School of Pharmaceutical Sciences, Changchun University of Chinese Medicine, Changchun, 130117, Jilin, China.
College of Vocational and Technical Education, Yunnan Normal University, Kunming, 650021, Yunnan, China.
Chem Biodivers. 2022 Apr;19(4):e202100928. doi: 10.1002/cbdv.202100928. Epub 2022 Mar 16.
To integrate the active advantages of 18β-glycyrrhetinic acid (18β-GA) and emodin, improve bioavailability, increase efficiency, and reduce toxicity, a one-step innovative synthetic route was set up for the first time: 4-dimethylaminopyridine (DMAP) was used as catalyst, 1-ethyl-(3-dimethylaminopropyl)carboimide hydrochloride (EDCI) as condensation agent, dry dichloromethane (DCM) as solvent at 25 °C for 12 h, the three target products were obtained and purified by high performance liquid chromatography (HPLC), the chemical structures of them were characterized by nuclear magnetic resonance (NMR) technique and high resolution electron ionization mass spectrometry (HREI-MS), namely, 18β-glycyrrhetinic acid-3-emodin ester (1, yield 78.83 %, known), di-18β-glycyrrhetinic acid-1-emodin ester (2, yield 6.49 %, new), and di-18β-glycyrrhetinic acid-8-emodin ester (3, yield 1.81 %, new). To estimate their effects of the products on toxicity in zebrafish embryos and juvenile fishes, the two precursors and three target products were assayed involving in hatching rate, survival rate, morphology, heart rate, and apoptosis of cardiomyocytes. The results showed that the target products enhanced the hatching and survival rate of zebrafish embryos, decreased the malformation rate and the apoptosis of cardiomyocytes. It should be suggested that the one-step synthesis route with high yield makes the industrial application of the target products possible due to significantly reduced toxicity. The two new by-products provide potential candidates for the applications of pharmaceutical industry in the future.
为了整合 18β-甘草次酸(18β-GA)和大黄素的活性优势,提高生物利用度,增加效率,降低毒性,首次建立了一步创新合成路线:使用 4-二甲氨基吡啶(DMAP)作为催化剂,1-乙基-(3-二甲基氨基丙基)碳二亚胺盐酸盐(EDCI)作为缩合剂,干燥二氯甲烷(DCM)作为溶剂,在 25°C 下反应 12 小时,通过高效液相色谱(HPLC)获得并纯化了三种目标产物,通过核磁共振(NMR)技术和高分辨电子电离质谱(HREI-MS)对它们的化学结构进行了表征,即 18β-甘草次酸-3-大黄素酯(1,产率 78.83%,已知)、二-18β-甘草次酸-1-大黄素酯(2,产率 6.49%,新)和二-18β-甘草次酸-8-大黄素酯(3,产率 1.81%,新)。为了评估这些产物对斑马鱼胚胎和幼鱼毒性的影响,对两种前体和三种目标产物进行了孵化率、存活率、形态、心率和心肌细胞凋亡的测定。结果表明,目标产物提高了斑马鱼胚胎的孵化率和存活率,降低了畸形率和心肌细胞凋亡率。这表明该高收率的一步合成路线使目标产物的工业应用成为可能,因为毒性明显降低。这两个新的副产物为未来医药工业的应用提供了潜在的候选物。