Spray Mechanism of Contained-Electrospray Ionization
Spray Mechanism of Contained-Electrospray Ionization
复制标题
封闭式电喷雾电离喷雾机理
DOI：
10.1021/jasms.0c00044
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发表时间：
2020
影响因子：
3.2
通讯作者：
Badu-Tawiah, Abraham K.
中科院分区：
文献类型：
--
作者：
Miller, Colbert F.;Burris, Benjamin J.;Badu-Tawiah, Abraham K.
总结了包含电喷雾电离(ESI)的分析特征，即在液滴形成阶段对分析物溶液进行修改的潜力，从而提供机会产生天然的和变性的生物分子气相离子，而不需要对大块相分析物进行修改。带电微滴的实时修饰发生在所含ESI离子源出口中的空腔中。使用高速摄像机对空腔内部进行了仔细检查，发现形成了离散的液滴以及液滴尾迹中的薄液膜。当在20psi N2压力下操作时，观察到液滴的平均移动速度为8 mm/S，为∼1 S在10 mm腔长中提供了混合时间。根据不同喷雾条件下肌红蛋白的电荷状态分布、脱脂肌红蛋白含量和离子迁移率漂移时间分布，提供了高活性带电液滴存在的证据。还描述了不同操作模式对气相试剂捕获和液滴动力学的影响的机理见解。
Analytical characteristics of contained electrospray ionization (ESI) are summarized in terms of its potential to modify the analyte solution during the stages of droplet formation to provide opportunities to generate native versus denatured biomolecular gas-phase ions, without the need for bulk-phase analyte modifications. The real-time modification of the charged microdroplets occurs in a cavity that is included in the outlet of the contained-ESI ion source. Close examination of the inside of the cavity using a high-speed camera revealed the formation of discrete droplets as well as thin liquid films in the droplets wake. When operated at 20 psi N2pressure, the droplets were observed to move at an average speed of 8 mm/s providing ∼1 s mixing time in a 10 mm cavity length. Evidence is provided for the presence of highly reactive charged droplets based on myoglobin charge state distribution, apo-myoglobin contents, and ion mobility drift time profiles under different spray conditions. Mechanistic insights for the capture of vapor-phase reagents and droplet dynamics as influenced by different operational modes are also described.