Wu Y, Roberts M F
Merkert Chemistry Center, Boston College, Chestnut Hill, Massachusetts 02167, USA.
Biochemistry. 1997 Jul 15;36(28):8514-21. doi: 10.1021/bi970560j.
Large enhancements (maximum of 82-fold in terms of enzyme efficiency, Vmax/Km) of bacterial PI-PLC cyclic phosphodiesterase activity were observed in the presence of organic solvents miscible in water (dimethyl sulfoxide, dimethylformamide, and 2-propanol). In general, organic solvents lowered the Km for myo-inositol 1,2-cyclic phosphate (cIP) and increased Vmax substantially. This kinetic effect was similar to that obtained with phosphatidylcholine micelles and bilayers in an aqueous assay system for cyclic inositol phosphate hydrolysis [Zhou, C., et al. (1997) Biochemistry 36, 347-355]. Solvent properties were examined to determine which ones correlated with the activation of PI-PLC toward cIP in each solvent. Activation correlated best with the solvent polarity as measured by ET(30); no significant correlation was observed with solution surface tension, the bulk dielectric constant (epsilon), 1/epsilon (a measure of the strength of charge interactions), or the Hildebrand solubility parameter. The sigmoidal curve of the enzyme activity versus solvent polarity was consistent with the solvent promoting a transition in the enzyme from a low-activity to a high-activity form. Possible candidates for this change, including enzyme dimerization, helix B/loop stabilization, and dehydration of the active site, are discussed.
在与水混溶的有机溶剂(二甲基亚砜、二甲基甲酰胺和2-丙醇)存在的情况下,观察到细菌磷脂酰肌醇特异性磷脂酶C(PI-PLC)环磷酸二酯酶活性有大幅增强(就酶效率Vmax/Km而言,最高可达82倍)。一般来说,有机溶剂降低了肌醇1,2-环磷酸酯(cIP)的Km,并显著提高了Vmax。这种动力学效应与在用于环磷酸肌醇水解的水性分析系统中,磷脂酰胆碱胶束和双层膜所产生的效应相似[周,C.等人(1997年)《生物化学》36卷,347 - 355页]。研究了溶剂性质,以确定每种溶剂中哪些性质与PI-PLC对cIP的激活相关。激活与通过ET(30)测量的溶剂极性相关性最佳;与溶液表面张力、本体介电常数(ε)、1/ε(电荷相互作用强度的一种度量)或希尔布兰德溶解度参数均未观察到显著相关性。酶活性与溶剂极性的S形曲线与溶剂促使酶从低活性形式转变为高活性形式一致。讨论了这种变化的可能候选因素,包括酶二聚化、螺旋B/环稳定化以及活性位点脱水。