Plasmonic nanoshells enhanced laser desorption/ionization mass spectrometry for detection of serum metabolites.
Plasmonic nanoshells enhanced laser desorption/ionization mass spectrometry for detection of serum metabolites.
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DOI：
10.1016/j.aca.2016.11.017
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发表时间：
2017-01
影响因子：
6.2
通讯作者：
Xiang Wei;Zhonghui Liu;Xiulong Jin;Lin Huang;D. Gurav;Xuming Sun;Baohong Liu;Jian Ye;Kun Qian
中科院分区：
文献类型：
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作者：
Xiang Wei;Zhonghui Liu;Xiulong Jin;Lin Huang;D. Gurav;Xuming Sun;Baohong Liu;Jian Ye;Kun Qian
基于激光解吸/电离质谱（LDI-MS）的小分子代谢物检测对于临床诊断具有重要意义。等离子体材料已被用作这些分子的LDI-MS的有效基底。但是，对于使用等离子体材料用于小代谢物的增强LDI MS的机制还没有明确的理解，从而限制了它们对真实的病例血清样品的应用。在这项工作中，我们报告使用等离子体纳米壳增强LDI MS检测小的分析物。Au纳米壳层的反键模式为在紫外光范围内产生热载流子提供了独特的机会。与Au纳米棒/纳米球和常规有机基质相比，Au纳米壳的这种效果显示出对复杂蛋白质/混合物中的小代谢物（例如氨基酸）的期望的分析灵敏度和耐久性。此外，我们实现了LDI-MS分析和检测的小代谢物从复杂的血清样品的Au纳米壳。我们的工作不仅阐明了等离子体纳米粒子与热载体增强激光多普勒电离质谱检测的机理，而且有助于激光多普勒电离质谱在临床研究中的真实的应用。
Laser desorption/ionization mass spectrometry (LDI MS)-based small metabolites detection is fundamentally important for the clinic prognoses and diagnoses. Plasmonic materials have been applied as efficient substrates for LDI MS of these molecules. However, there is no clear understanding of the mechanism of using plasmonic materials for enhanced LDI MS of small metabolites, thus restricting their application for real case serum samples. In this work, we report the use of plasmonic nanoshells for enhanced LDI MS detection of small analytes. The antibonding modes of Au nanoshells provided unique opportunity for the generation of hot carriers in the ultra-violet (UV) optical range. This effect of the Au nanoshells displayed desirable analytical sensitivity and endurance towards small metabolites (e.g. amino acids) in complex protein/mixtures as compared to Au nanorods/nanospheres and conventional organic matrix. Further we achieved LDI MS profiling and detection of small metabolites from complex serum samples by Au nanoshells. Our work not only shed light on the enhancement mechanism of LDI MS detection using plasmonic nanoparticles with hot carriers, but also contributed to the real case application of LDI MS in clinical study.