Sato Rina, Itabashi Yutaka, Hatanaka Tadashi, Kuksis Arnis
Graduate School of Fisheries Sciences, Hokkaido University, Hakodate 041-8611, Japan.
Lipids. 2004 Oct;39(10):1013-8. doi: 10.1007/s11745-004-1324-1.
Using chiral-phase HPLC, we determined the stereochemical configuration of the phosphatidylglycerols (PtdGro) synthesized in vitro from 1,2-diacyl-sn-glycero-3-phosphocholine (PtdCho, R configuration) or 1,2-diacyl-sn-glycero-3-phosphoethanolamine (PtdEtn, R configuration) and glycerol by transphosphatidylation with bacterial phospholipase D (PLD). The results obtained with PLD preparations from three Streptomyces strains (S. septatus TH-2, S. halstedii K5, and S. halstedii subsp. scabies K6) and one Actinomadura species were compared with those obtained using cabbage and peanut PLD. The reaction was carried out at 30 degrees C in a biphasic system consisting of diethyl ether and acetate buffer. The resulting PtdGro were then converted into bis(3,5-dinitrophenylurethane) derivatives, which were separated on an (R)-1-(1-naphthyl)ethylamine polymer. In contrast to the cabbage and peanut PLD, which gave equimolar mixtures of the R,S and R,R diastereomers, as previously established, the bacterial PLD yielded diastereomixtures of 30-40% 1,2-diacyl-sn-glycero-3-phospho-1'-sn-glycerol (R,S configuration) and 60-70% 1,2-diacyl-sn-glycero-3-phospho-3'-sn-glycerol (R,R configuration). The highest disproportionation was found for the Streptomyces K6 species. The present study demonstrates that bacterial PLD-catalyzed transphosphatidylation proceeds to a considerable extent stereoselectively to produce PtdGro from PtdCho or PtdEtn and prochiral glycerol, indicating a preference for the sn-3' position of the glycerol molecule.
我们使用手性相高效液相色谱法,确定了通过细菌磷脂酶D(PLD)的转磷脂酰基作用,由1,2-二酰基-sn-甘油-3-磷酸胆碱(PtdCho,R构型)或1,2-二酰基-sn-甘油-3-磷酸乙醇胺(PtdEtn,R构型)与甘油在体外合成的磷脂酰甘油(PtdGro)的立体化学构型。将来自三种链霉菌菌株(隔孢链霉菌TH-2、哈氏链霉菌K5和哈氏链霉菌疥癣亚种K6)和一种马杜拉放线菌属物种的PLD制剂的实验结果,与使用白菜和花生PLD所获得的结果进行了比较。反应在30℃下于由乙醚和乙酸盐缓冲液组成的双相体系中进行。然后将所得的PtdGro转化为双(3,5-二硝基苯基脲)衍生物,这些衍生物在(R)-1-(1-萘基)乙胺聚合物上进行分离。与先前确定的产生R,S和R,R非对映异构体等摩尔混合物的白菜和花生PLD不同,细菌PLD产生了30 - 40%的1,2-二酰基-sn-甘油-3-磷酸-1'-sn-甘油(R,S构型)和60 - 70%的1,2-二酰基-sn-甘油-3-磷酸-3'-sn-甘油(R,R构型)的非对映异构体混合物。在链霉菌K6物种中发现了最高的歧化作用。本研究表明,细菌PLD催化的转磷脂酰基作用在很大程度上以立体选择性方式进行,从PtdCho或PtdEtn和前手性甘油生成PtdGro,这表明对甘油分子的sn-3'位置具有偏好性。