Measurement and Theory of Gas-Phase Ion Mobility Shifts Resulting from Isotopomer Mass Distribution Changes.

Autor: Harrilal CP; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Gandhi VD; Department of Mechanical Engineering, Purdue University, 585 Purdue Mall, West Lafayette, Indiana 47907, United States.; Department of Mechanical and Energy Engineering, IUPUI, 723 W. Michigan Street, Indianapolis, Indiana 46202, United States., Nagy G; Chemistry Department, University of Utah, Salt Lake City, Utah 84112, United States., Chen X; Department of Mechanical Engineering, Purdue University, 585 Purdue Mall, West Lafayette, Indiana 47907, United States.; Department of Mechanical and Energy Engineering, IUPUI, 723 W. Michigan Street, Indianapolis, Indiana 46202, United States., Buchanan MG; Department of Mechanical and Energy Engineering, IUPUI, 723 W. Michigan Street, Indianapolis, Indiana 46202, United States., Wojcik R; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Conant CR; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Donor MT; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Ibrahim YM; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Garimella SVB; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Smith RD; Biological Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States., Larriba-Andaluz C; Department of Mechanical and Energy Engineering, IUPUI, 723 W. Michigan Street, Indianapolis, Indiana 46202, United States.
Jazyk: angličtina
Zdroj: Analytical chemistry [Anal Chem] 2021 Nov 16; Vol. 93 (45), pp. 14966-14975. Date of Electronic Publication: 2021 Nov 02.
DOI: 10.1021/acs.analchem.1c01736
Abstrakt: The unanticipated discovery of recent ultra-high-resolution ion mobility spectrometry (IMS) measurements revealing that isotopomers─compounds that differ only in the isotopic substitution sites─can be separated has raised questions as to the physical basis for their separation. A study comparing IMS separations for two isotopomer sets in conjunction with theory and simulations accounting for ion rotational effects provides the first-ever prediction of rotation-mediated shifts. The simulations produce observable mobility shifts due to differences in gas-ion collision frequency and translational-to-rotational energy transfer. These differences can be attributed to distinct changes in the moment of inertia and center of mass between isotopomers. The simulations are in broad agreement with the observed experiments and consistent with relative mobility differences between isotopomers. These results provide a basis for refining IMS theory and a new foundation to obtain additional structural insights through IMS.
Databáze: MEDLINE
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