Yoneda Aki, Kuo Hsion-Wen David, Ishihara Mayumi, Azadi Parastoo, Yu Su-May, Ho Tuan-hua David
Department of Biology, Washington University in St. Louis, St. Louis, Missouri, United States of America; Department of Pathology and Immunology, School of Medicine, Washington University in St. Louis, St. Louis, Missouri, United States of America.
Department of Environmental Science and Engineering, Tunghai University, Taichung, Taiwan, Republic of China.
PLoS One. 2014 Sep 2;9(9):e106306. doi: 10.1371/journal.pone.0106306. eCollection 2014.
Cellulosic biomass is an abundant and promising energy source. To make cellulosic biofuels competitive against conventional fuels, conversion of rigid plant materials into sugars must become efficient and cost-effective. During cellulose degradation, cellulolytic enzymes generate cellobiose (β-(1→4)-glucose dimer) molecules, which in turn inhibit such enzymes by negative feedback. β-Glucosidases (BGLs) cleave cellobiose into glucose monomers, assisting overall cellulolytic activities. Therefore, BGLs are essential for efficient conversion of cellulosic biomass into biofuels, and it is important to characterize newly isolated BGLs for useful traits. Here, we report our discovery that the indigenous Taiwanese fungus Chaetomella raphigera strain D2 produces two molecular weight variants of a single BGL, D2-BGL (shortened to "D2"), which differ in O-glycosylation. The more extensively O-glycosylated form of native D2 (nD2L) has increased activity toward the natural substrate, cellobiose, compared to the less O-glycosylated form (nD2S). nD2L is more stable at 60°C, in acidic pH, and in the presence of the ionic detergent sodium dodecyl sulfate than nD2S. Furthermore, unlike nD2S, nD2L does not display substrate inhibition by an artificial substrate p-nitrophenyl glucopyranoside (pNPG), and the glucose feedback inhibition kinetics of nD2L is competitive (while it is non-competitive for nD2S), suggesting that these two glycovariants of D2 bind substrates differently. Interestingly, D2 produced in a heterologous system, Pichia pastoris, closely mimics properties of nD2S. Our studies suggest that O-glycosylation of D2 is important in determining its catalytic and biochemical properties.
纤维素生物质是一种丰富且有前景的能源。为使纤维素生物燃料能与传统燃料竞争,将坚硬的植物材料转化为糖的过程必须高效且具成本效益。在纤维素降解过程中,纤维素分解酶会产生纤维二糖(β-(1→4)-葡萄糖二聚体)分子,而这些分子又会通过负反馈抑制此类酶。β-葡萄糖苷酶(BGLs)将纤维二糖裂解为葡萄糖单体,辅助整体纤维素分解活性。因此,BGLs对于将纤维素生物质高效转化为生物燃料至关重要,鉴定新分离的BGLs的有用特性很重要。在此,我们报告我们的发现,即台湾本土真菌嗜热毁丝霉菌株D2产生单一BGL的两种分子量变体,D2-BGL(简称为“D2”),它们在O-糖基化方面存在差异。与O-糖基化程度较低的形式(nD2S)相比,天然D2的O-糖基化程度更高的形式(nD2L)对天然底物纤维二糖的活性有所增加。nD2L在60°C、酸性pH以及存在离子去污剂十二烷基硫酸钠的情况下比nD2S更稳定。此外,与nD2S不同,nD2L不会被人工底物对硝基苯基吡喃葡萄糖苷(pNPG)抑制,并且nD2L的葡萄糖反馈抑制动力学是竞争性的(而nD2S是非竞争性),这表明D2的这两种糖变体结合底物的方式不同。有趣的是,在异源系统毕赤酵母中产生的D2紧密模拟nD2S的特性。我们的研究表明,D2的O-糖基化对于确定其催化和生化特性很重要。