Nefliu Marcela, Zelesky Todd, Jansen Patrick, Sluggett Gregory W, Foti Christopher, Baertschi Steven W, Harmon Paul A
Merck Research Laboratories, Merck & Co., Inc., West Point, Pennsylvania 19486.
Pfizer Inc., Analytical Research & Development, Eastern Point Road, Groton, Connecticut 06340.
J Pharm Sci. 2015 Dec;104(12):4287-4298. doi: 10.1002/jps.24667. Epub 2015 Nov 13.
We report artifactual degradation of pharmaceutical compounds containing primary and secondary amines during peroxy radical-mediated oxidative stress carried out using azoalkane initiators. Two degradation products were detected when model drug compounds dissolved in methanol/water were heated to 40°C with radical initiators such as 2,2'-azobis(2-methylpropionitrile) (AIBN). The primary artifact was identified as an α-aminonitrile generated from the reaction of the amine group of the model drug with formaldehyde and hydrogen cyanide, generated as byproducts of the stress reaction. A minor artifact was generated from the reaction between the amine group and isocyanic acid, also a byproduct of the stress reaction. We report the effects of pH, initiator/drug molar ratio, and type of azoalkane initiator on the formation of these artifacts. Mass spectrometry and nuclear magnetic resonance were used for structure elucidation, whereas mechanistic studies, including stable isotope labeling experiments, cyanide analysis, and experiments exploring the effects of butylated hydroxyanisole addition, were employed to support the degradation pathways.
我们报告了在使用偶氮烷引发剂进行过氧自由基介导的氧化应激过程中,含有伯胺和仲胺的药物化合物出现的人为降解情况。当溶解在甲醇/水中的模型药物化合物与自由基引发剂(如2,2'-偶氮二异丁腈(AIBN))一起加热到40°C时,检测到两种降解产物。主要的人为产物被鉴定为模型药物的胺基与甲醛和氰化氢反应生成的α-氨基腈,甲醛和氰化氢是应激反应的副产物。一种次要的人为产物是由胺基与异氰酸反应产生的,异氰酸也是应激反应的副产物。我们报告了pH值、引发剂/药物摩尔比和偶氮烷引发剂类型对这些人为产物形成的影响。使用质谱和核磁共振进行结构解析,同时采用包括稳定同位素标记实验、氰化物分析以及探索添加丁基羟基茴香醚效果的实验等机理研究来支持降解途径。