Kelly Ryan T, Wang Chenchen, Rausch Sarah J, Lee Cheng S, Tang Keqi
Environmental Molecular Sciences Laboratory and §Biological Sciences Division, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States.
Anal Chem. 2014 Jul 1;86(13):6723-9. doi: 10.1021/ac501910p. Epub 2014 Jun 9.
A hybrid microchip/capillary electrophoresis (CE) system was developed to allow unbiased and lossless sample loading and high-throughput repeated injections. This new hybrid CE system consists of a poly(dimethylsiloxane) (PDMS) microchip sample injector featuring a pneumatic microvalve that separates a sample introduction channel from a short sample loading channel, and a fused-silica capillary separation column that connects seamlessly to the sample loading channel. The sample introduction channel is pressurized such that when the pneumatic microvalve opens briefly, a variable-volume sample plug is introduced into the loading channel. A high voltage for CE separation is continuously applied across the loading channel and the fused-silica capillary separation column. Analytes are rapidly separated in the fused-silica capillary, and following separation, high-sensitivity MS detection is accomplished via a sheathless CE/ESI-MS interface. The performance evaluation of the complete CE/ESI-MS platform demonstrated that reproducible sample injection with well controlled sample plug volumes could be achieved by using the PDMS microchip injector. The absence of band broadening from microchip to capillary indicated a minimum dead volume at the junction. The capabilities of the new CE/ESI-MS platform in performing high-throughput and quantitative sample analyses were demonstrated by the repeated sample injection without interrupting an ongoing separation and a linear dependence of the total analyte ion abundance on the sample plug volume using a mixture of peptide standards. The separation efficiency of the new platform was also evaluated systematically at different sample injection times, flow rates, and CE separation voltages.
开发了一种混合微芯片/毛细管电泳(CE)系统,以实现无偏且无损的样品加载以及高通量重复进样。这种新型混合CE系统由一个聚二甲基硅氧烷(PDMS)微芯片样品进样器和一个熔融石英毛细管分离柱组成,前者具有一个将样品引入通道与短样品加载通道分隔开的气动微阀,后者与样品加载通道无缝连接。对样品引入通道施加压力,使得当气动微阀短暂打开时,一个可变体积的样品塞被引入加载通道。在加载通道和熔融石英毛细管分离柱上持续施加用于CE分离的高电压。分析物在熔融石英毛细管中快速分离,分离后,通过无鞘CE/ESI-MS接口完成高灵敏度MS检测。对完整的CE/ESI-MS平台的性能评估表明,使用PDMS微芯片进样器可以实现具有良好控制的样品塞体积的可重复样品进样。从微芯片到毛细管没有出现谱带展宽,表明连接处的死体积最小。通过在不中断正在进行的分离的情况下重复样品进样以及使用肽标准混合物时总分析物离子丰度对样品塞体积的线性依赖性,证明了新型CE/ESI-MS平台在进行高通量和定量样品分析方面的能力。还在不同的样品进样时间、流速和CE分离电压下系统地评估了新平台的分离效率。