Consumption of foods and dietary supplements (DS) adulterated with unprescribed or non-permitted phosphodiesterase-5 inhibitors (PDE-5i) and their analogs can cause serious risk to human health. This study aims to analyze 93 PDE-5i and their analogs present in adulterated foods and DS using an established and validated method involving high-performance liquid chromatography (HPLC). The method was validated in solid and liquid samples, resulting in a limit of detection and quantitation of 0.03–0.5 and 0.08–1.6 μg/mL, respectively. Using the validated method, a total of 404 samples were screened. It was found that 32% of 404 samples were illegally adulterated with PDE-5i and their analogs; moreover, 16.9% of the adulterated samples were found to contain more than three compounds. HPLC-quadrupole-time-of-flight (TOF)/mass spectrometry (MS) analysis was conducted on all the samples to confirm the detected compounds accurately based on fragmentation ion patterns. In addition, sildenafil and tadalafil were detected from the capsule shells of DS unusually. Subsequently, the detected compounds were identified and quantified using HPLC at concentrations ranging from 0.007 to 370.0 mg/g. NMR analysis was carried out to confirm the accurate chemical structure of a compound found during the TOF/MS analysis, which did not match with the 93 reference standards.; it was identified to be N-desmethylthiosildenafil. In this study, various PDE-5i compounds and their analogs were detected from low to high concentrations in a sample. Therefore, the study sheds light on the misuse of PDE-5i and their analogs in consumable products, which pose a severe threat to public health.

中文翻译：

---

使用 HPLC 和 LC-Q-TOF/MS 检测各种膳食补充剂配方和食品样品中的 94 种 PDE-5is 及其类似物，包括 N-去甲基硫代西地那非

食用掺有未经处方或未经许可的磷酸二酯酶 5 抑制剂 (PDE-5i) 及其类似物的食品和膳食补充剂 (DS) 会对人类健康造成严重风险。本研究旨在使用涉及高效液相色谱 (HPLC) 的成熟且经过验证的方法分析掺假食品和 DS 中存在的 93 PDE-5i 及其类似物。该方法在固体和液体样品中得到验证，检测限和定量限分别为 0.03–0.5 和 0.08–1.6 μg/mL。使用经过验证的方法，总共筛选了 404 个样品。发现404份样品中有32%被非法掺入PDE-5i及其类似物；此外，发现 16.9% 的掺假样品含有三种以上的化合物。对所有样品进行 HPLC-四极杆飞行时间 (TOF)/质谱 (MS) 分析，以根据碎片离子模式准确确认检测到的化合物。此外，从DS的胶囊壳中异常检出西地那非和他达拉非。随后，使用 HPLC 对检测到的化合物进行鉴定和定量，浓度范围为 0.007 至 370.0 mg/g。进行 NMR 分析以确认在 TOF/MS 分析过程中发现的化合物的准确化学结构，这与 93 种参考标准不匹配。鉴定为N-去甲基硫代西地那非。在这项研究中，在样品中检测了从低浓度到高浓度的各种 PDE-5i 化合物及其类似物。因此，该研究揭示了 PDE-5i 及其类似物在消费品中的滥用，