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Darusentan, HMR-4005, LU-135252

达芦生坦Chemical Name: (+)-2(S)-(4,6-Dimethoxypyrimidin-2-yloxy)-3-methoxy-3,3-diphenylpropionic acid
CAS No. 171714-84-4
项目整合开发状态: Phase II
项目研究机构: Abbott (Originator), Myogen (Originator), Aventis Pharma (Licensee)
合成路线:The condensation of benzophenone (I) with chloroacetic acid methyl ester (II) by means of sodium methoxide in THF gives the epoxide (III),which is treated with methanol/BF3.Et2O,yielding 2-hydroxy-3-methoxy-3,3-diphenylpropionic acid methyl ester (IV).The condensation of (IV) with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) by means of K2CO3 in DMF affords 2-(4,6-dimethoxypyrimidin-2-yloxy)-3-methoxy-3,3-diphenylpropionic acid methyl ester (VI),which is hydrolyzed with NaOH in hot dioxane/water to give the corresponding free acid (VII).Finally,this compound is submitted to optical resolution,affording LU-135252.Optical resolution of (VIII),the free acid derivative of (IV),with (R)-phenylethylamine,L-proline methyl ester,(S)-1-(4-nitrophenyl)ethylamine or (S)-1-(4--chlorophenyl)ethylamine leads to the enantiomerically pure (S)-enatiomer (IX),which by reaction with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) directly affords LU-135252.
📌 参考资料/链接:
参考文献标题:New carboxylic acid derivs.,their preparation and their use
文献作者:Riechers,H.; Klinge,D.; Amberg,W.; Kling,A.; M黮ler,S.; Baumann,E.; Rheinheimer,J.; Vogelbacher,U.J.; Wernet,W.; Unger,L.; Raschack,M.(BASF AG)
参考来源:EP 0785926; JP 1998507190; WO 9611914

📄 详细内容


合成路线:The condensation of benzophenone (I) with chloroacetic acid methyl ester (II) by means of sodium methoxide in THF gives the epoxide (III),which is treated with methanol/BF3.Et2O,yielding 2-hydroxy-3-methoxy-3,3-diphenylpropionic acid methyl ester (IV).The condensation of (IV) with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) by means of K2CO3 in DMF affords 2-(4,6-dimethoxypyrimidin-2-yloxy)-3-methoxy-3,3-diphenylpropionic acid methyl ester (VI),which is hydrolyzed with NaOH in hot dioxane/water to give the corresponding free acid (VII).Finally,this compound is submitted to optical resolution,affording LU-135252.Optical resolution of (VIII),the free acid derivative of (IV),with (R)-phenylethylamine,L-proline methyl ester,(S)-1-(4-nitrophenyl)ethylamine or (S)-1-(4--chlorophenyl)ethylamine leads to the enantiomerically pure (S)-enatiomer (IX),which by reaction with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) directly affords LU-135252.

合成路线:The condensation of benzophenone (I) with methyl 2-chloroacetate (II) by means of NaOMe in THF gives 3,3-diphenyloxirane-2-carboxylic acid methyl ester (III),which by treatment with BF3/Et2O and methanol,followed by optical resolution,yielded the pure enantiomer 2(S)-hydroxy-3-methoxy-3,3-diphenylpropionic acid methyl ester (IV).The condensation of (IV) with 4,6-dimethyl-2-(methylsulfonyl)pyrimidine (V) by means of K2CO3 in DMF affords 2-(4,6-dimethylpyrimidin-2-yloxy)-3-methoxy-3,3-diphenylpropionic acid methyl ester (VI),which is finally hydrolyzed with KOH in hot dioxane to afford the target propionic acid as a racemic mixture.

参考文献标题:Discovery and optimization of a novel class of orally active nonpeptidic endothelin-A receptor antagonists
文献作者:Albrecht,H.-P.; Riechers,H.; Amberg,W.; Baumann,E.; Bernard,H.; Bohm,H.J.; Klinge,D.; Kling,A.; Muller,S.; Raschack,M.; Unger,L.; Walker,N.; Wernet,W.
参考来源:J Med Chem 1996,39(11),2123


合成路线:The condensation of benzophenone (I) with chloroacetic acid methyl ester (II) by means of sodium methoxide in THF gives the epoxide (III),which is treated with methanol/BF3.Et2O,yielding 2-hydroxy-3-methoxy-3,3-diphenylpropionic acid methyl ester (IV).The condensation of (IV) with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) by means of K2CO3 in DMF affords 2-(4,6-dimethoxypyrimidin-2-yloxy)-3-methoxy-3,3-diphenylpropionic acid methyl ester (VI),which is hydrolyzed with NaOH in hot dioxane/water to give the corresponding free acid (VII).Finally,this compound is submitted to optical resolution,affording LU-135252.Optical resolution of (VIII),the free acid derivative of (IV),with (R)-phenylethylamine,L-proline methyl ester,(S)-1-(4-nitrophenyl)ethylamine or (S)-1-(4--chlorophenyl)ethylamine leads to the enantiomerically pure (S)-enatiomer (IX),which by reaction with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) directly affords LU-135252.

参考文献标题:LU-135252
文献作者:Silvestre,J.S.; Sorbera,L.A.; Castar,J.
参考来源:Drugs Fut 1999,24(2),141


合成路线:The condensation of benzophenone (I) with chloroacetic acid methyl ester (II) by means of sodium methoxide in THF gives the epoxide (III),which is treated with methanol/BF3.Et2O,yielding 2-hydroxy-3-methoxy-3,3-diphenylpropionic acid methyl ester (IV).The condensation of (IV) with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) by means of K2CO3 in DMF affords 2-(4,6-dimethoxypyrimidin-2-yloxy)-3-methoxy-3,3-diphenylpropionic acid methyl ester (VI),which is hydrolyzed with NaOH in hot dioxane/water to give the corresponding free acid (VII).Finally,this compound is submitted to optical resolution,affording LU-135252.Optical resolution of (VIII),the free acid derivative of (IV),with (R)-phenylethylamine,L-proline methyl ester,(S)-1-(4-nitrophenyl)ethylamine or (S)-1-(4--chlorophenyl)ethylamine leads to the enantiomerically pure (S)-enatiomer (IX),which by reaction with 4,6-dimethoxy-2-(methylsulfonyl)pyrimidine (V) directly affords LU-135252.

合成路线:A pilot plant process was further developed for the (S)-enantiomer.Darzens condensation of benzophenone (VIII) with methyl chloroacetate gave the glycidic ester (X).Epoxide opening in (X) with trimethylaluminum furnished methyl 2-hydroxy-3,3-diphenylbutyrate (XI),which was hydrolyzed to the corresponding acid (VI) by using KOH in isopropanol.Treatment of the racemic acid (VI) with (S)-1-(4-chlorophenyl)ethylamine (XII) provided the desired (S)-acid salt (XIII).This was finally condensed with 4,6-dimethyl-2-(methylsulfonyl)pyrimidine (XIV) in the presence of lithium amide to yield the title compound.
参考文献标题:Structural similarity and its suprises: Endothelin receptor antagonists - Process research and development report
文献作者:Jansen,R.; et al.
参考来源:Org Process Res Dev 2001,5(1),16


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