Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning

Data related to the paper "Improved Extraction Repeatability and Spectral Reproducibility for Liquid Extraction Surface Analysis–Mass Spectrometry Using Superhydrophobic–Superhydrophilic Patterning" A major problem limiting reproducible use of liquid extraction surface analysis (LESA) array sampling of dried surface-deposited liquid samples is the unwanted spread of extraction solvent beyond the dried sample limits, resulting in unreliable data. Here, we explore the use of the Droplet Microarray (DMA), which consists of an array of superhydrophilic spots bordered by a superhydrophobic material giving the potential to confine both the sample spot and the LESA extraction solvent in a defined area. We investigated the DMA method in comparison with a standard glass substrate using LESA analysis of a mixture of biologically relevant compounds with a wide mass range and different physicochemical properties. The optimized DMA method was subsequently applied to urine samples from a human intervention study. Relative standard deviations for the signal intensities were all reduced at least 3-fold when performing LESA-MS on the DMA surface compared with a standard glass surface. Principal component analysis revealed more tight clusters indicating improved spectral reproducibility for a human urine sample extracted from the DMA compared to glass. Lastly, in urine samples from an intervention study, more significant ions (145) were identified when using LESA-MS spectra of control and test urine extracted from the DMA. We demonstrate that DMA provides a surface-assisted LESA-MS method delivering significant improvement of the surface extraction repeatability leading to the acquisition of more robust and higher quality data. The DMA shows potential to be used for LESA-MS for controlled and reproducible surface extraction and for acquisition of high quality, qualitative data in a high-throughput manner.

与论文《基于超疏水-超亲水图案化技术提升液体萃取表面分析-质谱法的萃取重复性与光谱重现性》相关的数据。限制液体萃取表面分析（LESA）阵列对干燥表面沉积液体样品进行可重复采样的主要问题在于萃取溶剂意外扩散至干燥样品边界之外，导致数据不可靠。本文探索了液滴微阵列（DMA）的应用，该阵列由超亲水斑点阵列构成，斑点周围环绕超疏水材料，有望将样品斑点与LESA萃取溶剂均限制在特定区域内。我们通过对具有宽质量范围和不同理化性质的生物相关化合物混合物进行LESA分析，将DMA方法与标准玻璃基底进行了对比研究。优化后的DMA方法随后应用于人体干预研究的尿液样品。在DMA表面进行LESA-MS分析时，信号强度的相对标准偏差相较于标准玻璃表面均降低了至少3倍。主成分分析显示，DMA上萃取的人体尿液样品形成了更紧密的聚类，表明其光谱重现性优于玻璃基底。最后，在干预研究的尿液样品中，利用DMA上萃取的对照与测试尿液的LESA-MS光谱，鉴定出了更多显著离子（145种）。我们证明，DMA提供了一种表面辅助的LESA-MS方法，可显著提升表面萃取重复性，从而获得更稳健、更高质量的数据。DMA在LESA-MS中展现出潜力，可用于可控且可重复的表面萃取，以及高通量获取高质量定性数据。