Starovoytov Oleg N, Liu Yalin, Tan Liuxi, Yang Shizhong
Department of Chemistry, Wayne State University , Detroit, Michigan 48202, United States.
Chem Res Toxicol. 2014 Aug 18;27(8):1371-9. doi: 10.1021/tx500082r. Epub 2014 Aug 7.
Bisphenol-A (4,4'-dihydroxy-2,2-diphenylpropane, BPA, or BPA-A) and its derivatives, when exposed to humans, may affect functions of multiple organs by specific binding to the human estrogen-related receptor γ (ERRγ). We carried out atomistic molecular dynamics (MD) simulations of three ligand compounds including BPA-A, 4-α-cumylphenol (BPA-C), and 2,2-diphenylpropane (BPA-D) binding to the ligand binding domain (LBD) of a human ERRγ to study the structures and energies associated with the binding. We used the implicit Molecular Mechanics/Poisson-Boltzmann Surface Area (MM/PBSA) method to estimate the free energies of binding for the phenyl based compound/ERRγ systems. The addition of hydroxyl groups to the aromatic ring had only a minor effect on binding structures and a significant effect on ligand/protein binding energy in an aqueous solution. Free binding energies of BPA-D to the ERRγ were found to be considerably less than those of BPA-A and BPA-C to the ERRγ. These results are well correlated with those from experiments where no binding affinities were determined in the BPA-D/ERRγ complex. No conformational change was observed for the helix 12 (H-12) of ERRγ upon binding of these compounds preserving an active transcriptional conformation state.
双酚A(4,4'-二羟基-2,2-二苯基丙烷,BPA或BPA-A)及其衍生物在接触人体时,可能通过与人雌激素相关受体γ(ERRγ)特异性结合而影响多个器官的功能。我们对包括BPA-A、4-α-异丙苯基苯酚(BPA-C)和2,2-二苯基丙烷(BPA-D)在内的三种配体化合物与人ERRγ的配体结合域(LBD)结合进行了原子分子动力学(MD)模拟,以研究与结合相关的结构和能量。我们使用隐式分子力学/泊松-玻尔兹曼表面积(MM/PBSA)方法来估计基于苯基的化合物/ERRγ系统的结合自由能。在芳环上添加羟基对结合结构的影响较小,但对水溶液中的配体/蛋白质结合能有显著影响。发现BPA-D与ERRγ的自由结合能远低于BPA-A和BPA-C与ERRγ的自由结合能。这些结果与实验结果高度相关,在实验中未测定BPA-D/ERRγ复合物的结合亲和力。在这些化合物结合后,ERRγ的螺旋12(H-12)未观察到构象变化,保持了活性转录构象状态。