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Abstract：
This work presents the first systematic comparison of selenium (Se) speciation in plasma from cancer patients treated orally with three Se compounds (sodium selenite, SS; L-selenomethionine, SeMet; or Se-methylselenocysteine, MSC) at 400 µg/day for 28 days. The primary goal was to investigate how these chemical forms of Se affect the plasma Se distribution, aiming to identify the most effective Se compound for optimal selenoprotein expression. This was achieved using methodology based on HPLC-ICP-MS after sample preparation/fractionation approaches. Measurements of total Se in plasma samples collected before and after 4 weeks of treatment showed that median total Se levels increased significantly from 89.6 to 126.4 µg kg-1 Se (p < 0.001), particularly when SeMet was administered (190.4 µg kg-1 Se). Speciation studies showed that the most critical differences between treated and baseline samples were seen for selenoprotein P (SELENOP) and selenoalbumin after administration with MSC (p = 5.8 × 10-4) and SeMet (p = 6.8 × 10-5), respectively. Notably, selenosugar-1 was detected in all low-molecular-weight plasma fractions following treatment, particularly with MSC. Two different chromatographic approaches and spiking experiments demonstrated that about 45% of that increase in SELENOP levels (to ~ 8.8 mg L-1) with SeMet is likely due to the non-specific incorporation of SeMet into the SELENOP affinity fraction. To the authors\' knowledge, this has not been reported to date. Therefore, SELENOP is probably part of both the regulated (55%) and non-regulated (45%) Se pools after SeMet administration, whereas SS and MSC mainly contribute to the regulated one.
摘要：
这项工作首次对口服三种硒化合物（亚硒酸钠，SS；L-硒代蛋氨酸，SeMet；或Se-甲基硒代半胱氨酸，MSC），每天400微克，持续28天。主要目标是研究Se的这些化学形式如何影响等离子体Se分布，旨在确定最佳硒蛋白表达的最有效硒化合物。这是在样品制备/分级分离方法之后使用基于HPLC-ICP-MS的方法实现的。在治疗前和治疗后4周收集的血浆样本中总硒的测量显示，总硒水平中位数从89.6μgkg-1硒显著增加到126.4μgkg-1(p<0.001)，特别是当使用SeMet时（190.4µgkg-1Se）。形态研究表明，在使用MSC（p=5.8×10-4）和SeMet（p=6.8×10-5）后，硒蛋白P（SELENOP）和硒白蛋白（p=5.8×10-5），分别。值得注意的是,硒糖-1在治疗后的所有低分子量血浆部分检测，特别是MSC。两种不同的色谱方法和加标实验表明，用SeMet增加SELENOP水平（至〜8.8mgL-1）的约45％可能是由于SeMet非特异性掺入SELENOP亲和分数。就作者所知，到目前为止还没有报告。因此,SELENOP可能是SeMet施用后调节（55％）和非调节（45％）Se池的一部分，而SS和MSC主要是受调控的。
