College of Chemistry, Beijing Normal University, Beijing, People's Republic of China.
J Am Soc Mass Spectrom. 2013 Jun;24(6):966-74. doi: 10.1007/s13361-013-0601-5. Epub 2013 Apr 5.
Growth process information and molecular structure identification are very important for characterization of self-assembled films. Here, we explore the possible application of desorption electrospray ionization mass spectrometry (DESI-MS) that provides the assembled information of rhodamine B (Rh B) and rhodamine 123 (Rh 123) films. With the help of lab-made DESI source, two characteristic ions Rh B and Rh 123 are observed directly in the open environment. To evaluate the reliability of this technique, a comparative study of ultraviolet-visible (UV-vis) spectroscopy and our method is carried out, and the result shows good correlation. According to the signal intensity of characteristic ions, the layer-by-layer adsorption process of dyes can be monitored, and the thicknesses of multilayer films can also be comparatively determined. Combining the high sensitivity, selectivity, and speed of mass spectrometry, the selective adsorption of similar structure molecules under different pH is recognized easily from extracted ion chronograms. The variation trend of dyes signalling intensity with concentration of polyelectrolyte is studied as well, which reflects the effect of surface charge on dyes deposition. Additionally, the desorption area, surface morphology, and thicknesses of multilayer films are investigated using fluorescence microscope, scanning electron microscope (SEM), and atomic force microscopy (AFM), respectively. Because the desorption area was approximately as small as 2 mm(2), the distribution situation of organic dyes in an arbitrary position could be gained rapidly, which means DESI-MS has advantages on in situ analysis.
生长过程信息和分子结构鉴定对于自组装膜的特性描述非常重要。在这里,我们探索了解吸电喷雾电离质谱(DESI-MS)的可能应用,它提供了罗丹明 B(Rh B)和罗丹明 123(Rh 123)膜的组装信息。在自制的 DESI 源的帮助下,我们直接在开放环境中观察到了两个特征离子Rh B和Rh 123。为了评估该技术的可靠性,我们进行了紫外-可见(UV-vis)光谱法和我们的方法的比较研究,结果显示出良好的相关性。根据特征离子的信号强度,可以监测染料的逐层吸附过程,并且还可以比较确定多层膜的厚度。结合质谱的高灵敏度、选择性和速度,可以从提取的离子时间图中容易地识别出不同 pH 值下类似结构分子的选择性吸附。我们还研究了染料信号强度随聚电解质浓度的变化趋势,这反映了表面电荷对染料沉积的影响。此外,分别使用荧光显微镜、扫描电子显微镜(SEM)和原子力显微镜(AFM)研究了多层膜的解吸面积、表面形貌和厚度。由于解吸面积大约只有 2mm(2),可以快速获得有机染料在任意位置的分布情况,这意味着 DESI-MS 具有原位分析的优势。