Department of Pharmaceutical Sciences, University of Maryland, Baltimore, Maryland 21201, United States.
J Chem Inf Model. 2013 May 24;53(5):1127-37. doi: 10.1021/ci400147s. Epub 2013 May 15.
The antiproliferative factor (APF) involved in interstitial cystitis is a glycosylated nonapeptide (TVPAAVVVA) containing a sialylated core 1 α-O-disaccharide linked to the N-terminal threonine. The chemical structure of APF was deduced using spectroscopic techniques and confirmed using total synthesis. The synthetic APF provided a platform to study amino acid modifications and their effect on APF activity, based on which a structure-activity relationship (SAR) for APF activity was previously proposed. However, this SAR model could not explain the change in activity associated with minor alterations in the peptide sequence. Presented is computational analysis of 14 APF derivatives to identify structural trends from which a more detailed SAR is obtained. The APF activity is found to be dictated by the close interplay between carbohydrate-peptide and peptide-peptide interactions. The former involves hydrogen bond and hydrophobic interactions, and the latter is dominated by hydrophobic interactions. The highly flexible hydrophobic peptide adopts collapsed conformations separated by low energy barriers. APF activity correlates with hydrophobic clustering associated with amino acids 4A, 6V, and 8V. Peptide conformations are highly sensitive to single point mutations, which explain the experimental trends. The presented SAR will act as a guide for lead optimization of more potent APF analogues of potential therapeutic utility.
参与间质性膀胱炎的增殖抑制因子 (APF) 是一种糖基九肽 (TVPAAVVVA),包含一个连接到 N 端苏氨酸的唾液酸化核心 1α-O-二聚糖。使用光谱技术推断 APF 的化学结构,并通过全合成证实。合成的 APF 为研究氨基酸修饰及其对 APF 活性的影响提供了一个平台,在此基础上提出了 APF 活性的构效关系 (SAR)。然而,该 SAR 模型无法解释与肽序列的微小改变相关的活性变化。本文介绍了对 14 种 APF 衍生物的计算分析,以确定结构趋势,从而获得更详细的 SAR。发现 APF 活性是由碳水化合物-肽和肽-肽相互作用之间的紧密相互作用决定的。前者涉及氢键和疏水相互作用,后者主要由疏水相互作用主导。高度灵活的疏水肽呈折叠构象,分离能低。APF 活性与氨基酸 4A、6V 和 8V 相关的疏水性聚集有关。肽构象对单点突变非常敏感,这解释了实验趋势。提出的 SAR 将作为潜在治疗用途的更有效 APF 类似物的先导优化指南。