Release of Native-like Gaseous Proteins from Electrospray Droplets via the Charged Residue Mechanism: Insights from Molecular Dynamics Simulations

Journal of the American Chemical Society
Robert G McAllisterLars Konermann

Abstract

The mechanism whereby gaseous protein ions are released from charged solvent droplets during electrospray ionization (ESI) remains a matter of debate. Also, it is unclear to what extent electrosprayed proteins retain their solution structure. Molecular dynamics (MD) simulations offer insights into the temporal evolution of protein systems. Surprisingly, there have been no all-atom simulations of the protein ESI process to date. The current work closes this gap by investigating the behavior of protein-containing aqueous nanodroplets that carry excess positive charge. We focus on "native ESI", where proteins initially adopt their biologically active solution structures. ESI proceeds while the protein remains entrapped within the droplet. Protein release into the gas phase occurs upon solvent evaporation to dryness. Droplet shrinkage is accompanied by ejection of charge carriers (Na(+) for the conditions chosen here), keeping the droplet at ∼85% of the Rayleigh limit throughout its life cycle. Any remaining charge carriers bind to the protein as the final solvent molecules evaporate. The outcome of these events is largely independent of the initial protein charge and the mode of charge carrier binding. ESI charge states and collis...Continue Reading

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Citations

Aug 11, 2016·Journal of the American Society for Mass Spectrometry·James G BonnerRyan R Julian
Sep 27, 2016·Journal of the American Chemical Society·Michael B CammarataJennifer S Brodbelt
Oct 7, 2016·Journal of the American Society for Mass Spectrometry·Wenjing LiMaureen A Kane
Dec 14, 2016·Journal of the American Chemical Society·Joseph D EschweilerBrandon T Ruotolo
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Apr 5, 2017·Journal of the American Society for Mass Spectrometry·Yana A LyonRyan R Julian
May 18, 2020·Proceedings of the National Academy of Sciences of the United States of America·Jie LiTimothy M Swager
Mar 18, 2021·Journal of the American Society for Mass Spectrometry·Melanie Cheung See KitIan K Webb
Jun 1, 2021·ACS Omega·Mohamed Ahmed KhairehDavid A Bonhommeau
Jan 14, 2017·Journal of the American Society for Mass Spectrometry·David Z KeiferMartin F Jarrold
Jul 16, 2017·Journal of the American Society for Mass Spectrometry·Lars Konermann
Jul 26, 2018·Journal of the American Society for Mass Spectrometry·Karen C B De Freitas
Jun 22, 2021·Journal of the American Society for Mass Spectrometry·Shannon A RaabDavid E Clemmer
Dec 28, 2019·The Journal of Physical Chemistry. B·Emvia I CalixteElyssia S Gallagher
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Sep 25, 2021·Mass Spectrometry Reviews·Ashley PhetsanthadLingjun Li
Nov 5, 2021·Journal of the American Society for Mass Spectrometry·Emvia I CalixteElyssia S Gallagher

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