Sato Rina, Itabashi Yutaka, Suzuki Akira, Hatanaka Tadashi, Kuksis Arnis
Graduate School of Fisheries Sciences, Hokkaido University, Hakodate 041-8611, Japan.
Lipids. 2004 Oct;39(10):1019-23. doi: 10.1007/s11745-004-1325-0.
In this study, the effect of temperature on the stereoselectivity of phospholipase D (PLD) toward the two primary hydroxyl groups of glycerol in the transphosphatidylation reaction of phosphatidylcholine to phosphatidylglycerol (PtdGro) was investigated. For this purpose, PLD from bacteria (Streptomyces septatus TH-2, S. halstedii subsp. scabies K6, and Actinomadura sp.) and cabbage were tested. At the reaction temperatures employed (0-60 degrees C), the proportions of the two PtdGro diastereomers, namely, 1,2-dioleoyl-sn-glycero-3-phospho-3'-sn-glycerol (R,R configuration) and 1 ,2-dioleoyl-sn-glycero-3-phospho-1'-sn-glycerol (R,S configuration), which were produced with PLD from Streptomyces TH-2 and Actinomadura sp., changed gradually from 50% R,R and 50% R,S at 50-60 degrees C to 70% R,R and 30% R,S at 0 degrees C. These alterations suggested that the stereoselectivity of the bacterial PLD toward the two primary hydroxyl groups of prochiral glycerol was significantly influenced by reaction temperature. PLD from Streptomyces K6 showed relatively little effect of temperature on stereoselectivity, giving 65-69% R,R in the temperature range of 60-10 degrees C examined. The plots of In ([R,R]/[R,S]) vs. 1/T gave good linear fits for these three bacterial PLD. No temperature effect was observed for cabbage PLD, which gave an almost equimolar mixture of the R,R and R,S diastereomers in the range from 0 to 40 degrees C. The temperature-dependent change in enantiomeric selectivity of the bacterial PLD promises potentially profitable commercial exploitation.
在本研究中,考察了温度对磷脂酶D(PLD)在磷脂酰胆碱向磷脂酰甘油(PtdGro)的转磷脂酰基反应中对甘油两个伯羟基的立体选择性的影响。为此,测试了来自细菌(链霉菌属的链霉菌TH - 2、哈氏链霉菌亚种疥疮链霉菌K6和马杜拉放线菌)和卷心菜的PLD。在所采用的反应温度(0 - 60℃)下,由链霉菌TH - 2和马杜拉放线菌的PLD产生的两种PtdGro非对映异构体,即1,2 - 二油酰 - sn - 甘油 - 3 - 磷酸 - 3'- sn - 甘油(R,R构型)和1,2 - 二油酰 - sn - 甘油 - 3 - 磷酸 - 1'- sn - 甘油(R,S构型)的比例,在50 - 60℃时从50% R,R和50% R,S逐渐变化到0℃时的70% R,R和30% R,S。这些变化表明,细菌PLD对前手性甘油的两个伯羟基的立体选择性受反应温度的显著影响。来自链霉菌K6的PLD在立体选择性上受温度的影响相对较小,在所考察的60 - 10℃温度范围内,R,R的比例为65 - 69%。对于这三种细菌PLD,ln([R,R]/[R,S])对1/T的作图呈现出良好的线性拟合。对于卷心菜PLD未观察到温度效应,在0至40℃范围内,它产生的R,R和R,S非对映异构体几乎是等摩尔混合物。细菌PLD对映体选择性的温度依赖性变化有望带来潜在的商业开发价值。