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首页> 外文期刊>Scientific reports. >Increased throughput and ultra-high mass resolution in DESI FT-ICR MS imaging through new-generation external data acquisition system and advanced data processing approaches
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Increased throughput and ultra-high mass resolution in DESI FT-ICR MS imaging through new-generation external data acquisition system and advanced data processing approaches

机译：通过新一代外部数据采集系统和高级数据处理方法提高吞吐量和超高质量分辨率MS成像和高级数据处理方法

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Desorption electrospray ionisation-mass spectrometry imaging (DESI-MSI) is a powerful imaging technique for the analysis of complex surfaces. However, the often highly complex nature of biological samples is particularly challenging for MSI approaches, as options to appropriately address molecular complexity are limited. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) offers superior mass accuracy and mass resolving power, but its moderate throughput inhibits broader application. Here we demonstrate the dramatic gains in mass resolution and/or throughput of DESI-MSI on an FT-ICR MS by developing and implementing a sophisticated data acquisition and data processing pipeline. The presented pipeline integrates, for the first time, parallel ion accumulation and detection, post-processing absorption mode Fourier transform and pixel-by-pixel internal re-calibration. To achieve that, first, we developed and coupled an external high-performance data acquisition system to an FT-ICR MS instrument to record the time-domain signals (transients) in parallel with the instrument's built-in electronics. The recorded transients were then processed by the in-house developed computationally-efficient data processing and data analysis software. Importantly, the described pipeline is shown to be applicable even to extremely large, up to 1 TB, imaging datasets. Overall, this approach provides improved analytical figures of merits such as: (i) enhanced mass resolution at no cost in experimental time; and (ii) up to 4-fold higher throughput while maintaining a constant mass resolution. Using this approach, we not only demonstrate the record 1?million mass resolution for lipid imaging from brain tissue, but explicitly show such mass resolution is required to resolve the complexity of the lipidome.
机译：解吸电喷雾电离质谱成像（Desi-MSI）是用于分析复杂表面的强大成像技术。然而，生物样品的通常高度复杂性质对于MSI方法特别具有挑战性，因为适当地解决了分子复杂性的选择是有限的。傅里叶变换离子回旋谐振质谱（FT-ICR MS）提供卓越的质量精度和质量分辨率，但其中等吞吐量抑制更广泛的应用。在这里，我们通过开发和实施复杂的数据采集和数据处理管道，展示了在FT-ICR MS上的质量分辨率和/或Desi-MSI吞吐量的巨大收益。所提出的管道是第一次，并行离子累积和检测，后处理吸收模式傅里叶变换和像素 - 逐个像素内部重新校准。为实现这一目标，首先，我们开发并耦合了外部高性能数据采集系统到FT-ICR MS仪器，以与仪器的内置电子设备并联地记录时域信号（瞬态）。然后由内部开发的计算有效的数据处理和数据分析软件处理录制的瞬变。重要的是，所描述的流水线甚至可以适用于极大的，最多1个TB成像数据集。总的来说，这种方法提供了改进的分析图，例如：（i）在实验时间内没有成本增强质量分辨率; （ii）吞吐量高达4倍，同时保持恒定质量分辨率。使用这种方法，我们不仅证明了从脑组织的脂质成像的记录1？百万质量分辨率，但明确地显示了这些质量分辨率来解决脂质体的复杂性。

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