Borozan Sunčica Z, Zlatović Mario V, Stojanović Srđan Đ
Department of Chemistry, Faculty of Veterinary Medicine, University of Belgrade, Belgrade, Serbia.
Faculty of Chemistry, University of Belgrade, Belgrade, Serbia.
J Biol Inorg Chem. 2016 Jun;21(3):357-68. doi: 10.1007/s00775-016-1346-y. Epub 2016 Feb 24.
We analyzed the potential influence of anion-π interactions on the stability of complexes of proteins and halogen-containing non-natural amino acids. Anion-π interactions are distance and orientation dependent and our ab initio calculations showed that their energy can be lower than -8 kcal mol(-1), while most of their interaction energies lie in the range from -1 to -4 kcal mol(-1). About 20 % of these interactions were found to be repulsive. We have observed that Tyr has the highest occurrence among the aromatic residues involved in anion-π interactions, while His made the least contribution. Furthermore, our study showed that 67 % of total interactions in the dataset are multiple anion-π interactions. Most of the amino acid residues involved in anion-π interactions tend to be buried in the solvent-excluded environment. The majority of the anion-π interacting residues are located in regions with helical secondary structure. Analysis of stabilization centers for these complexes showed that all of the six residues capable of anion-π interactions are important in locating one or more of such centers. We found that anion-π interacting residues are sometimes involved in simultaneous interactions with halogens as well. With all that in mind, we can conclude that the anion-π interactions can show significant influence on molecular organization and on the structural stability of the complexes of proteins and halogen-containing non-natural amino acids. Their influence should not be neglected in supramolecular chemistry and crystal engineering fields as well.
我们分析了阴离子-π相互作用对蛋白质与含卤素非天然氨基酸复合物稳定性的潜在影响。阴离子-π相互作用取决于距离和方向,我们的从头算计算表明,其能量可能低于-8千卡/摩尔(-1),而其大多数相互作用能在-1至-4千卡/摩尔(-1)范围内。发现约20%的此类相互作用具有排斥性。我们观察到,在参与阴离子-π相互作用的芳香族残基中,酪氨酸出现的频率最高,而组氨酸的贡献最小。此外,我们的研究表明,数据集中67%的总相互作用是多重阴离子-π相互作用。参与阴离子-π相互作用的大多数氨基酸残基往往埋藏在溶剂排除环境中。大多数参与阴离子-π相互作用的残基位于具有螺旋二级结构的区域。对这些复合物的稳定中心分析表明,所有六个能够进行阴离子-π相互作用的残基对于定位一个或多个此类中心都很重要。我们发现,参与阴离子-π相互作用的残基有时也会同时与卤素相互作用。考虑到所有这些因素,我们可以得出结论,阴离子-π相互作用对蛋白质与含卤素非天然氨基酸复合物的分子组织和结构稳定性可产生显著影响。在超分子化学和晶体工程领域,其影响也不应被忽视。