Electrospray Ionization of Polypropylene Glycol: Rayleigh-Charged Droplets, Competing Pathways, and Charge State-Dependent Conformations

Analytical Chemistry
Quentin DuezLars Konermann

Abstract

Recent molecular dynamics (MD) simulations from various laboratories have advanced the general understanding of electrospray ionization (ESI)-related processes. Unfortunately, computational cost has limited most of those previous endeavors to ESI droplets with radii of ∼3 nm or less, which represent the low end of the size distribution in the ESI plume. The current work extends this range by conducting simulations on aqueous ESI droplets with radii of 5.5 nm (∼23 000 water molecules). Considering that computational cost increases with r6, this is a significant step forward. We focused on the ESI process for polypropylene glycol (PPG) which is a common ESI-MS calibrant. Different chain lengths (PPG10, 30, and 60) were tested in droplets that were charged with excess Na+. Solvent evaporation and Na+ ejection, with occasional progeny droplet formation, kept the systems at 80-100% of the Rayleigh limit throughout their life cycle. PPG chains migrated to the droplet surface where they captured Na+ via binding to ether oxygens. Various possible pathways for PPG release into the gas phase were encountered. Some PPG10 runs showed ejection from the droplet surface, consistent with the ion evaporation model (IEM). In other instances, PPG...Continue Reading

References

Aug 10, 2000·Journal of Mass Spectrometry : JMS·R B Cole
Nov 20, 2001·Chemical Reviews·S D Hanton
May 9, 2002·Mass Spectrometry Reviews·N B Cech, C G Enke
Jul 2, 2002·Analytical Chemistry·Charles N McEwen, Patricia M Peacock
Jan 10, 2003·Nature·Denis DuftThomas Leisner
Feb 20, 2003·Journal of the American Chemical Society·Anthony T Iavarone, Evan R Williams
Sep 24, 2004·Journal of the American Chemical Society·S UdeB A Thomson
Feb 8, 2005·Journal of the American Society for Mass Spectrometry·Sándor KékiMiklós Zsuga
Aug 16, 2005·Analytical Chemistry·Igor A Kaltashov, Anirban Mohimen
Oct 8, 2005·Journal of Computational Chemistry·David Van Der SpoelHerman J C Berendsen
Jan 6, 2006·The Journal of Chemical Physics·J L F Abascal, C Vega
Oct 25, 2006·The Journal of Chemical Physics·Carl Caleman, David van der Spoel
Jan 11, 2007·Proceedings of the National Academy of Sciences of the United States of America·Steve Nguyen, John B Fenn
Mar 24, 2007·Analytical Chemistry·Peter NemesAkos Vertes
Jun 4, 2008·Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics·E GiglioC Guet
Dec 17, 2008·Analytical Chemistry·Gillian R HiltonJames H Scrivens
Jan 2, 2009·Analytical Chemistry·Christopher J HoganMichael L Gross
Jun 25, 2009·Mass Spectrometry Reviews·Paul Kebarle, Udo H Verkerk
Jul 25, 2009·Mass Spectrometry Reviews·Thomas R CoveyBradley B Schneider
Aug 14, 2009·Journal of Mass Spectrometry : JMS·Anna C CreceliusUlrich S Schubert
Oct 24, 2009·The Journal of Physical Chemistry. a·Ronald L Grimm, J L Beauchamp
Dec 8, 2009·Journal of the American Society for Mass Spectrometry·Rui Wang, Renato Zenobi
May 14, 2010·Journal of the American Society for Mass Spectrometry·Alan G GonçalvesMiguel D Noseda
May 25, 2010·Analytical Chemistry·Steffen M Weidner, Sarah Trimpin
Apr 26, 2012·The Journal of Physical Chemistry. B·Jun Kyung Chung, Styliani Consta
Nov 9, 2012·Analytical Chemistry·Lars KonermannSiavash Vahidi
Jul 9, 2013·Journal of Computational Chemistry·Jing Huang, Alexander D MacKerell
Jun 14, 2014·Journal of the American Society for Mass Spectrometry·Carlos LarribaDavid E Clemmer
Aug 20, 2014·Journal of the American Society for Mass Spectrometry·Rachel R Ogorzalek LooJoseph A Loo
Nov 25, 2014·The Journal of Chemical Physics·Carlos Larriba-Andaluz, Christopher J Hogan
May 9, 2015·Mass Spectrometry Reviews·Jinyu LiRita Grandori
May 28, 2015·Physical Chemistry Chemical Physics : PCCP·Hidenori HigashiYoshio Otani
Nov 18, 2015·Journal of Chemical Theory and Computation·Nina M FischerDavid van der Spoel
Jun 11, 2013·Journal of Chemical Theory and Computation·Sarah K Fegan, Mark Thachuk
Jul 12, 2016·Journal of the American Chemical Society·Kenneth J LaszloMatthew F Bush
Feb 15, 2017·Journal of the American Society for Mass Spectrometry·Simon A EwingJames S Prell
Jun 3, 2017·ACS Central Science·Massimiliano PorriniValérie Gabelica
Jul 27, 2017·Journal of the American Society for Mass Spectrometry·Piia LiigandAnneli Kruve

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Citations

Mar 9, 2019·Journal of Mass Spectrometry : JMS·Piia LiigandAnneli Kruve
Apr 18, 2019·Journal of the American Society for Mass Spectrometry·Xi ChenCarlos Larriba-Andaluz
Jun 9, 2020·Journal of the American Society for Mass Spectrometry·Calvin A AustinBarbara S Larsen
Aug 25, 2020·The Journal of Physical Chemistry. a·Michael J ApsokarduMurray V Johnston
Aug 27, 2021·Comprehensive Reviews in Food Science and Food Safety·Anto Pradeep Raja CharlesYing Wu
Jan 17, 2020·Biomacromolecules·Sébastien HoyasJérôme Cornil
Apr 15, 2020·The Journal of Physical Chemistry. a·Jincheng ZhangCharles Michael McCallum
Jan 25, 2022·Journal of the American Society for Mass Spectrometry·Amber D RollandJames S Prell

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