Cedars-Sinai Medical Center, 121 N San Vicente, Beverly Hills, California 90211, United States.
University of Pittsburgh School of Medicine, 300 Halket Street, Pittsburgh, Pennsylvania 15213, United States.
Anal Chem. 2022 Sep 13;94(36):12452-12460. doi: 10.1021/acs.analchem.2c02609. Epub 2022 Aug 31.
Proteomic analysis on the scale that captures population and biological heterogeneity over hundreds to thousands of samples requires rapid mass spectrometry methods, which maximize instrument utilization (IU) and proteome coverage while maintaining precise and reproducible quantification. To achieve this, a short liquid chromatography gradient paired to rapid mass spectrometry data acquisition can be used to reproducibly quantify a moderate set of analytes. High-throughput profiling at a limited depth is becoming an increasingly utilized strategy for tackling large sample sets but the time spent on loading the sample, flushing the column(s), and re-equilibrating the system reduces the ratio of meaningful data acquired to total operation time and IU. The dual-trap single-column configuration (DTSC) presented here maximizes IU in rapid analysis (15 min per sample) of blood and cell lysates by parallelizing trap column cleaning and sample loading and desalting with the analysis of the previous sample. We achieved 90% IU in low microflow (9.5 μL/min) analysis of blood while reproducibly quantifying 300-400 proteins and over 6000 precursor ions. The same IU was achieved for cell lysates and over 4000 proteins (3000 at CV below 20%) and 40,000 precursor ions were quantified at a rate of 15 min/sample. Thus, DTSC enables high-throughput epidemiological blood-based biomarker cohort studies and cell-based perturbation screening.
在数百到数千个样本中捕获人群和生物异质性的规模进行蛋白质组学分析需要快速的质谱方法,这些方法最大限度地提高仪器利用率 (IU) 和蛋白质组覆盖率,同时保持精确和可重复的定量。为了实现这一目标,可以使用短的液相色谱梯度与快速质谱数据采集相结合,以可重复地定量中等数量的分析物。在有限的深度进行高通量分析正成为处理大样本集的越来越常用的策略,但用于加载样品、冲洗柱和重新平衡系统的时间会降低有意义的数据与总操作时间和 IU 的比例。这里提出的双阱单柱配置 (DTSC) 通过并行化阱柱清洗和样品加载以及用前一个样品的分析进行脱盐,在快速分析(每个样品 15 分钟)血液和细胞裂解物时最大限度地提高 IU。我们在低微流量(9.5 μL/min)分析血液时实现了 90%的 IU,可重现定量 300-400 种蛋白质和超过 6000 个前体离子。对于细胞裂解物,也实现了相同的 IU,可定量超过 4000 种蛋白质(CV 低于 20% 的 3000 种)和以 15 分钟/样本的速度定量 40000 个前体离子。因此,DTSC 能够实现高通量基于血液的流行病学生物标志物队列研究和基于细胞的扰动筛选。