期刊
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
卷 23, 期 6, 页码 1077-1084出版社
SPRINGER
DOI: 10.1007/s13361-012-0365-3
关键词
Microsolvated compounds; Ion/surface reactions; Solvent effects; Mass spectrometry; Charged droplets; Desorption electrospray ionization; Ion soft landing
资金
- National Science Foundation [CHE NSF 0848650]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0848650] Funding Source: National Science Foundation
- Div Of Biological Infrastructure
- Direct For Biological Sciences [0852740] Funding Source: National Science Foundation
The exposure of charged microdroplets containing organic ions to solid-phase reagents at ambient surfaces results in heterogeneous ion/surface reactions. The electrosprayed droplets were driven pneumatically in ambient air and then electrically directed onto a surface coated with reagent. Using this reactive soft landing approach, acid-catalyzed Girard condensation was achieved at an ambient surface by directing droplets containing Girard T ions onto a dry keto-steroid. The charged droplet/surface reaction was much more efficient than the corresponding bulk solution-phase reaction performed on the same scale. The increase in product yield is ascribed to solvent evaporation, which causes moderate pH values in the starting droplet to reach extreme values and increases reagent concentrations. Comparisons are made with an experiment in which the droplets were pneumatically accelerated onto the ambient surface (reactive desorption electrospray ionization, DESI). The same reaction products were observed but differences in spatial distribution were seen associated with the splash of the high velocity DESI droplets. In a third type of experiment, the reactions of charged droplets with vapor phase reagents were examined by allowing electrosprayed droplets containing a reagent to intercept the headspace vapor of an analyte. Deposition onto a collector surface and mass analysis showed that samples in the vapor phase were captured by the electrospray droplets, and that instantaneous derivatization of the captured sample is possible in the open air. The systems examined under this condition included the derivatization of cortisone vapor with Girard T and that of 4-phenylpyridine N-oxide and 2-phenylacetophenone vapors with ethanolamine.
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