Online Hydrogen/Deuterium Exchange Performed in the Ion Mobility Cell of a Hybrid Mass Spectrometer
Online Hydrogen/Deuterium Exchange Performed in the Ion Mobility Cell of a Hybrid Mass Spectrometer
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DOI：
10.1021/ac901736j
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发表时间：
2009-11-15
影响因子：
7.4
通讯作者：
Rezzi, Serge
中科院分区：
文献类型：
--
作者：
Nagy, Kornel;Redeuil, Karine;Rezzi, Serge
本文介绍了四极杆飞行时间质谱仪的离子迁移池中实现的在线气相氢/氘交换的性能。利用氧化氘和氘代甲醇来产生氘代蒸气，该氘代蒸气被引入质谱仪的离子迁移率区域。氢/氘交换在毫秒时间范围内自发发生，而无需将仪器切换到离子迁移率模式。在低分子量分子和蛋白质的情况下，交换进行了研究。对于所有低分子量化合物，观察到的交换氢的数量等于理论上可交换氢的数量。该方法仅需对仪器进行最小的修改，简单、廉价、环境友好，与超高效液相色谱兼容，并且可以在市售仪器上实现。它不会影响液相色谱溶剂的选择和准确的质量或平行碎片（MSE）方法。将该方法的性能与其中将氘代溶剂引入仪器的锥气体中的常规替代方法的性能进行比较。尽管两种方法之间的交换程度相似，但“锥形气体方法”需要10倍更高的氘代溶剂体积（50 μ L/min），并且在串联质谱（MS/MS）模式中提供降低的灵敏度。所提出的方法建议作为一个标准的未来元素的质谱仪，以帮助在线未知的结构表征和研究蛋白质的构象变化与氢/氘交换。
The present paper describes the performance of online, gas-phase hydrogen/deuterium exchange implemented in the ion mobility cell of a quadrupole time-of-flight mass spectrometer. Deuterium oxide and deuterated methanol were utilized to create deuterated vapor that is introduced into the ion mobility region of the mass spectrometer. Hydrogen/deuterium exchange occurs spontaneously in the milliseconds time frame without the need of switching the instrument into ion mobility mode. The exchange was studied in case of low molecular weight molecules and proteins. The observed number of exchanged hydrogens was equal to the number of theoretically exchangeable hydrogens for all low molecular weight compounds. This method needs only minimal instrumental modifications, is simple, cheap, environment friendly, compatible with ultraperformance liquid chromatography, and can be implemented on commercially available instruments. It does not compromise choice of liquid chromatographic solvents and accurate mass or parallel-fragmentation (MSE) methods. The performance of this method was compared to that of conventional alternatives where the deuterated solvent is introduced into the cone gas of the instrument. Although the degree of exchange was similar between the two methods, the "cone gas method" requires 10 times higher deuterated solvent volumes (50 mu L/min) and offers reduced sensitivity in the tandem mass spectrometry (MS/MS) mode. The presented method is suggested as a standard future element of mass spectrometers to aid online structural characterization of unknowns and to study conformational changes of proteins with hydrogen/deuterium exchange.