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Freselestat, ONO-PO-736, ONO-6818

5-氨基-N-[1-[[5-(1,1-二甲基乙基)-1,3,4-恶二唑-2-基]羰基]-2-甲基丙基]-6-氧-2-苯基-1(6H)-嘧啶乙酰胺Chemical Name: 2-(5-Amino-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl)-N-[1-(5-tert-butyl-1,3,4-oxadiazol-2-ycarbonyl)-2-methylpropyl]acetamide
CAS No. 208848-19-5
项目整合开发状态: Discontinued
项目研究机构: Ono (Originator)
合成路线:The intermediate oxadiazole (VIII) has been obtained as follows: The reaction of methyl pivalate (I) with refluxing hydrazine hydrate gives the corresponding hydrazide (II),which is cyclized with methyl orthoformate catalyzed by Ts-OH to yield 2-tert-butyl-1,3,4-oxadiazole (III).The condensation of (III) with N2-(tert-butoxycarbonyl)-N1-methoxy-N1-methyl-DL-valinamide (VI) by means of LDA in THF affords the acylated oxadiazole (VII),which is finally deprotected with HCl in ethyl acetate to provide the target intermediate (VIII).

合成路线:The reaction of 3-(2,2-dimethoxyethyl)-2-phenyl-4-oxo-3,4-dihydropyrimidine-5-carboxylic acid (IX) with isobutyl chloroformate and hydroxylamine gives the corresponding hydroxamic acid (X),which is acylated with Ac2O in pyridine to yield the acetoxy compound (XI).The degradation of (XI) by reaction with DBU in refluxing THF affords the amine (XII),which is protected with benzyl chloroformate (XIII) and NaHCO3,providing the carbamate (XIV).The hydrolysis of the dimethylacetal group of (XIV) with HCl in hot acetic acid gives the acetaldehyde derivative (XV),which is oxidized with NaClO2 in tert-butanol/water yielding the corresponding acetic acid derivative (XVI).The condensation of (XVI) with the intermediate amine (VIII) by means of ethyl chloroformate and NMM in THF affords the amide (XVII),which is hydrogenolyzed with H2 over Pd/C in order to eliminate its carbamate protecting group and provide the target racemic 285811.
📌 参考资料/链接:
参考文献标题:1,3,4-Oxadiazole derivs.and process for producing the same
文献作者:Kojima,T.; Hachiya,K.; Ohmoto,K.(Ono Pharmaceutical Co.,Ltd.)
参考来源:EP 1162199; WO 0055145

📄 详细内容


合成路线:The intermediate 2-(5-nitro-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl)acetic acid (IV) has been obtained by several related ways:1.The cyclization of N-(tert-butoxycarbonylmethyl)benzamidine (I) with 3-methoxy-2-nitro-2-propenoic acid methyl ester (II) by means of Na2CO3 gives 2-(5-nitro-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl)acetic acid tert-butyl ester (III),which is hydrolyzed by means of TFA to the target intermediate acid (IV).2.The direct cyclization of N-(carboxymethyl)benzamidine (V) with propenoic ester (II) by means of NaOH gives the target intermediate (IV).3.The cyclization of N-allylbenzamidine (VI) with propenoic ester (II) by means of HCl in methanol gives the allyl pyrimidinone (VII),which is oxidized with NaIO4 and RhCl3 to afford the target intermediate acid (IV).4.The cyclization of N-(2-furylmethyl)benzamidine (VIII) with propenoic ester (II) by means of HCl in toluene/methanol gives the furylmethyl pyrimidinone (IX),with is treated with ozone,NaIO4 and RhCl3 in acetonitrile to yield the target intermediate acid (IV).5.The cyclization of N-(2,2-dimethoxyethyl(benzamidine (X) with propenoic ester (II) in methanol gives the pyrimidinone acetaldehyde dimethylacetal (XI),which is hydrolyzed with TFA to the corresponding aldehyde (XII).Finally,this compound is oxidized with NaClO2 to afford the target intermediate acid (IV).

合成路线:The condensation of intermediate acetic acid (IV) with 2-tert-butyl-5-(DL-valyl)-1,3,4-oxadiazole (XIII) by means of methyl chloroformate and NMM gives the corresponding amide (XIV),which is finally reduced with H2 over Pd/C in MeOH.

参考文献标题:Pyrimidine derivs.,process for preparing the derivs.and drugs containing the same as the active ingredient
文献作者:Okada,T.; Hachiya,K.; Motoi,T.; Kojima,T.; Hashimoto,S.(Ono Pharmaceutical Co.,Ltd.)
参考来源:WO 0123361


合成路线:The reaction of methyl pivalate (I) with hydrazine gives the expected hydrazide (II),which is cyclized with methyl or ethyl orthoformate and Ts-OH,yielding the 2-tert-butyl-1,3,4-oxadiazole (III).The condensation of (III) with N-(tert-butoxycarbonyl)-L-valinal (IV) by means of BuLi and MgBr2 in THF affords the alcohol (V),which is treated with HCl in dioxane to provide the amino alcohol (VI).The condensation of (VI) with 2-[5-(benzyloxycarbonyl)-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl]acetic acid (VII) by means of EDC,HOBT and NMM in DMF gives the corresponding amide (VIII),which is treated with DMP or (COCl)2 in order to oxidize the secondary OH group to the ketone (IX).Finally,this compound is deprotected by means of AlCl3 and anisole or HBr in HOAc to afford the target compound.

参考文献标题:Serine protease inhibitors
文献作者:Spruce,L.W.; Gyorkos,A.(Cortech,Inc.)
参考来源:JP 2001192398; JP 2001507679; WO 9824806


合成路线:The reaction of methyl pivalate (I) with hydrazine gives the expected hydrazide (II),which is cyclized with methyl or ethyl orthoformate and Ts-OH,yielding the 2-tert-butyl-1,3,4-oxadiazole (III).The condensation of (III) with N-(tert-butoxycarbonyl)-L-valinal (IV) by means of BuLi and MgBr2 in THF affords the alcohol (V),which is treated with HCl in dioxane to provide the amino alcohol (VI).The condensation of (VI) with 2-[5-(benzyloxycarbonyl)-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl]acetic acid (VII) by means of EDC,HOBT and NMM in DMF gives the corresponding amide (VIII),which is treated with DMP or (COCl)2 in order to oxidize the secondary OH group to the ketone (IX).Finally,this compound is deprotected by means of AlCl3 and anisole or HBr in HOAc to afford the target compound.

参考文献标题:Design and synthesis of new orally active nonpeptide inhibitors of human neutrophil elastase
文献作者:Ohmoto,K.; Yamamoto,T.; Horiuchi,T.; Imanishi,H.; Odagaki,Y.; Kawabata,K.; Sekioka,T.; Hirota,Y.; Matsuoka,S.; Nakai,H.; Toda,M.; Cheronis,J.C.; Spruce,L.W.; Gyorkos,A.; Wieczorek,M.
参考来源:J Med Chem 2000,43(26),4927


合成路线:The reaction of methyl pivalate (I) with hydrazine gives the expected hydrazide (II),which is cyclized with methyl or ethyl orthoformate and Ts-OH,yielding the 2-tert-butyl-1,3,4-oxadiazole (III).The condensation of (III) with N-(tert-butoxycarbonyl)-L-valinal (IV) by means of BuLi and MgBr2 in THF affords the alcohol (V),which is treated with HCl in dioxane to provide the amino alcohol (VI).The condensation of (VI) with 2-[5-(benzyloxycarbonyl)-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl]acetic acid (VII) by means of EDC,HOBT and NMM in DMF gives the corresponding amide (VIII),which is treated with DMP or (COCl)2 in order to oxidize the secondary OH group to the ketone (IX).Finally,this compound is deprotected by means of AlCl3 and anisole or HBr in HOAc to afford the target compound.

合成路线:The intermediate 2-(5-nitro-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl)acetic acid (IV) has been obtained by several related ways:1.The cyclization of N-(tert-butoxycarbonylmethyl)benzamidine (I) with 3-methoxy-2-nitro-2-propenoic acid methyl ester (II) by means of Na2CO3 gives 2-(5-nitro-6-oxo-2-phenyl-1,6-dihydropyrimidin-1-yl)acetic acid tert-butyl ester (III),which is hydrolyzed by means of TFA to the target intermediate acid (IV).2.The direct cyclization of N-(carboxymethyl)benzamidine (V) with propenoic ester (II) by means of NaOH gives the target intermediate (IV).3.The cyclization of N-allylbenzamidine (VI) with propenoic ester (II) by means of HCl in methanol gives the allyl pyrimidinone (VII),which is oxidized with NaIO4 and RhCl3 to afford the target intermediate acid (IV).4.The cyclization of N-(2-furylmethyl)benzamidine (VIII) with propenoic ester (II) by means of HCl in toluene/methanol gives the furylmethyl pyrimidinone (IX),with is treated with ozone,NaIO4 and RhCl3 in acetonitrile to yield the target intermediate acid (IV).5.The cyclization of N-(2,2-dimethoxyethyl(benzamidine (X) with propenoic ester (II) in methanol gives the pyrimidinone acetaldehyde dimethylacetal (XI),which is hydrolyzed with TFA to the corresponding aldehyde (XII).Finally,this compound is oxidized with NaClO2 to afford the target intermediate acid (IV).

合成路线:The condensation of intermediate acetic acid (IV) with 2-tert-butyl-5-(DL-valyl)-1,3,4-oxadiazole (XIII) by means of methyl chloroformate and NMM gives the corresponding amide (XIV),which is finally reduced with H2 over Pd/C in MeOH.
参考文献标题:Development of orally active nonpeptidic inhibitors of human neutrophil elastase
文献作者:Ohmoto,K.; Yamamoto,T.; Okuma,M.; Horiuchi,T.; Imanishi,H.; Odagaki,Y.; Kawabata,K.; Sekioka,T.; Hirota,Y.; Matsuoka,S.; Nakai,H.; Toda,M.; Cheronis,J.C.; Spruce,L.W.; Gyorkos,A.; Wieczorek,M.
参考来源:J Med Chem 2001,44(8),1268


产品链接: CAS No. 208848-19-5››