Chain Ejection Model for Electrospray Ionization of Unfolded Proteins: Evidence from Atomistic Simulations and Ion Mobility Spectrometry

Analytical Chemistry
Haidy MetwallyLars Konermann

Abstract

The ion evaporation model (IEM) and the charged residue model (CRM) represent cornerstones of any discussion related to the mechanism of electrospray ionization (ESI). Molecular dynamics (MD) simulations have confirmed that small ions such as Na+ are ejected from the surface of aqueous ESI droplets (IEM), while folded proteins in native ESI are released by water evaporation to dryness (CRM). ESI of unfolded proteins yields [M + zH] z+ ions that are much more highly charged than their folded counterparts. A chain ejection model (CEM) has been proposed to account for the protein ESI behavior under such non-native conditions (Konermann, L., et al. Anal. Chem. 2013, 85, 2-9). The CEM envisions that unfolded proteins are driven to the droplet surface by hydrophobic and electrostatic factors, followed by gradual ejection via intermediates where droplets carry extended protein tails. Thus far, it has not been possible to support the CEM through MD simulations using realistic protein models and atomistic force fields. Such endeavors require much larger droplets than in previous MD studies. Also, the incorporation of CEM-related H+ migration is difficult. This work overcomes these challenges in MD simulations on unfolded apo-myoglobin (...Continue Reading

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Citations

Nov 30, 2018·The Analyst·Zijie Xia, Evan R Williams
Oct 8, 2019·Chemical Science·Jean-François GreischAlbert J R Heck
Feb 28, 2020·Nature Communications·Xiaoqin ZhongRichard N Zare
Jul 25, 2019·Journal of the American Society for Mass Spectrometry·Yu-Fu LinLaurence A Angel
Nov 24, 2019·Journal of the American Society for Mass Spectrometry·Roshan JavanshadAndre R Venter
Aug 19, 2020·Journal of the American Society for Mass Spectrometry·Jacob W SilzelRyan R Julian
Aug 20, 2020·Journal of the American Society for Mass Spectrometry·J Michael SuttonMichael G Bartlett

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