Giordano Braden C, Jin Lianji, Couch Abigail J, Ferrance Jerome P, Landers James P
Department of Chemistry, University of Virginia, McCormick Road, Charlottesville, Virginia 22901, USA.
Anal Chem. 2004 Aug 15;76(16):4705-14. doi: 10.1021/ac030349f.
We have previously demonstrated on-column dynamic labeling of protein-SDS complexes on capillaries and microchips for laser-induced fluorescence (LIF) detection using both a commercially available fluor and a protein separation buffer. Upon binding to hydrophobic moieties (of the analyte or separation buffer), the fluor undergoes a conformational change allowing fluorescence detection at 590 nm following excitation with 488-nm light. Our original work showed on-chip limits of detection (LOD) comparable with those using UV detection (1 x 10(-5) M) on capillaries-falling significantly short of the detection limits expected for LIF. This was largely a function of the physicochemical characteristics of the separation buffer components, which provided significant background fluorescence. Having defined the contributing factors involved, a new separation buffer was produced which reduced the background fluorescence and, consequently, increased the available dye for binding to protein-SDS complexes, improving the sensitivity in both capillaries and microchips by at least 2 orders of magnitude. The outcome is a rapid, sensitive method for protein sizing and quantitation applicable to both capillary and microchip separations with a LOD of 500 ng/mL for bovine serum albumin. Interestingly, sensitivity on microdevices was improved by inclusion of the dye in the sample matrix, while addition of dye to samples in conventional CE resulted in a drastic reduction in sensitivity and resolution. This can be explained by the differences in the injection schemes used in the two systems. The linear range for protein quantitation covered at least 2 orders of magnitude in microchip applications. On-chip analysis of human sera allowed abnormalities, specifically the presence of elevated levels of gamma-globulins, to be determined.
我们之前已经证明了在毛细管和微芯片上对蛋白质-SDS复合物进行柱上动态标记,用于激光诱导荧光(LIF)检测,使用的是市售荧光染料和蛋白质分离缓冲液。荧光染料与(分析物或分离缓冲液的)疏水部分结合后,会发生构象变化,在用488纳米光激发后可在590纳米处进行荧光检测。我们最初的工作表明,芯片上的检测限(LOD)与毛细管上使用紫外检测(1×10⁻⁵ M)时相当,但远低于LIF预期的检测限。这在很大程度上是分离缓冲液成分的物理化学特性所导致的,这些成分产生了显著的背景荧光。在确定了相关影响因素后,制备了一种新的分离缓冲液,它降低了背景荧光,因此增加了可用于与蛋白质-SDS复合物结合的染料量,使毛细管和微芯片的灵敏度都提高了至少2个数量级。结果是得到了一种快速、灵敏的蛋白质大小测定和定量方法,适用于毛细管和微芯片分离,牛血清白蛋白的LOD为500 ng/mL。有趣的是,在微器件上,通过将染料包含在样品基质中提高了灵敏度,而在传统毛细管电泳中向样品中添加染料会导致灵敏度和分辨率大幅降低。这可以通过两种系统中使用的进样方案的差异来解释。在微芯片应用中,蛋白质定量的线性范围至少覆盖2个数量级。对人血清进行芯片分析能够确定异常情况,特别是γ球蛋白水平升高的情况。