Huang Ke-xue, Zahn James, Han Lei
Key Lab of Microbial Molecular Biology of Hunan Province, College of Life Science, Hunan Normal University, 410081, Changsha, China.
J Ind Microbiol Biotechnol. 2008 Dec;35(12):1669-76. doi: 10.1007/s10295-008-0431-9. Epub 2008 Aug 14.
Deoxysugar, 2', 3', 4'-tri-O-methylrhamnose is an essential structural component of spinosyn A and D, which are the active ingredients of the commercial insect control agent, Spinosad. The spnH gene, which was previously assigned as a rhamnose O-methyltransferase based on gene sequence homology, was cloned from the wild-type Saccharopolyspora spinosa and from a spinosyn K-producing mutant that was defective in the 4'-O-methylation of 2', 3'-tri-O-methylrhamnose. DNA sequencing confirmed a mutation resulting in an amino acid substitution of G-165 to A-165 in the rhamnosyl 4'-O-methyltransferase of the mutant strain, and the subsequent sequence analysis showed that the mutation occurred in a highly conserved region of the translated amino acid sequence. Both spnH and the gene defective in 4'-O-methylation activity (spnH165A) were expressed heterologously in E. coli and were then purified to homogeneity using a His-tag affinity column. Substrate bioconversion studies showed that the enzyme encoded by spnH, but not spnH165A, could utilize spinosyn K as a substrate. When the wild-type spnH gene was transformed into the spinosyn K-producing mutant, spinosyn A production was restored. These results establish that the enzyme encoded by the spnH gene in wild-type S. spinosa is a rhamnosyl 4'-O-methyltransferase that is responsible for the final rhamnosyl methylation step in the biosynthesis of spinosyn A.
脱氧糖,2',3',4'-三-O-甲基鼠李糖是多杀菌素A和D的必需结构成分,多杀菌素A和D是商业杀虫剂多杀霉素的活性成分。spnH基因先前基于基因序列同源性被指定为鼠李糖O-甲基转移酶,该基因从野生型多刺糖多孢菌以及一个生产多杀菌素K的突变体中克隆得到,该突变体在2',3'-三-O-甲基鼠李糖的4'-O-甲基化过程中存在缺陷。DNA测序证实突变体菌株的鼠李糖基4'-O-甲基转移酶中发生了导致G-165至A-165氨基酸替换的突变,随后的序列分析表明该突变发生在翻译后的氨基酸序列的高度保守区域。spnH和4'-O-甲基化活性缺陷的基因(spnH165A)均在大肠杆菌中进行异源表达,然后使用His标签亲和柱纯化至同质。底物生物转化研究表明,spnH编码的酶而非spnH165A能够利用多杀菌素K作为底物。当将野生型spnH基因转化到生产多杀菌素K的突变体中时,多杀菌素A的产量得以恢复。这些结果表明,野生型多刺糖多孢菌中spnH基因编码的酶是一种鼠李糖基4'-O-甲基转移酶,它负责多杀菌素A生物合成中的最终鼠李糖基甲基化步骤。