is carried out on white rabbits of the New Zealand strain having a body weight of 2.5-3 kg. for oral administration of 10 mg / kg of active ingredient.

I livelli plasmatici di Piroxicam, ottenuti con la somministrazione dei complessi secondo l'invenzione sono di circa 4 volte superiori a quelli del Piroxicam somministrato in quantit? equivalenti. The plasma levels of Piroxicam obtained by administering the complexes according to the invention are approximately 4 times higher than those of Piroxicam administered in quantities. equivalents.

Claims (12)

RIVENDICAZIONI 1. Complessi 4-idrossi-2-metil-N-2-piridinil-2-H,2-benzotiazina -3-carbossiammide-l,1-diossido, avente formula (I) CLAIMS 1. 4-hydroxy-2-methyl-N-2-pyridinyl-2-H, 2-benzothiazine -3-carboxyamide-1,1-dioxide complexes, having formula (I) con una ciclodestrina scelta tra ?, ?, ? dimetil-? , idrossipropil-? ciclodestrina. with a cyclodextrin chosen from?,?,? dimethyl-? , hydroxypropyl-? cyclodextrin. 2. I complessi secondo la rivendicazione 1 dove la ciclodestrina ? dimetil-? o idrossipropil-? ciclodestrina. 2. The complexes according to claim 1 where the cyclodextrin? dimethyl-? or hydroxypropyl-? cyclodextrin. 3. I complessi secondo la rivendicazione 1 dove il composto di formula (I) e la ciclodestrina scelta sono presenti in rapporti molecolari compresi tra 1:1 ed 1:4. 3. The complexes according to claim 1 wherein the compound of formula (I) and the selected cyclodextrin are present in molecular ratios ranging from 1: 1 to 1: 4. 4. I complessi secondo la rivendicazione 3 dove il composto di formula (I) e la ciclodestrina scelta sono present? in rapporti molecolari compresi tra 1:1 ed 1:3- 4. The complexes according to claim 3 where the compound of formula (I) and the selected cyclodextrin are present? in molecular ratios between 1: 1 and 1: 3- 5. Processo per preparare i complessi di formula comprendente i seguenti passaggi: 1) a - si sospende il composto di formula (I) in una soluzione contenente la ciclodestrina scelta si agita la miscela ottenuta, fino a completa solubilizzazione della sospensione, oppure b - il principio attivo di formula (I) previamente disciolto in un solvente organico insolubile in acqua viene miscelato con una soluzione acquosa della ciclodestrina scelta, 2) a - si separa il complesso ottenuto mediante precipitazione a bassa temperatura, oppure b - si separa il complesso per evaporazione dell'acqua, mediante la tecnica della liofilizzazione, o a caldo con l?aiuto del vuoto 5. Process for preparing the formula complexes comprising the following steps: 1) a - the compound of formula (I) is suspended in a solution containing the selected cyclodextrin, the mixture obtained is stirred, until the suspension is completely dissolved, or b - the active principle of formula (I) previously dissolved in an organic solvent insoluble in water is mixed with an aqueous solution of the selected cyclodextrin, 2) a - the complex obtained is separated by precipitation at low temperature, or b - the complex is separated by evaporation of water, by means of the freeze-drying technique, or by heat with the help of vacuum 6. Il processo secondo la rivendicazione 5 dove lo stadio 1-a viene condotto preferibilmente a temperatura compresa tra 30 e 70 ?C. 6. The process according to claim 5 wherein stage 1-a is preferably carried out at a temperature comprised between 30 and 70 ° C. 7. Il processo secondo la rivendicazione 5 dove lo stadio 1-b viene condotto in un solvente organico scelto tra cloroformio, cloruro di metilene, ed acetato di etile. 7. The process according to claim 5 wherein step 1-b is carried out in an organic solvent selected from chloroform, methylene chloride, and ethyl acetate. 8. Il processo secondo la rivendicazione 5 dove lo stadio 2 -a viene condotto a temperature comprese tra 0 e 5?C. 8. The process according to claim 5 wherein stage 2 -a is carried out at temperatures ranging from 0 to 5 ° C. 9? Il processo secondo la rivendicazione 5 dove il composto di formula (I) e la ciclodestrina scelta vengono fatti reagire in rapporti molecolari rispettivamente 1:1, 1:2, 1:3, 1:4. 9? The process according to claim 5 wherein the compound of formula (I) and the selected cyclodextrin are reacted in molecular ratios respectively 1: 1, 1: 2, 1: 3, 1: 4. 10. Composizioni farmaceutiche aventi attivit? antiinfiammatoria,contenenti come principio attivo i complessi secondo la rivendicazione 1 in combinazione con supporti e/o eccipienti farmacologicamente accettabili. 10. Pharmaceutical compositions having activity anti-inflammatory, containing as the active principle the complexes according to claim 1 in combination with pharmacologically acceptable carriers and / or excipients. 11. Le composizioni farmaceutiche secondo la rivendicazione 10, contenenti da 20 a 50 mg di principio attivo. 11. The pharmaceutical compositions according to claim 10, containing from 20 to 50 mg of active principle. 12. Le composizioni farmaceutiche secondo la rivendicazione 10, adatte per la somministrazione orale e rettale. The pharmaceutical compositions according to claim 10, suitable for oral and rectal administration.
IT02192989A 1989-10-05 1989-10-05 Complexes of 4-hydroxy-2-methyl-N-2-piridinyl-2-H,2-benzothiazine-3-carboxamide-1,1-dioxide with cyclodextrin, with anti-inflammatory action, procedure for their preparation and relevant pharmaceutical composition IT1236834B (en)

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IT02192989A IT1236834B (en) 1989-10-05 1989-10-05 Complexes of 4-hydroxy-2-methyl-N-2-piridinyl-2-H,2-benzothiazine-3-carboxamide-1,1-dioxide with cyclodextrin, with anti-inflammatory action, procedure for their preparation and relevant pharmaceutical composition

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IT02192989A IT1236834B (en) 1989-10-05 1989-10-05 Complexes of 4-hydroxy-2-methyl-N-2-piridinyl-2-H,2-benzothiazine-3-carboxamide-1,1-dioxide with cyclodextrin, with anti-inflammatory action, procedure for their preparation and relevant pharmaceutical composition

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