Biomolecular Medicine, Division of Computational and Systems Medicine, Department of Surgery and Cancer, Imperial College London , South Kensington, London SW7 2AZ, United Kingdom.
Institute of Liver Studies and Transplantation, Kings College Hospital , Denmark Hill, London SE5 9RS, United Kingdom.
Anal Chem. 2017 Feb 21;89(4):2478-2487. doi: 10.1021/acs.analchem.6b04623. Epub 2017 Feb 7.
A targeted reversed-phase gradient UPLC-MS/MS assay has been developed for the quantification /monitoring of 66 amino acids and amino-containing compounds in human plasma and serum using precolumn derivatization with 6-aminoquinolyl-N-hydroxysuccinimidyl carbamate (AccQTag Ultra). Derivatization of the target amines required minimal sample preparation and resulted in analytes with excellent chromatographic and mass spectrometric detection properties. The resulting method, which requires only 10 μL of sample, provides the reproducible and robust separation of 66 analytes in 7.5 min, including baseline resolution of isomers such as leucine and isoleucine. The assay has been validated for the quantification of 33 amino compounds (predominantly amino acids) over a concentration range from 2 to 20 and 800 μM. Intra- and interday accuracy of between 0.05 and 15.6 and 0.78-13.7% and precision between 0.91 and 16.9% and 2.12-15.9% were obtained. A further 33 biogenic amines can be monitored in samples for relative changes in concentration rather than quantification. Application of the assay to samples derived from healthy controls and patients suffering from acetaminophen (APAP, paracetamol)-induced acute liver failure (ALF) showed significant differences in the amounts of aromatic and branched chain amino acids between the groups as well as a number of other analytes, including the novel observation of increased concentrations of sarcosine in ALF patients. The properties of the developed assay, including short analysis time, make it suitable for high-throughput targeted UPLC-ESI-MS/MS metabonomic analysis in clinical and epidemiological environments.
一种靶向反相梯度 UPLC-MS/MS 分析方法已经开发出来,用于使用 6-氨基喹啉基-N-羟基琥珀酰亚胺基碳酸酯(AccQTag Ultra)进行预柱衍生化,对人血浆和血清中的 66 种氨基酸和含氨基酸的化合物进行定量/监测。目标胺的衍生化需要最小的样品制备,并且得到的分析物具有出色的色谱和质谱检测特性。该方法仅需 10μL 样品,可在 7.5 分钟内重现性地分离 66 种分析物,包括对异构体(如亮氨酸和异亮氨酸)进行基线分离。该测定方法已针对 33 种氨基酸化合物(主要是氨基酸)的定量进行了验证,浓度范围为 2 至 20 和 800μM。日内和日间的准确度在 0.05 至 15.6 和 0.78 至 13.7%之间,精密度在 0.91 至 16.9%和 2.12 至 15.9%之间。还可以监测样品中 33 种生物胺的浓度变化,而不是定量分析。该测定方法应用于来自健康对照者和乙酰氨基酚(APAP,扑热息痛)诱导的急性肝衰竭(ALF)患者的样品,结果显示两组之间芳香族和支链氨基酸的含量存在显著差异,以及其他一些分析物,包括在 ALF 患者中观察到的肌氨酸浓度增加的新现象。所开发的测定方法的特性,包括短的分析时间,使其适合于临床和流行病学环境中的高通量靶向 UPLC-ESI-MS/MS 代谢组学分析。