Multinozzle emitter arrays for nanoelectrospray mass spectrometry.

Multinozzle emitter arrays for nanoelectrospray mass spectrometry.
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DOI:
10.1021/ac2011813
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发表时间:
2011-08-01
影响因子:
7.4
通讯作者:
Wang, Daojing
Wang, Daojing
中科院分区:
化学1区
文献类型:
--
作者:
Mao, Pan;Wang, Hung-Ta;Yang, Peidong;Wang, Daojing

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质谱(MS)是蛋白质组学和代谢组学的使能技术。然而,仍然需要在灵敏度和通量方面的显着改进以实现常规的基于MS的单细胞蛋白质组学和代谢组学。在这里,我们报告的硅基单片多喷嘴发射器阵列(MEA),并证明其在高灵敏度和高通量的纳米电喷雾质谱的原理证明的应用。我们的MEA由96个相同的10喷嘴发射器在一个3英寸的硅芯片上的圆形阵列。发射器的几何形状和配置、喷嘴的尺寸和数量以及嵌入在主通道中的微柱阵列可以在微制造过程期间系统地和精确地控制。结合静电模拟和实验测试,我们证明了在个别多喷嘴发射器的茎尖处的尖锐端几何形状显著增强了其突出喷嘴尖端处的电场,从而实现了高密度发射器阵列的连续纳米电喷雾。结果表明,在给定的总流量下,多喷嘴发射器的电喷雾电流与其喷嘴数的平方根近似成正比,表明多喷嘴发射器具有高的质谱灵敏度。使用传统的Z-喷雾质谱仪,我们证明了可重复的MS检测的肽和蛋白质的串行MEA发射器,实现灵敏度和稳定性的商业毛细管发射器。我们强大的硅基MEA芯片为超高灵敏度和超高通量蛋白质组学和代谢组学的完全集成微流体系统开辟了可能性。
Mass spectrometry (MS) is the enabling technology for proteomics and metabolomics. However, dramatic improvements in both sensitivity and throughput are still required to achieve routine MS-based single cell proteomics and metabolomics. Here, we report the silicon-based monolithic multinozzle emitter array (MEA), and demonstrate its proof-of-principle applications in high-sensitivity and high-throughput nanoelectrospray mass spectrometry. Our MEA consists of 96 identical 10-nozzle emitters in a circular array on a 3-inch silicon chip. The geometry and configuration of the emitters, the dimension and number of the nozzles, and the micropillar arrays embedded in the main channel, can be systematically and precisely controlled during the microfabrication process. Combining electrostatic simulation and experimental testing, we demonstrated that sharpened-end geometry at the stem of the individual multinozzle emitter significantly enhanced the electric fields at its protruding nozzle tips, enabling sequential nanoelectrospray for the high-density emitter array. We showed that electrospray current of the multinozzle emitter at a given total flow rate was approximately proportional to the square root of the number of its spraying-nozzles, suggesting the capability of high MS sensitivity for multinozzle emitters. Using a conventional Z-spray mass spectrometer, we demonstrated reproducible MS detection of peptides and proteins for serial MEA emitters, achieving sensitivity and stability comparable to the commercial capillary emitters. Our robust silicon-based MEA chip opens up the possibility of a fully-integrated microfluidic system for ultrahigh-sensitivity and ultrahigh-throughput proteomics and metabolomics.
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