CH531495A - Antiinflammatory pregnene-diones - Google Patents

Antiinflammatory pregnene-diones

Info

Publication number
CH531495A
CH531495A CH860572A CH860572A CH531495A CH 531495 A CH531495 A CH 531495A CH 860572 A CH860572 A CH 860572A CH 860572 A CH860572 A CH 860572A CH 531495 A CH531495 A CH 531495A
Authority
CH
Switzerland
Prior art keywords
beta
pregnene
acid
methylene
dione
Prior art date
Application number
CH860572A
Other languages
German (de)
Inventor
Andor Fuerst
Marcel Mueller
Peter Mueller
Arno Johannes Schocher
Elisabeth Becher
Original Assignee
Hoffmann La Roche
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 Hoffmann La Roche filed Critical Hoffmann La Roche
Priority to CH860572A priority Critical patent/CH531495A/en
Publication of CH531495A publication Critical patent/CH531495A/en

Links

Classifications

    • GPHYSICS
    • G01MEASURING; TESTING
    • G01DMEASURING NOT SPECIALLY ADAPTED FOR A SPECIFIC VARIABLE; ARRANGEMENTS FOR MEASURING TWO OR MORE VARIABLES NOT COVERED IN A SINGLE OTHER SUBCLASS; TARIFF METERING APPARATUS; MEASURING OR TESTING NOT OTHERWISE PROVIDED FOR
    • G01D9/00Recording measured values
    • G01D9/28Producing one or more recordings, each recording being of the values of two or more different variables
    • G01D9/30Producing one or more recordings, each recording being of the values of two or more different variables there being a separate recording element for each variable, e.g. multiple-pen recorder
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07JSTEROIDS
    • C07J53/00Steroids in which the cyclopenta(a)hydrophenanthrene skeleton has been modified by condensation with a carbocyclic rings or by formation of an additional ring by means of a direct link between two ring carbon atoms, including carboxyclic rings fused to the cyclopenta(a)hydrophenanthrene skeleton are included in this class
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07JSTEROIDS
    • C07J75/00Processes for the preparation of steroids in general
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01DMEASURING NOT SPECIALLY ADAPTED FOR A SPECIFIC VARIABLE; ARRANGEMENTS FOR MEASURING TWO OR MORE VARIABLES NOT COVERED IN A SINGLE OTHER SUBCLASS; TARIFF METERING APPARATUS; MEASURING OR TESTING NOT OTHERWISE PROVIDED FOR
    • G01D18/00Testing or calibrating apparatus or arrangements provided for in groups G01D1/00 - G01D15/00
    • GPHYSICS
    • G07CHECKING-DEVICES
    • G07CTIME OR ATTENDANCE REGISTERS; REGISTERING OR INDICATING THE WORKING OF MACHINES; GENERATING RANDOM NUMBERS; VOTING OR LOTTERY APPARATUS; ARRANGEMENTS, SYSTEMS OR APPARATUS FOR CHECKING NOT PROVIDED FOR ELSEWHERE
    • G07C3/00Registering or indicating the condition or the working of machines or other apparatus, other than vehicles
    • G07C3/08Registering or indicating the production of the machine either with or without registering working or idle time
    • G07C3/12Registering or indicating the production of the machine either with or without registering working or idle time in graphical form
    • GPHYSICS
    • G08SIGNALLING
    • G08GTRAFFIC CONTROL SYSTEMS
    • G08G1/00Traffic control systems for road vehicles
    • G08G1/01Detecting movement of traffic to be counted or controlled

Landscapes

  • Physics & Mathematics (AREA)
  • General Physics & Mathematics (AREA)
  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Steroid Compounds (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Preparation Of Compounds By Using Micro-Organisms (AREA)

Abstract

Trihydroxypregnene-3,20-diones (I) and especially 11 beta, 17 alpha, 21-trihydroxy-15, 16 beta-methylene-pregnene (4)-(and pregna-1,4-diene)-3,20-dione, for use as anti-inflammatories. R6 and R9 independently are H, halogen, R17, R21 independently are OH or O-acyl; Z is CO or beta-CH2OH. Preparation of (I) and 1,2-dehydro-deriv. by numerous methods e.g. (a) microbiological 11-hydroxylation of (I) (Z=CH2); (b) 1,2-dehydrogenation of a cmpd. (I); (c) adding HOCl or HOBr to the 9,11-double bond a cmpd. (I) or its, 1,2-dehydro-derivs. (Z = HC). In an example 11 beta, 17 alpha-21-trihydroxy-15,16 beta-methylene-pregnene (4)-3,20-dione, m.p. 219-221 degrees is obtained by microbiological hydroxylation of 17 alpha, 21-dihydroxy-15,16 beta-methylene-pregnene (4)-3,20-dione using Coniothyrium hellebori as organism.

Description

       

  
 



  Verfahren zur Herstellung neuer Steroide der Pregnanreihe
Die Erfindung betrifft ein Verfahren zur   Herstellun]    neuer Steroide der Formel
EMI1.1     
 in der R6 und   R5    unabhängig voneinander Wasserstoff,
Fluor, Chlor oder Brom, R21 Hydroxy oder Acetoxy und Z Carbonyl oder   -Hydroxymethylen    bedeuten.



   Eine Acyloxygruppe enthält vorzugsweise den Rest einer gesättigten oder ungesättigten aliphatischen oder cycloaliphatischen, einer araliphatischen oder aromati schen Carbonsäure mit bis zu 20, vorzugsweise bis zu 12 C-Atomen. Beispiele solcher Säuren sind, Ameisensäure, Essigsäure, Pivalinsäure, Propionsäure, Buttersäure, Capronsäure. Önanthsäure, Ölsäure, Palmitinsäure, Stearinsäure, Bernsteinsäure, Malonsäure, Fumarsäure, Zitronensäure, Cyclohexylpropionsäure, Phenylessigsäure und Benzoesäure.



   Bevorzugte, erfindungsgemäss erhältliche Verbindungen sind diejenigen, in denen R6 und   R5    Wasserstoff oder Fluor, R21   Cl 6-Alkanoyloxy    und Z   9-Hydroxyme-    thylen darstellen.



   Das erfindungsgemässe Verfahren ist dadurch gekennzeichnet, dass man die   17(20)-Doppelbindung    eines Steroids der Formel
EMI1.2     
 oxidiert
Die Oxydation der 17(20)-Doppelbindung einer Ver bindung der Formel II kann beispielsweise mit Oxyda tionsmitteln, wie einem tertiären Amin-N-oxid-peroxid in   tert. -Butanol/Pyridin    in Gegenwart ketalystischer
Mengen Osmiumtetroxid vorgenommen werden. Beispie le von tertiären Amin-N-oxid-peroxiden sind das N-Me   thylmorpholin-N-oxid-peroxid    und das Triäthylaminoxidperoxid. Andererseits kann man mit Oxidationsmitteln wie Osmiumtetroxid oder Permanganat zum 17,20-Glycol oxidieren und letzteres mit Oxidationsmitteln, wie Chromsäure, weiter zum Hydroxyketon oxidieren.



   Zur Herstellung der Ausgangsstoffe kann auf die belgische Patentschrift Nr. 760 392 verwiesen werden.



   Die erfindungsgemäss erhältlichen Steroide sind endocrin, insbesondere anti-inflammatorisch wirksam. Sie können als Heilmittel z.B. in Form pharmazeutischer Präparate Verwendung finden, welche sie in Mischung mit einem für die enterale, perkutane oder parenterale Applikation   -   geeigneten pharmazeutischen, organischen oder anorganischen inerten Trägermaterial enthalten.  



  Die pharmazeutischen Präparate können in fester Form, in halbfester od. in flüssiger Form vorliegen. Gegebenenfalls enthalten sie Hilfsstoffe, wie   Konservierungs-,    Stabilisierungs-, Netz- oder Emulgiermittel, Salze zur Veränderung des osmotischen Druckes oder Puffer. Sie können auch noch andere therapeutisch wertvolle Stoffe enthalten.

 

   Beispiel
Zu einer Mischung von 2,0 g   21-Acetoxy-11ss-hy-    droxy-l5ss,16ss-methylen-pregna-4,17(20)-dien-3-on, 25 ml Methylenchlorid und 60 ml tert. Butanol gab man unter Rühren 4 ml Pyridin, 6,6 ml 1,3 molare N-Methyl-morpholinoxid-peroxid-Lösung und 20 mg Osmiumtetroxid.



  Die Lösung wurde 5 Stunden bei Raumtemperatur gehalten, dann nochmals mit 3,3 ml derselben Oxidationslösung und 10 mg   OSO4    versetzt. Nach weiteren 3 Stunden wurde wie üblich aufgearbeitet. Man erhielt 2,1 g Substanz, die auf Silicagel chromatographiert wurde. Mit Methylenchlorid-Äther 9:1 konnte reines 21-Acetoxy   -l      l7-dihydroxy-l5 1 6 - methylen -    pregn-4-en -3,20 -dion vom Schmelzpunkt   237-239     erhalten werden. 



  
 



  Process for the production of new steroids of the Pregnan range
The invention relates to a process for the production of new steroids of the formula
EMI1.1
 in which R6 and R5 are independently hydrogen,
Fluorine, chlorine or bromine, R21 is hydroxy or acetoxy and Z is carbonyl or hydroxymethylene.



   An acyloxy group preferably contains the remainder of a saturated or unsaturated aliphatic or cycloaliphatic, an araliphatic or aromatic carboxylic acid with up to 20, preferably up to 12, carbon atoms. Examples of such acids are formic acid, acetic acid, pivalic acid, propionic acid, butyric acid, caproic acid. Enanthic acid, oleic acid, palmitic acid, stearic acid, succinic acid, malonic acid, fumaric acid, citric acid, cyclohexylpropionic acid, phenylacetic acid and benzoic acid.



   Preferred compounds obtainable according to the invention are those in which R6 and R5 represent hydrogen or fluorine, R21 represents Cl 6-alkanoyloxy and Z 9-hydroxymethylene.



   The method according to the invention is characterized in that the 17 (20) double bond of a steroid of the formula
EMI1.2
 oxidized
The oxidation of the 17 (20) double bond of a compound of formula II can, for example, with oxidizing agents, such as a tertiary amine-N-oxide peroxide in tert. -Butanol / pyridine in the presence of ketalystic
Amounts of osmium tetroxide can be made. Examples of tertiary amine-N-oxide peroxides are N-methylmorpholine-N-oxide peroxide and triethylamine oxide peroxide. On the other hand, oxidizing agents such as osmium tetroxide or permanganate can be used to oxidize to 17,20-glycol and oxidizing agents such as chromic acid to further oxidize the latter to hydroxyketone.



   For the preparation of the starting materials, reference can be made to Belgian patent specification No. 760 392.



   The steroids obtainable according to the invention are endocrine, in particular anti-inflammatory. They can be used as a remedy e.g. in the form of pharmaceutical preparations which they contain in a mixture with a pharmaceutical, organic or inorganic inert carrier material suitable for enteral, percutaneous or parenteral administration.



  The pharmaceutical preparations can be in solid, semi-solid or liquid form. They may contain auxiliaries, such as preservatives, stabilizers, wetting agents or emulsifiers, salts to change the osmotic pressure or buffers. They can also contain other therapeutically valuable substances.

 

   example
To a mixture of 2.0 g of 21-acetoxy-11ss-hydroxy-l5ss, 16ss-methylen-pregna-4,17 (20) -dien-3-one, 25 ml of methylene chloride and 60 ml of tert. 4 ml of pyridine, 6.6 ml of 1.3 molar N-methylmorpholine oxide peroxide solution and 20 mg of osmium tetroxide were added to butanol with stirring.



  The solution was kept at room temperature for 5 hours, then another 3.3 ml of the same oxidation solution and 10 mg of OSO4 were added. After a further 3 hours, work-up was carried out as usual. 2.1 g of substance were obtained, which was chromatographed on silica gel. With methylene chloride-ether 9: 1 it was possible to obtain pure 21-acetoxy-17-dihydroxy-15 16 -methylene-pregn-4-en -3,20 -dione with a melting point of 237-239.


    

Claims (1)

PATENTANSPRUCH PATENT CLAIM Verfahren zur Herstellung neuer Steroide der Formel EMI2.1 in der R6 und R@ unabhängig voneinander Wasserstoff, Fluor, Chlor oder Brom, R21 Hydroxy oder Acetoxy und Z Carbonyl oder ,8-Hydroxymethylen bedeuten, dadurch gekennzeichnet, dass man die 17(20)-Doppelbindung eines Steroids der Formel EMI2.2 oxidiert. Process for making new steroids of the formula EMI2.1 in which R6 and R @ are independently hydrogen, fluorine, chlorine or bromine, R21 is hydroxy or acetoxy and Z is carbonyl or 8-hydroxymethylene, characterized in that the 17 (20) double bond of a steroid of the formula EMI2.2 oxidized. UNTERANSPRUCH Verfahren nach Patentanspruch, dadurch gekennzeichnet, dass man von Verbindungen der Formel II ausgeht, in denen R6 und R9 Wasserstoff oder Fluor, R21 C1-6-Alkanoyloxy und Z ss-Hydroxymethylen darstellen. SUBClaim Process according to claim, characterized in that one starts from compounds of the formula II in which R6 and R9 are hydrogen or fluorine, R21 is C1-6-alkanoyloxy and Z is ss-hydroxymethylene.
CH860572A 1969-12-17 1970-10-30 Antiinflammatory pregnene-diones CH531495A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CH860572A CH531495A (en) 1969-12-17 1970-10-30 Antiinflammatory pregnene-diones

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CH1883169A CH525872A (en) 1969-12-17 1969-12-17 Process for the production of new steroids of the Pregnan range
CH860572A CH531495A (en) 1969-12-17 1970-10-30 Antiinflammatory pregnene-diones

Publications (1)

Publication Number Publication Date
CH531495A true CH531495A (en) 1972-12-15

Family

ID=4435537

Family Applications (11)

Application Number Title Priority Date Filing Date
CH859972A CH531490A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH1883169A CH525872A (en) 1969-12-17 1969-12-17 Process for the production of new steroids of the Pregnan range
CH860272A CH531492A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860072A CH531491A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH859772A CH531485A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH859872A CH529734A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860472A CH531494A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860172A CH531487A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860372A CH531493A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860672A CH531486A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860572A CH531495A (en) 1969-12-17 1970-10-30 Antiinflammatory pregnene-diones

Family Applications Before (10)

Application Number Title Priority Date Filing Date
CH859972A CH531490A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH1883169A CH525872A (en) 1969-12-17 1969-12-17 Process for the production of new steroids of the Pregnan range
CH860272A CH531492A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860072A CH531491A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH859772A CH531485A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH859872A CH529734A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860472A CH531494A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860172A CH531487A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860372A CH531493A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones
CH860672A CH531486A (en) 1969-12-17 1969-12-17 Antiinflammatory pregnene-diones

Country Status (17)

Country Link
JP (1) JPS4920774B1 (en)
AT (8) AT316772B (en)
BE (1) BE760392A (en)
CA (1) CA955931A (en)
CH (11) CH531490A (en)
DE (1) DE2061183C3 (en)
ES (2) ES386503A1 (en)
FI (1) FI47484C (en)
FR (1) FR2081369B1 (en)
GB (1) GB1276419A (en)
HU (1) HU162802B (en)
IE (1) IE34816B1 (en)
IL (1) IL35790A (en)
NL (1) NL7016761A (en)
NO (1) NO135528C (en)
YU (1) YU34700B (en)
ZA (1) ZA708096B (en)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2740344A (en) * 1951-12-05 1956-04-03 Messrs Lumoprint Zindler K G Device for treating directly exposed photopapers
DE2453823C2 (en) * 1974-11-11 1984-08-09 Schering AG, 1000 Berlin und 4709 Bergkamen 11β, 17α-dihydroxy-15α, 16α-methylene-1,4-pregnadiene-3,20-dione
JPS56109115A (en) * 1980-12-05 1981-08-29 Fukui Kikai Kk Controlling method for feeder for strip material

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3438975A (en) * 1966-07-01 1969-04-15 Syntex Corp 15alpha,16alpha-methylene pregnanes and 19-nor-pregnanes
CH503712A (en) * 1968-04-22 1971-02-28 Hoffmann La Roche Hormone active steroids

Also Published As

Publication number Publication date
ZA708096B (en) 1971-09-29
AT316771B (en) 1974-07-25
ES403723A2 (en) 1975-05-01
AT315396B (en) 1974-05-27
CH531487A (en) 1972-12-15
ES386503A1 (en) 1973-03-16
CH531492A (en) 1972-12-15
FI47484C (en) 1973-12-10
AT316772B (en) 1974-07-25
JPS4920774B1 (en) 1974-05-27
GB1276419A (en) 1972-06-01
NL7016761A (en) 1971-06-21
AT315397B (en) 1974-05-27
FR2081369B1 (en) 1975-04-18
AT316773B (en) 1974-07-25
CA955931A (en) 1974-10-08
YU298070A (en) 1979-07-10
NO135528B (en) 1977-01-10
IL35790A0 (en) 1971-02-25
AT315395B (en) 1974-05-27
DE2061183C3 (en) 1980-01-17
AT308292B (en) 1973-06-25
CH531485A (en) 1972-12-15
DE2061183A1 (en) 1971-06-24
CH531490A (en) 1972-12-15
CH531486A (en) 1972-12-15
CH531491A (en) 1972-12-15
BE760392A (en) 1971-06-16
CH529734A (en) 1972-10-31
HU162802B (en) 1973-04-28
IL35790A (en) 1974-05-16
IE34816B1 (en) 1975-08-20
DE2061183B2 (en) 1979-05-23
YU34700B (en) 1979-12-31
NO135528C (en) 1977-04-20
AT316774B (en) 1974-07-25
IE34816L (en) 1971-06-17
FI47484B (en) 1973-08-31
FR2081369A1 (en) 1971-12-03
CH525872A (en) 1972-07-31
CH531493A (en) 1972-12-15
CH531494A (en) 1972-12-15

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