Department of Bioscience and Biotechnology, Faculty of Agriculture, Kyushu University, 6-10-1 Hakozaki, Fukuoka, 812-8581, Japan.
Department of Biotechnology, The University of Tokyo, 1-1-1 Yayoi, Bunkyo-ku, Tokyo, 113-8657, Japan.
Sci Rep. 2018 Aug 13;8(1):12013. doi: 10.1038/s41598-018-30508-4.
Pyruvyl modification of oligosaccharides is widely seen in both prokaryotes and eukaryotes. Although the biosynthetic mechanisms of pyruvylation have been investigated, enzymes that metabolize and degrade pyruvylated oligosaccharides are not well known. Here, we searched for a pyruvylated galactose (PvGal)-releasing enzyme by screening soil samples. We identified a Bacillus strain, as confirmed by the 16S ribosomal RNA gene analysis, that exhibited PvGal-ase activity toward p-nitrophenyl-β-D-pyruvylated galactopyranose (pNP-β-D-PvGal). Draft genome sequencing of this strain, named HMA207, identified three candidate genes encoding potential PvGal-ases, among which only the recombinant protein encoded by ORF1119 exhibited PvGal-ase activity. Although ORF1119 protein displayed broad substrate specificity for pNP sugars, pNP-β-D-PvGal was the most favorable substrate. The optimum pH for the ORF1119 PvGal-ase was determined as 7.5. A BLAST search suggested that ORF1119 homologs exist widely in bacteria. Among two homologs tested, BglC from Clostridium but not BglH from Bacillus showed PvGal-ase activity. Crystal structural analysis together with point mutation analysis revealed crucial amino acids for PvGal-ase activity. Moreover, ORF1119 protein catalyzed the hydrolysis of PvGal from galactomannan of Schizosaccharomyces pombe, suggesting that natural polysaccharides might be substrates of the PvGal-ase. This novel PvGal-catalyzing enzyme might be useful for glycoengineering projects to produce new oligosaccharide structures.
寡糖的丙酮酸修饰广泛存在于原核生物和真核生物中。虽然丙酮酸化的生物合成机制已经被研究过,但代谢和降解丙酮酸化寡糖的酶还不是很清楚。在这里,我们通过筛选土壤样本寻找一种丙酮酸化半乳糖(PvGal)释放酶。我们鉴定了一株芽孢杆菌,通过 16S 核糖体 RNA 基因分析证实,该菌对 p-硝基苯-β-D-丙酮酸半乳糖(pNP-β-D-PvGal)具有 PvGal-ase 活性。将该菌株命名为 HMA207,对其进行了全基因组测序,鉴定出三个编码潜在 PvGal-ase 的候选基因,其中只有 ORF1119 编码的重组蛋白表现出 PvGal-ase 活性。虽然 ORF1119 蛋白对 pNP 糖显示出广泛的底物特异性,但 pNP-β-D-PvGal 是最理想的底物。ORF1119 PvGal-ase 的最适 pH 值为 7.5。BLAST 搜索表明,ORF1119 同源物广泛存在于细菌中。在测试的两个同源物中,来自梭状芽孢杆菌的 BglC 而不是来自芽孢杆菌的 BglH 表现出 PvGal-ase 活性。晶体结构分析和定点突变分析揭示了 PvGal-ase 活性的关键氨基酸。此外,ORF1119 蛋白催化了来自裂殖酵母半乳甘露聚糖的 PvGal 的水解,表明天然多糖可能是 PvGal-ase 的底物。这种新型的 PvGal 催化酶可能在糖工程项目中用于生产新的寡糖结构。