Zhang Xiyun, Deng Qiaolin, Yoo Sandy H, Houk K N
Department of Chemistry and Biochemistry, University of California, Los Angeles 90095-1569, USA.
J Org Chem. 2002 Dec 13;67(25):9043-53. doi: 10.1021/jo0203894.
The binding of enantiomeric haptens and transition states by the Schultz Diels-Alderase antibody 39A11 and its germ-line antibody were studied theoretically. The mechanisms by which one hapten and one transition state stereoisomer is recognized selectively are explored with docking simulations and quantum mechanical models. Transition states of the relevant Diels-Alder reaction were located with density functional theory. A prediction is made that the stereoselectivity of 39A11 will be achieved by two strategically placed hydrogen bonds and pi-stacking interactions of the maleimide with a binding-site tryptophan, arranged so as to coordinate one enantiomeric transition state. Binding of other ligands by antibody 39A11 and the germ-line antibody has also been investigated. The polyspecific nature of 39A11 and its germ-line precursor was found to originate from the general ability of the binding pockets to achieve hydrophobic binding of small organic substrates. Comparison of the highly homologous progesterone and Diels-Alderase antibodies (DB3, 1E9, and 39A11) highlights the fact that differences of several key residues in the binding pockets are sufficient to confer selectivity for different antigens.
从理论上研究了舒尔茨狄尔斯-阿尔德酶抗体39A11及其种系抗体与对映体半抗原和过渡态的结合。通过对接模拟和量子力学模型探索了选择性识别一种半抗原和一种过渡态立体异构体的机制。用密度泛函理论确定了相关狄尔斯-阿尔德反应的过渡态。预测39A11的立体选择性将通过两个策略性定位的氢键以及马来酰亚胺与结合位点色氨酸的π-堆积相互作用来实现,其排列方式可协同一种对映体过渡态。还研究了抗体39A11和种系抗体与其他配体的结合。发现39A11及其种系前体的多特异性源于结合口袋实现小有机底物疏水结合的一般能力。高度同源的孕酮抗体和狄尔斯-阿尔德酶抗体(DB3、1E9和39A11)的比较突出了这样一个事实,即结合口袋中几个关键残基的差异足以赋予对不同抗原的选择性。