Ernholt B V, Thomsen Ib B, Lohse A, Plesner I W, Jensen K B, Hazell R G, Liang X, Jakobsen A, Bols M
Department of Chemistry, Aarhus University, Aarhus C, Denmark.
Chemistry. 2000 Jan;6(2):278-87. doi: 10.1002/(SICI)1521-3765(20000117)6:2<278::AID-CHEM278>3.0.CO;2-6.
For the first time the two enantiomeric forms of the glycosidase inhibitor 1-azafagomine have been synthesised starting from D- and L-xylose. D-Xylose was converted to the 2,3,5-tribenzylfuranose, which upon reductive amination with tert-butyl carbazate gave the protected 1-hydrazino-1-deoxypentitol in high yield. N-acetylation, mesylation of the 4-OH, removal of the Boc group, cyclisation and deprotection gave (+)-1-azafagomine ((+)-1). By a similar sequence of reactions, L-xylose was converted to (-)-1-azafagomine ((-)-1). Enzymatic and other routes to optically pure 1-azafagomine were also studied. Compound (-)-1 is a potent competitive glycosidase inhibitor, while (+)-1 has no biological activity. The inhibition of almond beta-glucosidase by (-)-1 was found to be slow owing to a slow binding step of inhibitor to enzyme, with no subsequent conformational rearrangement. The rate constants for binding and release were found to be 3.3 x 10(4)M(-1)s(-1) and 0.011 s(-1), respectively, yielding Ki = 0.33 microM.
首次从D-木糖和L-木糖出发合成了糖苷酶抑制剂1-氮杂法戈明的两种对映体形式。D-木糖转化为2,3,5-三苄基呋喃糖,其与叔丁基肼进行还原胺化反应,以高产率得到受保护的1-肼基-1-脱氧戊糖醇。N-乙酰化、4-羟基的甲磺酰化、Boc基团的去除、环化和脱保护得到(+)-1-氮杂法戈明((+)-1)。通过类似的反应序列,L-木糖转化为(-)-1-氮杂法戈明((-)-1)。还研究了制备光学纯1-氮杂法戈明的酶促及其他路线。化合物(-)-1是一种有效的竞争性糖苷酶抑制剂,而(+)-1没有生物活性。发现(-)-1对杏仁β-葡萄糖苷酶的抑制作用较慢,这是由于抑制剂与酶的结合步骤较慢,且随后没有构象重排。结合和释放的速率常数分别为3.3×10⁴M⁻¹s⁻¹和0.011 s⁻¹,得出Ki = 0.33 μM。