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Quantifying the Electrostatics of Polycation-Lipid Bilayer Interactions.

Julianne M Troiano1, Alicia C McGeachy1, Laura L Olenick1

  • 1Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States.

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|March 31, 2017
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Polycations like poly(allylamine) hydrochloride (PAH) interact with lipid bilayers without disruption. Despite lower adsorption energy, PAH covers the membrane surface by condensing counterions, unlike its monomer allylamine hydrochloride.

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Area of Science:

  • Biophysics
  • Materials Science
  • Surface Chemistry

Background:

  • Understanding polycation-membrane interactions is crucial for controlling their behavior.
  • Molecular-level insights into polycation adsorption and membrane disruption are challenging to obtain.
  • Polycations are widely used in biomedical applications, necessitating knowledge of their membrane interactions.

Purpose of the Study:

  • To elucidate the molecular mechanisms of polycation interaction with lipid bilayers.
  • To quantify the adsorption behavior and membrane disruption potential of poly(allylamine) hydrochloride (PAH) and allylamine hydrochloride (AH).
  • To provide experimental data for refining theoretical models of polycation-membrane interactions.

Main Methods:

  • Utilized second harmonic and vibrational sum frequency generation spectroscopies.
  • Employed quartz crystal microbalance with dissipation monitoring (QCM-D).
  • Performed extensive computer simulations to model polycation-membrane interactions.

Main Results:

  • PAH adsorption to lipid bilayers was found to be reversible and non-disruptive under experimental conditions.
  • PAH exhibited a less favorable free adsorption energy (-52.7 ± 0.6 kJ/mol) compared to AH (-14.6 ± 0.4 kJ/mol).
  • PAH utilizes condensed counterions to overcome backbone repulsion and adsorb extensively onto the bilayer surface, with amine groups showing altered pKa values.

Conclusions:

  • Polycation adsorption to lipid membranes is a complex process influenced by counterion condensation and environmental factors.
  • PAH adsorption is non-disruptive, contrary to potential assumptions, and involves significant structural rearrangements.
  • The study provides critical experimental constraints for atomistic simulations, enhancing predictive models of polycation-membrane interactions.