Liu Zhi-Qiang, Gao Ai-Cun, Wang Ya-Jun, Zheng Yu-Guo, Shen Yin-Chu
Institute of Bioengineering, Zhejiang University of Technology, Hangzhou, 310014, Zhejiang, People's Republic of China.
J Ind Microbiol Biotechnol. 2014 Jul;41(7):1145-58. doi: 10.1007/s10295-014-1443-2. Epub 2014 Apr 29.
A gene encoding halohydrin dehalogenase (HHDH) from Agrobacterium tumefaciens CCTCC M 87071 was cloned and expressed in Escherichia coli. To increase activity and stability of HHDH, 14 amino acid residues around the active site and substrate-binding pocket based on the structural analysis and molecular docking were selected as targets for site-directed mutagenesis. The studies showed that the mutant HHDH (Mut-HHDH) enzyme had a more accessible substrate-binding pocket than the wild-type HHDH (Wt-HHDH). Molecular docking revealed that the distance between the substrate and active site was closer in mutant which improved the catalytic activity. The expressed Wt-HHDH and Mut-HHDH were purified and characterized using 1,3-dichloro-2-propanol (1,3-DCP) as substrates. The specific activity of the mutant was enhanced 26-fold and the value of k cat was 18.4-fold as compared to the Wt-HHDH, respectively. The Mut-HHDH showed threefold extension of half-life at 45 °C than that of Wt-HHDH. Therefore it is possible to add 1,3-DCP concentration up to 100 mM and epichlorohydrin (ECH) was produced at a relatively high conversion and yield (59.6 %) using Mut-HHDH as catalyst. This Mut-HHDH could be a potential candidate for the upscale production of ECH.
克隆了来自根癌农杆菌CCTCC M 87071的编码卤代醇脱卤酶(HHDH)的基因,并在大肠杆菌中进行表达。为了提高HHDH的活性和稳定性,基于结构分析和分子对接,选择活性位点和底物结合口袋周围的14个氨基酸残基作为定点诱变的靶点。研究表明,与野生型HHDH(Wt-HHDH)相比,突变型HHDH(Mut-HHDH)酶具有更易接近的底物结合口袋。分子对接显示,突变体中底物与活性位点之间的距离更近,这提高了催化活性。以1,3-二氯-2-丙醇(1,3-DCP)为底物,对表达的Wt-HHDH和Mut-HHDH进行纯化和表征。与Wt-HHDH相比,突变体的比活性提高了26倍,k cat值提高了18.4倍。Mut-HHDH在45℃下的半衰期比Wt-HHDH延长了三倍。因此,有可能将1,3-DCP浓度提高到100 mM,并以Mut-HHDH为催化剂,以相对较高的转化率和产率(59.6%)生产环氧氯丙烷(ECH)。这种Mut-HHDH可能是ECH规模化生产的潜在候选物。