EP0915905A1 - PROCEDE DE PREPARATION DE DERIVES DE 16$g(a)-HYDROXY-ESTRA-1,3,5(10)-TRIENE - Google Patents

PROCEDE DE PREPARATION DE DERIVES DE 16$g(a)-HYDROXY-ESTRA-1,3,5(10)-TRIENE

Info

Publication number
EP0915905A1
EP0915905A1 EP97935517A EP97935517A EP0915905A1 EP 0915905 A1 EP0915905 A1 EP 0915905A1 EP 97935517 A EP97935517 A EP 97935517A EP 97935517 A EP97935517 A EP 97935517A EP 0915905 A1 EP0915905 A1 EP 0915905A1
Authority
EP
European Patent Office
Prior art keywords
estra
derivative
triene
bromine
hydroxy
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Withdrawn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
EP97935517A
Other languages
German (de)
English (en)
Inventor
Helmut HÄUSER
Michael Meyer
Daniel Ramirez
Manuel Morales
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.)
Bayer Pharma AG
Original Assignee
Schering AG
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 Schering AG filed Critical Schering AG
Publication of EP0915905A1 publication Critical patent/EP0915905A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07JSTEROIDS
    • C07J1/00Normal steroids containing carbon, hydrogen, halogen or oxygen, not substituted in position 17 beta by a carbon atom, e.g. estrane, androstane
    • C07J1/0051Estrane derivatives
    • C07J1/0066Estrane derivatives substituted in position 17 beta not substituted in position 17 alfa
    • C07J1/007Estrane derivatives substituted in position 17 beta not substituted in position 17 alfa the substituent being an OH group free esterified or etherified
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07JSTEROIDS
    • C07J1/00Normal steroids containing carbon, hydrogen, halogen or oxygen, not substituted in position 17 beta by a carbon atom, e.g. estrane, androstane
    • C07J1/0051Estrane derivatives
    • C07J1/0059Estrane derivatives substituted in position 17 by a keto group
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07JSTEROIDS
    • C07J13/00Normal steroids containing carbon, hydrogen, halogen or oxygen having a carbon-to-carbon double bond from or to position 17
    • C07J13/005Normal steroids containing carbon, hydrogen, halogen or oxygen having a carbon-to-carbon double bond from or to position 17 with double bond in position 16 (17)
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07JSTEROIDS
    • C07J71/00Steroids in which the cyclopenta(a)hydrophenanthrene skeleton is condensed with a heterocyclic ring
    • C07J71/0005Oxygen-containing hetero ring
    • C07J71/001Oxiranes

Definitions

  • the invention relates to a process for the preparation of 16 ⁇ -hydroxy-estra-l, 3,5 (10) -triene derivatives of the general formula I.
  • R j represents a hydrogen atom, an alkyl group with a maximum of 4 carbon atoms, a benzyl group or an acyl group with a maximum of 8 carbon atoms,
  • X and Y together symbolize an oxo group, or wherein X represents a hydroxy group and Y represents a hydrogen atom, can be prepared by using an estra-1,3,5 (10), 16-tetraene derivative of the general formula II
  • Rj has the meaning given above and R 2 represents an acyl group with a maximum of 8 carbon atoms, converted into a 16 ⁇ , 17 ⁇ -epoxide by means of peracids and cleaved by means of mineral acids or by converting it into the corresponding 16 ⁇ -bromine derivative using a reagent supplying bromine cations and then rearranging the bromine and exchanging it for a hydroxyl group
  • R j has the meaning given above in the presence of a strong, aqueous buffer solution of pH 5-6.5 using sodium borohydride to give the corresponding 3, 16 ⁇ , 17 ⁇ -trihydroxy-estra-1,3,5 (10) -triene derivatives of the general formula I b
  • Estriol (Estra-l, 3,5 (10) -triene-3,16 ⁇ , 17ß-triol) is a naturally occurring estrogen that is also used in numerous pharmaceutical preparations.
  • the invention relates to the reduction of l ⁇ -hydroxy-estra-l, 3,5 (10) -trien-17-one derivatives of the general formula I a by means of sodium borohydride to the 3,16 ⁇ , 17ß-trihydroxy-estra-l , 3,5 (10) -triene derivatives of the general formula I b.
  • this reaction step can only be achieved with good yields of process product if it is carried out in the presence of a strong, aqueous buffer solution with a pH of 5 - 6.5.
  • estrone cannot be reduced with sodium borohydride even in the presence of a strong, aqueous buffer solution with a pH of 5 - 6.5.
  • buffer substances are used to prepare the buffer solutions, provided that the buffer substances are inert to sodium borohydride.
  • buffer substances which are readily biodegradable, such as sodium acetate.
  • the buffer solution should expediently be 0.5 to 15.0 mol of buffer substances (preferably
  • the procedure is such that the required 16 ⁇ -hydroxy-estra-1,3,5 (10), 16-trien-17-one derivative of the formula I a is not isolated, but from an Estra-1,3,5 (10), 16-tetraene derivative of the general formula ⁇ produces a solution of the 16 ⁇ -hydroxy-estra-1,3,5 (10) -triene derivative, which by an appropriate choice of the Reaction required acids and bases and / or by adding salts to a pH value of 5 - 6.5 is buffered.
  • the Estra-1, 3.5 (10), 16-tetraene derivative of the general formula ⁇ is dissolved in a polar organic solvent, such as, for example, a polar ether, and with an aqueous peracid solution such as perbenzoic acid solution or in particular peracetic acid solution.
  • a polar organic solvent such as, for example, a polar ether
  • an aqueous peracid solution such as perbenzoic acid solution or in particular peracetic acid solution.
  • the epoxide obtained is then isolated by concentrating the reaction mixture or precipitating with water, dissolved in a polar solvent and cleaved with a dilute mineral acid such as dilute sulfuric acid.
  • the reaction solution obtained can then, for example, be buffered to a pH of 5.0-6.5 by adding sodium acetate and used for further reaction.
  • the Estra-1,3,5 (10), 16-tetraene derivative of the general formula II is reacted with a bromine cation-providing reagent, such as N-bromosuccinimide, N-bromoacetamide or dibromodimethylhydantoin under the conditions known per se the corresponding 16-bromo compound is converted (Gary J. Matthews et al. "Synthesis of Oxirones, Aziridines and Episulfides" in John Fried et al. "Organic Reactions in Steroid Chemistry", by Norstrand Reinhold Comp., New York et al., 1972, Vol II, p 1 ff).
  • a bromine cation-providing reagent such as N-bromosuccinimide, N-bromoacetamide or dibromodimethylhydantoin
  • the 16 ⁇ -bromine derivative obtained in this way is dissolved in a polar organic solvent and then rearranged with aqueous alkali metal hydroxide solution to give the 16 ⁇ -bromine compound, which is hydrolyzed to the corresponding 16 ⁇ -hydroxy compound.
  • the reaction mixture is prepared and reacted in the same way as the reaction solution described in route A during the preparation.
  • the mixture is then cooled to -3 ° C. and 30 ml of triethylamine are added.
  • the still moist product is dissolved in a mixture of 560 ml of tetrahydrofuran and 240 ml of methanol, 150 ml of 6N aqueous sulfuric acid are added at 25 ° C. and the mixture is stirred at 55 ° C. for 4 hours.
  • Example 2 a) 25.0 g of 3, 17-diacetoxy-estra-1,3,5 (10), 16-tetraene (prepared according to Example 1) are dissolved in 175 ml of isopropanol and spatially at 20 ° C. with 12.5 G
  • Dibromodimethylhydantoin added. The mixture is stirred for a further 2 hours, 0.75 g of p-toluenesulfonic acid is added and the mixture is stirred for a further 30 minutes.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Steroid Compounds (AREA)

Abstract

L'invention concerne un procédé de préparation de dérivés de 16α-hydroxy-estra-1,3,5(10)-triène qui répondent à la formule générale (I), dans laquelle R1 désigne un atome d'hydrogène, un groupe alkyle avec au maximum 4 atomes de carbone, un groupe benzyle ou un groupe acyle avec au maximum 8 atomes de carbone; et X et Y symbolisent ensemble un groupe oxo ou X désigne un groupe hydroxyle et Y un atome d'hydrogène. Ce procédé se caractérise en ce que l'on convertit un dérivé d'estra-1,3,5(10),16-tétraène en 16α,17α-époxyde au moyen de peracides, on clive celui-ci au moyen d'acides minéraux ou on le convertit dans le dérivé correspondant de 16α-brome au moyen d'un réactif qui libère des cations de brome, puis on convertit celui-ci en un dérivé de 16β-brome, on remplace le brome par un groupe hydroxyle et on réduit le cas échéant le dérivé de 16α-hydroxy-1,3,5(10)triène-17-one ainsi obtenu au moyen d'hydrure de bore de sodium en présence d'une forte solution tampon aqueuse d'une valeur de pH comprise entre 5 et 6,5, jusqu'à obtenir le dérivé correspondant de 16α,17β-trihydroxy-estra-1,3,5(10)-triène.
EP97935517A 1996-07-25 1997-07-11 PROCEDE DE PREPARATION DE DERIVES DE 16$g(a)-HYDROXY-ESTRA-1,3,5(10)-TRIENE Withdrawn EP0915905A1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE19631541 1996-07-25
DE1996131541 DE19631541C1 (de) 1996-07-25 1996-07-25 Verfahren zur Herstellung von 16alpha-Hydroxy-estra-1,3,5(10)-trien-Derivaten
PCT/EP1997/003708 WO1998004577A1 (fr) 1996-07-25 1997-07-11 PROCEDE DE PREPARATION DE DERIVES DE 16α-HYDROXY-ESTRA-1,3,5(10)-TRIENE

Publications (1)

Publication Number Publication Date
EP0915905A1 true EP0915905A1 (fr) 1999-05-19

Family

ID=7801803

Family Applications (1)

Application Number Title Priority Date Filing Date
EP97935517A Withdrawn EP0915905A1 (fr) 1996-07-25 1997-07-11 PROCEDE DE PREPARATION DE DERIVES DE 16$g(a)-HYDROXY-ESTRA-1,3,5(10)-TRIENE

Country Status (6)

Country Link
EP (1) EP0915905A1 (fr)
JP (1) JP2000515163A (fr)
AU (1) AU3848297A (fr)
CA (1) CA2260121A1 (fr)
DE (1) DE19631541C1 (fr)
WO (1) WO1998004577A1 (fr)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1149838A1 (fr) * 2000-04-28 2001-10-31 AZIENDE CHIMICHE RIUNITE ANGELINI FRANCESCO A.C.R.A.F. S.p.A. Estriol substantiellement exempt de 16alpha, 17alpha-estra-1,3,5(10)-triène-3,16,17-triol
WO2012032529A1 (fr) 2010-09-08 2012-03-15 Reliance Life Sciences Pvt. Ltd Réduction stéréosélective de l'alpha-hydroxycétone
CN108047295A (zh) * 2017-12-29 2018-05-18 广西万德药业有限公司 雌三醇的高效合成方法

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO9804577A1 *

Also Published As

Publication number Publication date
JP2000515163A (ja) 2000-11-14
AU3848297A (en) 1998-02-20
DE19631541C1 (de) 1997-09-18
CA2260121A1 (fr) 1998-02-05
WO1998004577A1 (fr) 1998-02-05

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