期刊
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
卷 405, 期 22, 页码 6933-6951出版社
SPRINGER HEIDELBERG
DOI: 10.1007/s00216-013-7114-8
关键词
Mass spectrometry; Atmospheric pressure Ionization; Ion bound clusters; Sampling; Spectroscopy/instrumentation
资金
- Bruker Daltonics, Bremen, Germany
- Research Center Julich
- German Research Foundation [Be 2124/6-1]
We provide experimental and theoretical evidence that the primary ionization process in the dopant-assisted varieties of the atmospheric pressure ionization methods atmospheric pressure photoionization and atmospheric pressure laser ionization in typical liquid chromatography-mass spectrometry settings is-as suggested in the literature-dopant radical cation formation. However, instead of direct dopant radical cation-analyte interaction-the broadly accepted subsequent step in the reaction cascade leading to protonated analyte molecules-rapid thermal equilibration with ion source background water or liquid chromatography solvents through dopant ion-molecule cluster formation occurs. Fast intracluster chemistry then leads to almost instantaneous proton-bound water/solvent cluster generation. These clusters interact either directly with analytes by ligand switching or association reactions, respectively, or further downstream in the intermediate-pressure regions in the ion transfer stages of the mass spectrometer via electrical-field-driven collisional decomposition reactions finally leading to the predominantly observed bare protonated analyte molecules [M + H](+).
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