Comprehensive Ion Mobility Calibration: Poly(ethylene oxide) Polymer Calibrants and General Strategies

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作   者：

Jean R. N. Haler;  Christopher Kune;  Philippe Massonnet;  Clothilde Comby-Zerbino;  Jan Jordens;  Maarten Honing;  Ynze Mengerink;  Johann Far;  Edwin De Pauw; 

作者机构：

Institut Lumière Matière;  Université Lyon 1;  Mass Spectrometry Laboratory;  Quartier Agora;  The Netherlands;  University of Liège;  DSM Resolve;  Université de Lyon;  69100 Villeurbanne;  CNRS;  B-4000 Liège;  Geleen;  France;  Allée du Six Aout 11;  Belgium; 

期刊名称：

Analytical chemistry

i s s n：

0003-2700

年卷期：

2017 年 89 卷 22 期

页   码：

12076-12086

页   码：

摘   要：

Ion mobility (IM) is now a well-established and fast analytical technique. The IM hardware is constantly being improved, especially in terms of the resolving power. The Drift Tube (DTIMS), the Traveling Wave (TWIMS), and the Trapped Ion Mobility Spectrometry (TIMS) coupled to mass spectrometry are used to determine the Collision Cross-Sections (CCS) of ions. In analytical chemistry, the CCS is approached as a descriptor for ion identification and it is also used in physical chemistry for 3D structure elucidation with computational chemistry support. The CCS is a physical descriptor extracted from the reduced mobility (K₀) measurements obtainable only from the DTIMS. TWIMS and TIMS routinely require a calibration procedure to convert measured physical quantities (drift time for TWIMS and elution voltage for TIMS) into CCS values. This calibration is a critical step to allow interinstrument comparisons. The previous calibrating substances lead to large prediction bands and introduced rather large uncertainties during the CCS determination. In this paper, we introduce a new IM calibrant (CCS and K₀) using singly charged sodium adducts of poly(ethylene oxide) monomethyl ether (CH₃O-PEO-H) for positive ionization in both helium and nitrogen as drift gas. These singly charged calibrating ions make it possible to determine the CCS/K₀ of ions having higher charge states. The fitted calibration plots exhibit larger coverage with less data scattering and significantly improved prediction bands and uncertainties. The reasons for the improved CCS/K₀ accuracy, advantages, and limitations of the calibration procedures are also discussed. A generalized IM calibration strategy is suggested.