Effect of cocrystallization due to bile acid on molecular‐ion sensitivity of biological phospholipids in Bi cluster time‐of‐flight secondary ion mass spectrometry measurements
Effect of cocrystallization due to bile acid on molecular‐ion sensitivity of biological phospholipids in Bi cluster time‐of‐flight secondary ion mass spectrometry measurements
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Bi簇飞行时间二次离子质谱测量中胆汁酸共结晶对生物磷脂分子离子敏感性的影响
DOI：
10.1002/sia.7039
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发表时间：
2021
影响因子：
1.7
通讯作者：
Shishido Rie
中科院分区：
文献类型：
--
作者：
野村薫平;広木僚也;久田皓貴;伊藤雄太;會田忠弘;Shishido Rie
双团簇飞行时间二次离子质谱（TOF-西姆斯）是一种用于评估有机表面的有用方法。然而，它检测大分子的能力是有限的。问题之一是大分子的灵敏度低于小分子的灵敏度，因为较大的分子倾向于表现出较低的电离效率和/或较高的碎裂概率。基质增强（ME）-西姆斯是一种用于完整分子离子的灵敏度增强技术。已知由分析物和基质组成的混合物质的晶体结构影响分析目标的灵敏度。在本研究中，使用Bi簇TOF-西姆斯研究了由于胆汁酸的存在而发生的共结晶对分子离子灵敏度的影响。选择具有表面活性行为的生物磷脂和胆汁酸分别作为评价分子和添加剂。质谱表明，含胆汁酸的磷脂的二次离子产率显著高于原始脂质的二次离子产率。具体而言，分析物/胆汁酸比例为1：100的样本对[M + H]+和[2 M + H]+分子离子的灵敏度比原始样本的灵敏度提高约60-100倍。在分子分布的评价中，从共结晶区域获得的完整离子的信号计数较高，尽管从这些区域发射的碎片化离子较少。因此，结果表明，由于胆汁酸的存在，共结晶提供了一个有效的晶体结构，以促进较大分子的发射。
Bi cluster time‐of‐flight secondary ion mass spectrometry (TOF‐SIMS) is a useful method for evaluating organic surfaces. However, its ability to detect large molecules is limited. One of the problems is that the sensitivities of macromolecules are lower than those of small molecules because larger molecules tend to exhibit lower ionization efficiencies and/or higher probabilities of fragmentation. Matrix‐enhanced (ME)‐SIMS is a sensitivity enhancement technique for intact molecular ions. The crystal structure of a mixed substance composed of an analyte and a matrix is known to affect the sensitivity of the analysis target. In this study, the effect of cocrystallization, which occurs due to the presence of bile acid, on the molecular‐ion sensitivity was investigated using Bi cluster TOF‐SIMS. Biological phospholipids and bile acids, which exhibit surfactant behaviors, were selected as the evaluated molecules and additives, respectively. The mass spectra indicated that the secondary‐ion yields of phospholipids with bile acid were substantially greater than those of the pristine lipid. Specifically, samples with an analyte/bile acid ratio of 1:100 achieved approximately 60–100‐fold sensitivity enhancement of [M + H]+and [2M + H]+molecular ions than the sensitivity achieved with the pristine samples. In the evaluation of molecular distribution, higher signal counts of intact ions were obtained from the cocrystallization area, although less‐fragmented ions were emitted from these regions. Consequently, the results indicate that the cocrystallization due to the presence of bile acid provides an effective crystal structure for facilitating emission of larger molecules.
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