Department of Chemistry, Cleveland State University, Cleveland, OH 44115, USA.
Case Comprehensive Cancer Center, Case Western Reserve University, Cleveland, OH 44106, USA.
J Chromatogr B Analyt Technol Biomed Life Sci. 2018 Jul 15;1090:22-35. doi: 10.1016/j.jchromb.2018.05.008. Epub 2018 May 16.
Androgens play a vital role in prostate cancer development, and their elimination and blockade are essential in the disease management. DHT is the key ligand for androgen receptor (AR) in the prostate. It is locally synthesized from testosterone. In the prostate, DHT is predominantly metabolized to α-diol and β-diol. Recent studies indicate that impaired DHT catabolism is associated with prostate cancer, signifying the necessity of a sensitive quantitative method for the determination of DHT and its metabolites. In this work, an LC-MS/MS method for the simultaneous quantification of DHT and its metabolites was developed and validated. Steroid-free sera were prepared and used for the preparation of sera calibrators and quality controls (QCs). DHT and its metabolites along with their respective stable heavy isotope labeled analytes representing internal standards were first extracted with methyl tertiary-butyl ether (MTBE) and derivatized with picolinic acid (PA). The derivatized analytes were then extracted again with MTBE, dried under nitrogen and reconstituted in the mobile phase (80% methanol and 0.2% formic acid in water). Baseline chromatographic separation of the derivatized analytes was achieved isocratically on XTerra C18 column (2.1 × 100 mm) using the mobile phase at a flow rate of 0.25 mL/min. Quantitation was performed using multiple-reaction-monitoring mode with positive electrospray ionization. The method has calibration ranges from 0.0500 ng/mL to 50.0 ng/mL for DHT and its two metabolites with acceptable assay precision, accuracy, recovery, and matrix factor. It was applied to the determination of DHT and its metabolites in an animal study.
雄激素在前列腺癌的发展中起着至关重要的作用,其消除和阻断在疾病管理中至关重要。DHT 是前列腺中雄激素受体 (AR) 的关键配体。它是由睾酮在局部合成的。在前列腺中,DHT 主要代谢为 α-二醇和 β-二醇。最近的研究表明,DHT 代谢受损与前列腺癌有关,这表明需要一种灵敏的定量方法来测定 DHT 及其代谢物。在这项工作中,开发并验证了一种用于同时定量测定 DHT 及其代谢物的 LC-MS/MS 方法。制备无类固醇血清并用于制备血清校准品和质控品 (QC)。DHT 及其代谢物及其各自的稳定重同位素标记内标分析物首先用甲基叔丁基醚 (MTBE) 提取,并用吡啶酸 (PA) 衍生化。然后用 MTBE 再次提取衍生化的分析物,氮气干燥,在流动相中重新溶解(80%甲醇和 0.2%甲酸水溶液)。衍生化分析物在 XTerra C18 柱(2.1×100mm)上以等度洗脱,流动相流速为 0.25mL/min,实现了衍生化分析物的基线色谱分离。采用正电喷雾电离多反应监测模式进行定量。该方法对 DHT 及其两种代谢物的校准范围为 0.0500ng/mL 至 50.0ng/mL,具有可接受的分析精密度、准确度、回收率和基质因子。该方法已应用于动物研究中 DHT 及其代谢物的测定。