Hampton Christina Y, Forbes Thomas P, Varady Mark J, Meacham J Mark, Fedorov Andrei G, Degertekin F Levent, Fernández Facundo M
School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, USA.
Anal Chem. 2007 Nov 1;79(21):8154-61. doi: 10.1021/ac071297n. Epub 2007 Oct 3.
The analytical characterization of a novel ion source for mass spectrometry named array of micromachined ultrasonic electrosprays (AMUSE) is presented here. This is a fundamentally different type of ion generation device, consisting of three major components: (1) a piezoelectric transducer that creates ultrasonic waves at one of the resonant frequencies of the sample-filled device, (2) an array of pyramidally shaped nozzles micromachined on a silicon wafer, and (3) a spacer which prevents contact between the array and transducer ensuring the transfer of acoustic energy to the sample. A high-pressure gradient generated at the apexes of the nozzle pyramids forces the periodic ejection of multiple droplet streams from the device. With this device, the processes of droplet formation and droplet charging are separated; hence, the limitations of conventional electrospray-type ion sources, including the need for high charging potentials and the addition of organic solvent to decrease surface tension, can be avoided. In this work, a Venturi device is coupled with AMUSE in order to increase desolvation, droplet focusing, and signal stability. Results show that ionization of model peptides and small tuning molecules is possible with dc charging potentials of 100 Vdc or less. Ionization in rf-only mode (without dc biasing) was also possible. It was observed that, when combined with AMUSE, the Venturi device provides a 10-fold gain in signal-to-noise ratio for 90% aqueous sample solutions. Further reduction in the diameter of the orifices of the micromachined arrays led to an additional signal gain of at least 3 orders of magnitude, a 2-10-fold gain in the signal-to-noise ratio and an improvement in signal stability from 47% to 8.5% RSD. The effectiveness of this device for the soft ionization of model proteins in aqueous media, such as cytochrome c, was also examined, yielding spectra with an average charge state of 8.8 when analyzed with a 100 Vdc charging potential. Ionization of model proteins was also possible in rf-only mode.
本文介绍了一种用于质谱分析的新型离子源——微机械超声电喷雾阵列(AMUSE)的分析特性。这是一种从根本上不同类型的离子产生装置,由三个主要部件组成:(1)一个压电换能器,它在充满样品的装置的共振频率之一处产生超声波;(2)在硅片上微加工的金字塔形喷嘴阵列;(3)一个间隔物,它防止阵列与换能器接触,确保声能传递到样品。在喷嘴金字塔顶端产生的高压梯度迫使该装置周期性地喷出多股液滴流。使用该装置,液滴形成和液滴充电过程是分开的;因此,可以避免传统电喷雾型离子源的局限性,包括需要高充电电位以及添加有机溶剂以降低表面张力。在这项工作中,文丘里装置与AMUSE耦合,以提高去溶剂化、液滴聚焦和信号稳定性。结果表明,使用100 Vdc或更低的直流充电电位就可以实现模型肽和小分子调谐剂的电离。仅在射频模式(无直流偏置)下也可以电离。据观察,当与AMUSE结合使用时,文丘里装置可使90%的水性样品溶液的信噪比提高10倍。微加工阵列孔直径的进一步减小导致信号增益至少增加3个数量级,信噪比提高2至10倍,信号稳定性从47%相对标准偏差提高到8.5%相对标准偏差。还研究了该装置在水性介质中对模型蛋白质(如细胞色素c)进行软电离的有效性,当使用100 Vdc充电电位进行分析时,产生的光谱平均电荷态为8.8。在仅射频模式下也可以实现模型蛋白质的电离。