Department of Medicinal Chemistry and Pharmacognosy, College of Pharmacy , University of Illinois at Chicago , Chicago , Illinois 60612 , United States.
CAPES Foundation, Ministry of Education of Brazil , Brasília , Federal District 70040-020 , Brazil.
J Nat Prod. 2018 Sep 28;81(9):2083-2090. doi: 10.1021/acs.jnatprod.8b00432. Epub 2018 Sep 7.
Cyanobacteria are a source of chemically diverse metabolites with potential medicinal and biotechnological applications. Rapid identification of compounds is central to expedite the natural product discovery process. Mass spectrometry has been shown to be an important tool for dereplication of complex natural product samples. In addition, chromatographic separation and complementary spectroscopic analysis (e.g., UV) can enhance the confidence of the dereplication process. Here, we applied a droplet-liquid microjunction-surface sampling probe (droplet probe) coupled with UPLC-PDA-HRMS-MS/MS to identify two new natural products in situ from the freshwater strain Calothrix sp. UIC 10520. This allowed us to prioritize this strain for chemical investigation based on the presence of new metabolites very early in our discovery process, saving both time and resources. Subsequently, calothrixamides A (1) and B (2) were isolated from large-scale cultures, and the structures were elucidated by 1D and 2D NMR spectroscopy and mass spectrometry. The absolute configurations were determined by a combination of chemical degradation reactions, derivatization methods (Mosher's, Marfey's, and phenylglycine methyl ester), and J-based configurational analysis. Calothrixamides showed no cytotoxic activity against the MDA-MB-435, MDA-MB-231, and OVCAR3 cancer cell lines. They represent the first functionalized long-chain fatty acid amides reported from the Calothrix genus and from a freshwater cyanobacterium.
蓝细菌是具有潜在药用和生物技术应用的化学多样代谢物的来源。快速鉴定化合物是加速天然产物发现过程的关键。质谱已被证明是对复杂天然产物样品进行去重复鉴定的重要工具。此外,色谱分离和互补光谱分析(例如 UV)可以增强去重复过程的可信度。在这里,我们应用液滴-液相微连接-表面采样探针(液滴探针)与 UPLC-PDA-HRMS-MS/MS 相结合,从淡水菌株 Calothrix sp. UIC 10520 中现场鉴定出两种新的天然产物。这使我们能够根据在发现过程早期存在新代谢物,优先对该菌株进行化学研究,从而节省时间和资源。随后,从大规模培养物中分离出 calothrixamides A(1)和 B(2),并通过 1D 和 2D NMR 光谱和质谱法阐明了其结构。通过化学降解反应、衍生化方法(莫舍尔法、马费伊法和苯甘氨酸甲酯法)以及基于 J 的构象分析的组合确定了绝对构型。Calothrixamides 对 MDA-MB-435、MDA-MB-231 和 OVCAR3 癌细胞系没有细胞毒性活性。它们代表了从 Calothrix 属和淡水蓝细菌中首次报道的功能化长链脂肪酸酰胺。