Center for Natural Products Research, Chengdu Institute of Biology, Chinese Academy of Sciences, Chengdu, 610041, People's Republic of China.
University of Chinese Academy of Sciences, Beijing, 100049, People's Republic of China.
J Ind Microbiol Biotechnol. 2016 Sep;43(9):1281-92. doi: 10.1007/s10295-016-1802-2. Epub 2016 Jun 27.
Geraniol synthase (GES) catalyzes the conversion of geranyl diphosphate (GPP) into geraniol, an acyclic monoterpene alcohol that has been widely used in many industries. Here we report the functional characterization of CaGES from Camptotheca acuminata, a camptothecin-producing plant, and its application in production of geraniol in Escherichia coli. The full-length cDNA of CaGES was obtained from overlap extension PCR amplification. The intact and N-terminus-truncated CaGESs were overexpressed in E. coli and purified to homogeneity. Recombinant CaGES showed the conversion activity from GPP to geraniol. To produce geraniol in E. coli using tCaGES, the biosynthetic precursor GPP should be supplied and transferred to the catalytic pocket of tCaGES. Thus, ispA(S80F), a mutant of farnesyl diphosphate (FPP) synthase, was prepared to produce GPP via the head-to-tail condensation of isoprenyl diphosphate (IPP) and dimethylallyl diphosphate (DMAPP). A slight increase of geraniol production was observed in the fermentation broth of the recombinant E. coli harboring tCaGES and ispA(S80F). To enhance the supply of IPP and DMAPP, the encoding genes involved in the whole mevalonic acid biosynthetic pathway were introduced to the E. coli harboring tCaGES and the ispA(S80F) and a significant increase of geraniol yield was observed. The geraniol production was enhanced to 5.85 ± 0.46 mg L(-1) when another copy of ispA(S80F) was introduced to the above recombinant strain. The following optimization of medium composition, fermentation time, and addition of metal ions led to the geraniol production of 48.5 ± 0.9 mg L(-1). The present study will be helpful to uncover the biosynthetic enigma of camptothecin and tCaGES will be an alternative to selectively produce geraniol in E. coli with other metabolic engineering approaches.
香叶醇合酶(GES)催化香叶基二磷酸(GPP)转化为香叶醇,这是一种环状单萜醇,已广泛应用于许多行业。在这里,我们报告了来自喜树 Camptotheca acuminata 的 CaGES 的功能特征,喜树是一种喜树碱生产植物,及其在大肠杆菌中生产香叶醇的应用。通过重叠延伸 PCR 扩增获得 CaGES 的全长 cDNA。完整和 N 端截断的 CaGES 在大肠杆菌中过表达并均一纯化。重组 CaGES 显示出从 GPP 转化为香叶醇的转化活性。为了在大肠杆菌中使用 tCaGES 生产香叶醇,应该提供生物合成前体 GPP 并将其转移到 tCaGES 的催化口袋中。因此,制备了 FPP 合酶的突变体 ispA(S80F),通过异戊烯二磷酸(IPP)和二甲基烯丙基二磷酸(DMAPP)的头尾缩合来生产 GPP。在含有 tCaGES 和 ispA(S80F)的重组大肠杆菌发酵液中观察到香叶醇产量略有增加。为了增加 IPP 和 DMAPP 的供应,引入了参与整个甲羟戊酸生物合成途径的编码基因到含有 tCaGES 和 ispA(S80F)的大肠杆菌中,观察到香叶醇产量显著增加。当将另一个 ispA(S80F)拷贝引入上述重组菌株时,香叶醇的产量提高到 5.85 ± 0.46 mg L(-1)。进一步优化培养基组成、发酵时间和添加金属离子,导致香叶醇产量达到 48.5 ± 0.9 mg L(-1)。本研究将有助于揭示喜树碱的生物合成奥秘,并且 tCaGES 将成为其他代谢工程方法在大肠杆菌中选择性生产香叶醇的替代方法。