Tsukamoto Takashi, Majer Pavel, Vitharana Dilrukshi, Ni Chiyou, Hin Bunda, Lu Xi-Chun M, Thomas Ajit G, Wozniak Krystyna M, Calvin David C, Wu Ying, Slusher Barbara S, Scarpetti David, Bonneville George W
Guilford Pharmaceuticals Inc., 6611 Tributary Street, Baltimore, Maryland 21224, USA.
J Med Chem. 2005 Apr 7;48(7):2319-24. doi: 10.1021/jm049258g.
Two representative glutamate carboxypeptidase II (GCP II) inhibitors, 2-(hydroxypentafluorophenylmethyl-phosphinoylmethyl)pentanedioic acid 2 and 2-(3-mercaptopropyl)pentanedioic acid 3, were synthesized in high optical purities (>97%ee). The two enantiomers of 2 were prepared from previously reported chiral intermediates, (R)- and (S)-2-(hydroxyphosphinoylmethyl)pentanedioic acid benzyl esters 8. The synthesis of (R)- and (S)-3 involves the hydrolysis of (R)- and (S)-3-(2-oxo-tetrahydro-thiopyran-3-yl)propionic acids, (R)- and (S)-11, the corresponding optically pure thiolactones delivered by chiral chromatographic separation of the racemic 11. GCP II inhibitory assay revealed that (S)-2 is 40-fold more potent than (R)-2. In contrast, both enantiomers of 3 inhibited GCP II with nearly equal potency. The efficacy observed in subsequent animal studies with these enantiomers correlated well with the inhibitory potency in a GCP II assay.
合成了两种具有代表性的谷氨酸羧肽酶II(GCP II)抑制剂,2-(羟基五氟苯基甲基膦酰基甲基)戊二酸2和2-(3-巯基丙基)戊二酸3,其光学纯度均很高(对映体过量>97%)。2的两种对映体由先前报道的手性中间体(R)-和(S)-2-(羟基膦酰基甲基)戊二酸苄酯8制备。(R)-和(S)-3的合成涉及(R)-和(S)-3-(2-氧代-四氢噻喃-3-基)丙酸((R)-和(S)-11)的水解,(R)-和(S)-11是通过外消旋体11的手性色谱分离得到的相应光学纯硫代内酯。GCP II抑制试验表明,(S)-2的活性比(R)-2高40倍。相比之下,3的两种对映体对GCP II的抑制活性几乎相同。随后用这些对映体进行的动物研究中观察到的疗效与GCP II试验中的抑制活性密切相关。