School of Chemistry and Life Sciences, Suzhou University of Science and Technology, No. 99 Xuefu Rd., Huqiu District, Suzhou, Jiangsu Province, 215009, People's Republic of China.
Fujian Key Laboratory of Marine Enzyme Engineering, College of Biosciences and Engineering, Fuzhou University, Fuzhou, 350116, People's Republic of China.
Appl Biochem Biotechnol. 2022 Oct;194(10):4852-4866. doi: 10.1007/s12010-022-04015-2. Epub 2022 Jun 7.
L-ribulose, a kind of high-value rare sugar, could be utilized to manufacture L-form sugars and antiviral drugs, generally produced from L-arabinose as a substrate. However, the production of L-ribulose from L-arabinose is limited by the equilibrium ratio of the catalytic reaction, hence, it is necessary to explore a new biological enzymatic method to produce L-ribulose. Ribose-5-phosphate isomerase (Rpi) is an enzyme that can catalyze the reversible isomerization between L-ribose and L-ribulose, which is of great significance for the preparation of L-ribulose. In order to obtain highly active ribose-5-phosphate isomerase to manufacture L-ribulose, ribose-5-phosphate isomerase A (OsRpiA) from Ochrobactrum sp. CSL1 was engineered based on structural and sequence analyses. Through a rational design strategy, a triple-mutant strain A10T/T32S/G101N with 160% activity was acquired. The enzymatic properties of the mutant were systematically investigated, and the optimum conditions were characterized to achieve the maximum yield of L-ribulose. Kinetic analysis clarified that the A10T/T32S/G101N mutant had a stronger affinity for the substrate and increased catalytic efficiency. Furthermore, molecular dynamics simulations indicated that the binding of the substrate to A10T/T32S/G101N was more stable than that of wild type. The shorter distance between the catalytic residues of A10T/T32S/G101N and L-ribose illuminated the increased activity. Overall, the present study provided a solid basis for demonstrating the complex functions of crucial residues in RpiAs as well as in rare sugar preparation.
L-核酮糖,一种高附加值的稀有糖,可用于制造 L 型糖和抗病毒药物,通常以 L-阿拉伯糖为底物生产。然而,L-核酮糖的生产受到催化反应平衡比的限制,因此需要探索一种新的生物酶法来生产 L-核酮糖。核酮糖-5-磷酸异构酶(Rpi)是一种能够催化 L-核糖和 L-核酮糖之间可逆异构化的酶,对 L-核酮糖的制备具有重要意义。为了获得高活性的核酮糖-5-磷酸异构酶来制造 L-核酮糖,根据结构和序列分析对 Ochrobactrum sp. CSL1 的核糖-5-磷酸异构酶 A(OsRpiA)进行了工程改造。通过合理的设计策略,获得了活性提高 160%的三重突变体 A10T/T32S/G101N。系统研究了突变酶的酶学性质,并优化了条件以获得最大的 L-核酮糖产量。动力学分析表明,A10T/T32S/G101N 突变体对底物具有更强的亲和力并提高了催化效率。此外,分子动力学模拟表明,底物与 A10T/T32S/G101N 的结合更稳定。A10T/T32S/G101N 中催化残基之间的距离更短,表明活性增加。总体而言,本研究为阐明 RpiAs 中关键残基在稀有糖制备中的复杂功能提供了坚实的基础。