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Squalamine, MSI-1256F(lactate)

角鲨胺Chemical Name: 3beta-[3-(4-Aminobutylamino)propylamino]-7alpha-hydroxy-24(R)-(sulfooxy)-5alpha-cholestane
CAS No. 148717-90-2, 320725-47-1 (lactate)
项目整合开发状态: Phase II
项目研究机构: Genaera (Orphan Drug), Genaera (Originator)
合成路线:Protection of 3-beta-hydroxy-5-cholenic acid (I) with 2,3-dihydropyran in the presence of pyridinium p-toluenesulfonate provided the bis-tetrahydropyranyl derivative (II).Reduction of the tetrahydropyranyl ester group of (II) with LiAlH4 gave alcohol (III),which was further oxidized to aldehyde (IV) under Swern conditions.Addition of isopropylmagnesium bromide to the aldehyde (IV) yielded the secondary alcohol (V).After silylation of alcohol (V) with t-butyldimethylsilyl chloride and imidazole to (VI),the tetrahydropyranyl protecting group was removed under acidic conditions to afford alcohol (VII).This was further esterified with Ac2O in pyridine to provide acetate ester (VIII).

合成路线:Allylic oxidation of (VIII) by means of t-butyl hydroperoxide and chromium hexacarbonyl produced enone (IX).Subsequent Birch reduction of (IX) employing lithium metal in liquid ammonia gave the saturated ketone (X),which was further reduced to alcohol (XI) with K-Selectride in cold THF.Removal of the acetate ester of (XI) was achieved by treatment with NaCN in MeOH,giving diol (XII).The 3-beta hydroxyl group of (XII) was then selectively oxidized to ketone (XIII) under Oppenauer conditions.Ketone (XIII) was converted to the primary amine (XV) via formation of the O-benzyl oxime (XIV),which was reduced by LiAlH4.

合成路线:The condensation between 4-bromobutyronitrile (XVI) and 3-amino-1-propanol (XVII) gave the hydroxy amino nitrile (XVIII),which was further converted to the N,O-bis-tosylated derivative (XIX).Displacement of the tosylate ester group of (XIX) with NaI in boiling acetone afforded the alkyl iodide (XX).Alkylation of amine (XV) with iodide (XX) provided the secondary amine adduct (XXI).The p-toluenesulfonamido group of (XXI) was reductively removed by sodium in liquid ammonia,yielding diamine (XXII).Subsequent nitrile reduction by means of LiAlH4 furnished triamine (XXIII).

合成路线:After protection of triamine (XXIII) as the tris-benzyloxycarbonyl derivative (XXIV),its 7-hydroxyl was acetylated by means of Ac2O and DMAP.Further hydrogenolysis of the benzyloxycarbonyl groups in ethanolic HCl also removed the O-silyl group,yielding (XXV).Treatment of alcohol (XXV) with sulfur trioxide in pyridine generated the pyridinium sulfate salt (XXVI).The 7-acetate ester of (XXVI) was finally hydrolyzed with NaOH to furnish the title compound.

合成路线:Preparation of the key intermediate (XIII) starting from chenodeoxycholic acid (XLIV) was also reported.Diacetylation of (XLIV),followed by selective hydrolysis of diacetate (XLV),gave the C-3 alcohol (XLVI).This was oxidized to dienone (XLVII) following a previously reported procedure.Reduction of (XLVII) by lithium in liquid ammonia yielded the saturated ketone (XLVIII).Protection of the 7-hydroxyl group of (XLVIII) using methoxymethyl chloride,followed by ketalization of the 3-ketone,afforded (XLIX).Side-chain elongation in (XLIX) as in Scheme 20248401a produced (L),which was then deprotected giving (XIII).

合成路线:Alternatively,intermediate (XLVIII) can also be obtained by Oppenauer oxidation of chenodeoxycholic acid (XLIV) to yield ketone (LI),which is further oxidized employing SeO2 to provide conjugate ketone (LII).Birch reduction of (LII) with lithium in liquid ammonia led to the trans-fused A-B ring compound (XLVIII).
📌 参考资料/链接:
参考文献标题:Chemical synthesis of squalamine
文献作者:Moriarty,R.M.; Guo,L.; Tuladhar,S.M.(Genaera Corp.)
参考来源:WO 9419366

📄 详细内容


合成路线:In a further synthetic procedure,ketalization of enone (CV) with ethyleneglycol afforded (CVI).After silylation of the primary alcohol group of (CVI) to (CVII),allylic oxidation by means of tert-butyl hydroperoxide and Cr(CO)6 furnished ketone (CVIII).Catalytic hydrogenation of the double bond of (CVIII) to (CIX),followed by ketone reduction with K-Selectride,gave the C-7 alcohol (CX),which was esterified with benzoyl chloride,yielding benzoate ester (CXI).Subsequent desilylation of (CXI) using tetrabutylammonium fluoride provided (CXII).

合成路线:Alcohol (CXII) was converted to aldehyde (CXIII) either by Swern oxidation or by means of NaOCl and TEMPO.The Horner-Emmons condensation of phosphonate (CXV) (prepared from bromo ketone (CXIV) and triethyl phosphite) with aldehyde (CXIII) furnished the unsaturated ketone (CXVI).Asymmetric reduction of the carbonyl group of (CXVI) was accomplished by means of borane-dimethyl sulfide complex in the presence of (S)-MeCBS,yielding (CXVII).Catalytic hydrogenation of the resultant allylic alcohol (CXVII) afforded (CXVIII).The ethylene ketal group of (CXVIII) was then hydrolyzed under acidic conditions to the ketone (CXIX).

合成路线:Treatment of the OH group of (CXIX) with SO3-pyridine provided sulfate (CXX).The benzoate ester of (CXX) was subsequently hydrolyzed under basic conditions to give (CXXI).Reductive amination of (CXXI) with the cyanodiamine (CXXII) afforded (CXXIII).The cyano group of (CXXIII) was finally reduced to the target amine by catalytic hydrogenation.

参考文献标题:Stereoselective synthesis of 24-hydroxylated cpds.useful for the preparation of aminosterols,vitamin D analogs,and other cpds.
文献作者:Kinney,W.A.; Meckler,H.; Zhang,X.; Lee,N.; Jones,S.; Rao,M.N.; Bulliard,M.(Genaera Corp.)
参考来源:WO 9824800


合成路线:Steroid (CV) was treated with the fungal species Diplodia gossipina to yield the 7-hydroxylated compound (CXXXII) as a fermentation metabolite.Reduction of enone (CXXXII) by lithium in liquid ammonia afforded the saturated ketone (CXXXIII),which was subsequently protected as the ethylene ketal (CXXXIV) by treatment with ethylene glycol and chlorotrimethylsilane.Selective oxidation of the C-22 alcohol group of (CXXXIV) with NaOCl in the presence of TEMPO provided aldehyde (CXXXV).Wadsworth-Emmons condensation of (CXXXV) with phosphonate (CXV) gave enone (CXXXVI).Stereoselective reduction of (CXXXVI) to the 24-(S)-alcohol (CXXXVII) was achieved by treatment with borane-tetrahydrofuran complex in the presence of the chiral catalyst (R)-MeCBS.After catalytic hydrogenation of the double bond of (CXXXVII),the resultant ketal (CXXXVIII) was hydrolyzed to ketone (CXXXIX) under acidic conditions.Sulfation of (CXXXIX) by means of sulfur trioxide-pyridine furnished the key precursor (CXXI),which was then reductively aminated as in the precedent Scheme

参考文献标题:A process for the preparation of 7alpha-hydroxy 3-aminosubstd.sterols using intermediates with an unprotected 7alpha-hydroxy group
文献作者:Kinney,W.A.; Zhang,X.; Michalak,R.(Genaera Corp.)
参考来源:WO 0179255


合成路线:Steroid (CV) was treated with the fungal species Diplodia gossipina to yield the 7-hydroxylated compound (CXXXII) as a fermentation metabolite.Reduction of enone (CXXXII) by lithium in liquid ammonia afforded the saturated ketone (CXXXIII),which was subsequently protected as the ethylene ketal (CXXXIV) by treatment with ethylene glycol and chlorotrimethylsilane.Selective oxidation of the C-22 alcohol group of (CXXXIV) with NaOCl in the presence of TEMPO provided aldehyde (CXXXV).Wadsworth-Emmons condensation of (CXXXV) with phosphonate (CXV) gave enone (CXXXVI).Stereoselective reduction of (CXXXVI) to the 24-(S)-alcohol (CXXXVII) was achieved by treatment with borane-tetrahydrofuran complex in the presence of the chiral catalyst (R)-MeCBS.After catalytic hydrogenation of the double bond of (CXXXVII),the resultant ketal (CXXXVIII) was hydrolyzed to ketone (CXXXIX) under acidic conditions.Sulfation of (CXXXIX) by means of sulfur trioxide-pyridine furnished the key precursor (CXXI),which was then reductively aminated as in the precedent Scheme

参考文献标题:A short formal synthesis of squalamine from a microbial metabolite
文献作者:Kinney,W.A.; Zhang,X.; Williams,J.I.; Johnston,S.; Michalak,R.S.; Deshpande,M.N.; Dostal,L.; Rosazza,J.P.
参考来源:Org Lett 2000,2(19),2921


合成路线:Intermediate (CXXXIX) has been prepared by a new synthetic procedure:The known methyl 3-keto-5-alpha-chenodeoxycholanate (CXL) was protected as the methoxymethyl ether (CXLI) by treatment with dimethoxymethane and P2O5.Further protection of the keto group of (CXLI) as the ethylene ketal (CXLII),followed by reduction with LiAlH4,afforded alcohol (CXLIII).Swern oxidation of alcohol (CXLIII) yielded aldehyde (CXLIV).This was subjected to Wittig condensation with isopropylidene triphenylphosphorane to give olefin (CXLV).Sharpless asymmetric dihydroxylation of olefin (CXLV) furnished the target diol (CXLVI).Selective esterification of the secondary alcohol of (CXLVI) with Ac2O in pyridine gave rise to acetate (CXLVII).

合成路线:The tertiary alcohol group of (CXLVII) was dehydrated to (CXLVIII) upon treatment with methanesulfonyl chloride and triethylamine.Diimide reduction of the olefin double bond of (CXLVIII) produced (CXLIX).The acetate ester of (CXLIX) was further hydrolyzed to alcohol (CL) by methanolic KOH.Then,acidic hydrolysis of the ketal protecting groups of (CL) furnished the key precursor (CXXXIX).

参考文献标题:A new highly stereoselective construction of the sidechain of squalamine through improved Sharpless catalytic asymmetric dihydroxylation
文献作者:Zhou,X.D.; et al.
参考来源:Tetrahedron Lett 2001,42(13),2537


合成路线:In a further synthetic strategy,an azido precursor of spermidine (CXXX) was used in the reductive amination step.Condensation between 1,3-diaminopropane (CXXIV) and 4-chloro-1-butanol (CXXV) provided the diamino alcohol (CXXVI).Protection of the amino groups of (CXXVI) with di-tert-butyl dicarbonate yielded alcohol (CXXVII),which was converted to mesylate (CXXVIII) by treatment with methanesulfonyl chloride and triethylamine.Subsequent mesylate displacement in (CXXVIII) with NaN3 in DMF furnished the di-Boc-protected azide (CXXIX).The Boc protecting groups of (CXXIX) were then removed by treatment with HCl to give the desired diamino azide (CXXX).Reductive amination of the 3-keto steroid (CXXI) with amine (CXXX) yielded the 3-beta amino steroid (CXXXI).The azido group of (CXXXI) was finally reduced to the title triamino compound by catalytic hydrogenation over Raney-Ni.

参考文献标题:Synthesis of an azido spermidine equivalent
文献作者:Weis,A.L.; et al.
参考来源:Tetrahedron Lett 1999,40(26),4863


合成路线:Removal of the Boc and silyl protecting groups of (XLI) was accomplished by treatment with trifluoroacetic acid in chloroform to provide,after chromatographic separation,the 3-alpha-polyamino sterol (XLII).Subsequent catalytic hydrogenation removed the benzyl protecting group of (XLVII),yielding (XLIII).Finally,sulfation of alcohol (XLIII) with sulfur trioxide-pyridine gave rise to the title compound.

合成路线:Alcohol (CXII) was converted to aldehyde (CXIII) either by Swern oxidation or by means of NaOCl and TEMPO.The Horner-Emmons condensation of phosphonate (CXV) (prepared from bromo ketone (CXIV) and triethyl phosphite) with aldehyde (CXIII) furnished the unsaturated ketone (CXVI).Asymmetric reduction of the carbonyl group of (CXVI) was accomplished by means of borane-dimethyl sulfide complex in the presence of (S)-MeCBS,yielding (CXVII).Catalytic hydrogenation of the resultant allylic alcohol (CXVII) afforded (CXVIII).The ethylene ketal group of (CXVIII) was then hydrolyzed under acidic conditions to the ketone (CXIX).

合成路线:Treatment of the OH group of (CXIX) with SO3-pyridine provided sulfate (CXX).The benzoate ester of (CXX) was subsequently hydrolyzed under basic conditions to give (CXXI).Reductive amination of (CXXI) with the cyanodiamine (CXXII) afforded (CXXIII).The cyano group of (CXXIII) was finally reduced to the target amine by catalytic hydrogenation.

参考文献标题:Synthesis of squalamine utilizing a readily accessible spermidine equivalent
文献作者:Zhang,X.; et al.
参考来源:J Org Chem 1998,63(23),8599


产品链接: CAS No. 148717-90-2››

产品链接: CAS No.320725-47-1››