Hu Xin, Stebbins C Erec
Laboratory of Structural Microbiology, The Rockefeller University, New York, New York 10021, USA.
Biophys J. 2006 Aug 1;91(3):948-56. doi: 10.1529/biophysj.105.080259. Epub 2006 May 12.
The bacterial protein tyrosine phosphatase YopH is an essential virulence determinant in Yersinia spp., causing gastrointestinal diseases and the plague. Like eukaryotic PTPases, YopH catalyzes the hydrolysis of the phosphate moiety of phosphotyrosine within a highly conserved binding pocket, which is also characterized by the closure of the so-called "WPD loop" upon ligand binding. In this study, we investigate the conformational changes and dynamics of the WPD loop by molecular dynamics simulations. Consistent with experimental observations, our simulations show that the WPD loop of YopH is intrinsically flexible and fluctuates between the open and closed conformation with a frequency of approximately 4 ns for the apo, native protein. The region of helix alpha4 spanning loop 384-392, which has been revealed experimentally as a second substrate-binding site in YopH, is found to be highly associated with the WPD loop, stabilizing it in the closed, active conformation, and providing a structural basis for the cooperation of the second-substrate binding site in substrate recognition. Loop L4 (residues 323-327) is shown to be involved in a parallel, correlated motion mode with the WPD loop that contributes the stabilization of a more extended open conformation. In addition, we have simulated the loop reopening in the ligand-bound protein complex by applying the locally enhanced sampling method. Finally, the dynamic behavior of the WPD loop for the C403S mutant differs from the wild-type YopH remarkably. These results shed light on the role of the WPD loop in PTPase-mediated catalysis, and are useful in structure-based design for novel, selective YopH inhibitors as antibacterial drugs.
细菌蛋白酪氨酸磷酸酶YopH是耶尔森氏菌属中的一种重要毒力决定因素,可引发胃肠道疾病和鼠疫。与真核蛋白酪氨酸磷酸酶一样,YopH在一个高度保守的结合口袋内催化磷酸酪氨酸的磷酸基团水解,该口袋的特征还在于配体结合时所谓的“WPD环”会关闭。在本研究中,我们通过分子动力学模拟研究了WPD环的构象变化和动力学。与实验观察结果一致,我们的模拟表明,YopH的WPD环本质上具有灵活性,对于无配体的天然蛋白,其在开放和关闭构象之间波动的频率约为4纳秒。实验表明,跨越环384 - 392的α4螺旋区域是YopH中的第二个底物结合位点,发现它与WPD环高度相关,将其稳定在关闭的活性构象中,并为第二个底物结合位点在底物识别中的协同作用提供了结构基础。环L4(残基323 - 327)显示与WPD环以平行、相关的运动模式参与其中,有助于稳定更伸展的开放构象。此外,我们通过应用局部增强采样方法模拟了配体结合蛋白复合物中环的重新开放。最后,C403S突变体的WPD环的动态行为与野生型YopH有显著差异。这些结果揭示了WPD环在蛋白酪氨酸磷酸酶介导的催化中的作用,并且有助于基于结构设计新型、选择性的YopH抑制剂作为抗菌药物。