Improved Dynamic Range, Resolving Power, and Sensitivity Achievable with FT-ICR Mass Spectrometry at 21 T Reveals the Hidden Complexity of Natural Organic Matter,Analytical Chemistry

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Improved Dynamic Range, Resolving Power, and Sensitivity Achievable with FT-ICR Mass Spectrometry at 21 T Reveals the Hidden Complexity of Natural Organic Matter
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-08-02 , DOI: 10.1021/acs.analchem.2c02377
William Bahureksa ₁ , Thomas Borch _{1,

2} , Robert B Young ₃ , Chad R Weisbrod ₄ , Greg T Blakney ₄ , Amy M McKenna _{2,

4}

Affiliation

Fourier transform ion-cyclotron resonance mass spectrometry (FT-ICR MS) is the only mass analyzer that can resolve the molecular complexity of natural organic matter at the level of elemental composition assignment. Here, we leverage the high dynamic range, resolving power, resistance to peak coalescence, and maximum ion number and ion trapping duration in a custom built, 21 tesla hybrid linear ion trap /FT-ICR mass spectrometer for a dissolved organic matter standard (Suwanne River Fulvic Acid). We compare the effect of peak-picking threshold (3σ, 4σ, 5σ, and 6σ) on number of elemental composition assignments, mass measurement accuracy, and dynamic range for a 6.3 s transient across the mass range of m/z 200–1200 that comprises the highest achieved resolving power broadband FT-ICR mass spectrum collected to date. More than 36 000 species are assigned with signal magnitude greater than 3σ at root-mean-square mass error of 36 ppb, the most species identified reported to date for dissolved organic matter. We identify ¹⁸O and ¹⁷O isotopologues and resolve isobaric overlaps on the order of a few electrons across a wide mass range (up to m/z 1000) leveraging mass resolving powers (3 000 000 at m/z 200) only achievable by 21 T FT-ICR MS and increased by ∼30% through absorption mode data processing. Elemental compositions unique to the 3σ span a wide compositional range of aromaticity not detected at higher peak-picking thresholds. Furthermore, we leverage the high dynamic range at 21 T FT-ICR MS to provide a molecular catalogue of a widely utilized reference standard (SRFA) to the analytical community collected on the highest performing mass analyzer for complex mixture analysis to date. This instrument is available free of charge to scientists worldwide.

中文翻译：

FT-ICR 质谱在 21 T 下可提高动态范围、分辨能力和灵敏度，揭示天然有机物质隐藏的复杂性

傅里叶变换离子回旋共振质谱 (FT-ICR MS) 是唯一可以在元素组成分配水平上解析天然有机物分子复杂性的质量分析仪。在这里，我们利用定制的 21 特斯拉混合线性离子阱/FT-ICR 质谱仪中的高动态范围、分辨能力、峰聚结阻力以及最大离子数和离子捕获持续时间，用于溶解有机物标准品（Suwanne河黄腐酸）。我们比较了峰值拾取阈值（3σ、4σ、5σ 和 6σ）对元素组成分配数量、质量测量精度和在m / z质量范围内的 6.3 s 瞬态的动态范围的影响200–1200，包括迄今为止收集到的最高分辨能力宽带 FT-ICR 质谱。超过 36 000 个物种的信号幅度大于 3σ，均方根质量误差为 36 ppb，这是迄今为止报告的溶解有机物质中发现的大多数物种。我们识别¹⁸ O 和¹⁷ O 同位素体，并利用质量分辨能力（ 3 000 000 在m / z200）只能通过 21 T FT-ICR MS 实现，并通过吸收模式数据处理增加了 30%。3σ 独有的元素组成跨越了在较高的拾峰阈值下未检测到的广泛的芳香性组成范围。此外，我们利用 21 T FT-ICR MS 的高动态范围向分析界提供广泛使用的参考标准 (SRFA) 的分子目录，该目录收集在性能最高的质量分析仪上，用于迄今为止的复杂混合物分析。该仪器可供全世界的科学家免费使用。

更新日期：2022-08-02

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