Moscow Institute of Physics and Technology, Dolgoprudny, Russia.
Groningen Biomolecular Sciences and Biotechnology Institute, University of Groningen, Groningen, The Netherlands.
Sci Rep. 2023 Apr 24;13(1):6641. doi: 10.1038/s41598-023-32459-x.
Destabilase from the medical leech Hirudo medicinalis belongs to the family of i-type lysozymes. It has two different enzymatic activities: microbial cell walls destruction (muramidase activity), and dissolution of the stabilized fibrin (isopeptidase activity). Both activities are known to be inhibited by sodium chloride at near physiological concentrations, but the structural basis remains unknown. Here we present two crystal structures of destabilase, including a 1.1 Å-resolution structure in complex with sodium ion. Our structures reveal the location of sodium ion between Glu34/Asp46 residues, which were previously recognized as a glycosidase active site. While sodium coordination with these amino acids may explain inhibition of the muramidase activity, its influence on previously suggested Ser49/Lys58 isopeptidase activity dyad is unclear. We revise the Ser49/Lys58 hypothesis and compare sequences of i-type lysozymes with confirmed destabilase activity. We suggest that the general base for the isopeptidase activity is His112 rather than Lys58. pKa calculations of these amino acids, assessed through the 1 μs molecular dynamics simulation, confirm the hypothesis. Our findings highlight the ambiguity of destabilase catalytic residues identification and build foundations for further research of structure-activity relationship of isopeptidase activity as well as structure-based protein design for potential anticoagulant drug development.
来自医用水蛭 Hirudo medicinalis 的降解酶属于 I 型溶菌酶家族。它具有两种不同的酶活性:破坏微生物细胞壁(噬菌酶活性)和溶解稳定的纤维蛋白(异肽酶活性)。已知这两种活性都被接近生理浓度的氯化钠抑制,但结构基础仍不清楚。在这里,我们展示了两种降解酶的晶体结构,包括一个分辨率为 1.1Å 的与钠离子复合物结构。我们的结构揭示了钠离子位于 Glu34/Asp46 残基之间的位置,这些残基之前被认为是糖苷酶的活性位点。虽然钠离子与这些氨基酸的配位可能解释了噬菌酶活性的抑制,但它对先前提出的 Ser49/Lys58 异肽酶活性偶联的影响尚不清楚。我们修正了 Ser49/Lys58 假说,并比较了具有确定降解酶活性的 I 型溶菌酶序列。我们认为异肽酶活性的通用碱是 His112,而不是 Lys58。通过 1μs 分子动力学模拟评估这些氨基酸的 pKa 值,证实了这一假设。我们的研究结果强调了降解酶催化残基鉴定的模糊性,并为进一步研究异肽酶活性的结构-活性关系以及基于结构的蛋白质设计奠定了基础,以开发潜在的抗凝药物。