Plasmonic Gold Nanoshell-Assisted Laser Desorption/Ionization Mass Spectrometry for Small-Biomolecule Analysis and Tissue Imaging
Plasmonic Gold Nanoshell-Assisted Laser Desorption/Ionization Mass Spectrometry for Small-Biomolecule Analysis and Tissue Imaging
复制标题
用于小生物分子分析和组织成像的等离激元金纳米壳辅助激光解吸/电离质谱
DOI：
10.1021/acsanm.2c01850
复制
发表时间：
2022-06-22
影响因子：
5.9
通讯作者：
Wu, Xinzhou
中科院分区：
文献类型：
--
作者：
Du, Mingyi;Chen, Dong;Wu, Xinzhou
等离子体纳米壳已被公认为用于激光解吸/电离质谱（LDI-MS）检测各种小分子的有效纳米材料，而它们在质谱成像（MSI）中的应用开发较少。在这项工作中，我们构建和优化了SiO2@Au纳米壳，具有定制的壳结构和成分，用于高灵敏度LDI-MS分析和广泛的MSI应用。由于具有纳米级粗糙度和特定缝隙空间的等离子体壳层的协同效应，用于选择性捕获小分子和阳离子，SiO2@Au核-壳纳米颗粒表现出上级性能，用于检测各种各样的小分子，包括氨基酸、寡糖、染料和药物、肽、核苷和聚乙二醇。与有机基体相比，该方法具有基体干扰小、分析物覆盖度高、检测限低（fmol ~ pmol）、重复性好（RSD <5%）等优点。由于SiO2@Au纳米壳的纳米级尺寸和均匀沉积，各种小分子代谢物的空间分布可以在草莓组织中以100 μ m的像素尺寸可视化，而不会出现成像伪影。更有价值的是，SiO2@Au辅助的LDI-MSI的普遍性进一步证明了在斑马鱼（Danio rerio），蜜蜂（Apis cerana），和小鼠脑组织的全身组织内的脂质分布映射在空间分辨的方式在55，30，和50 μ m的像素大小，分别。这些结果有助于扩展等离子体核壳纳米粒子在实际MSI应用中的能力。综上所述，结果表明，SiO2@Au纳米壳有望成为具有上级DI效率和成像能力的有前途和有效的纳米材料，特别是在环境科学和生命科学领域。
Plasmonic nanoshells have been acknowledged as efficient nanomaterials for laser desorption/ionization mass spectrometry (LDI-MS) detection of a wide range of small molecules, whereas their applications in mass spectrometry imaging (MSI) are less developed. In this work, we constructed and optimized SiO2@Au nanoshells with tailor-made shell structures and compositions for high-sensitivity LDI-MS analysis and a wide range of MSI applications. Owing to the synergistic effects of plasmonic shells with nanoscale roughness and specific crevice space for the selective trapping of small molecules and cations, SiO2@Au core-shell nanoparticles exhibit superior performance for the detection of a vast diversity of small molecules, induding amino acids, oligosaccharides, dyestuff and drugs, peptides, nucleosides, and poly(ethylene glycols). Compared with organic matrices, this method affords a high reduction in matrix interference, higher analyte coverage, lower detection limits ranging from fmol to pmol, and good repeatability with relative standard deviation (RSD) below 5%. Due to the nanoscale size and homogeneous deposition of SiO2@Au nanoshells, the spatial distribution of various smallmolecule metabolites can be visualized in strawberry tissues at a pixel size of 100 mu m without imaging artifacts. More valuably, the universality of SiO2@Au-assisted LDI-MSI is further demonstrated for mapping the lipid distribution within the whole-body tissues of zebrafish (Danio rerio), honeybees (Apis cerana), and mouse brain tissues in a spatially resolved manner at pixel sizes of 55, 30, and 50 mu m, respectively. These results facilitate the expansion of the abilities of plasmonic core-shell nanoparticles in real-case MSI applications. Taken together, the results indicate that the SiO2@Au nanoshells are expected to be promising and efficient nanomaterials with superior DI efficiency and imaging capabilities, especially in the environmental science and life science fields.