Issue 2, 2024

Interaction of supported phospholipid bilayers with diamond nanoparticles non-covalently functionalized with a cationic polyelectrolyte

Abstract

We use diamond nanoparticles (DNPs) wrapped in the cationic polyelectrolyte poly(allylamine) hydrochloride (PAH) and bilayers composed of either pure DOPC or a mixture of DOPC/DOPG to investigate the influence of membrane phospholipid composition and net surface charge on nanoparticle-membrane interactions and the extent of nanoparticle adhesion to supported phospholipid bilayers. Our results show that in all cases electrostatic attractions between the negatively charged bilayer and cationic PAH-DNP were responsible for the initial attachment of particles, and the lateral electrostatic repulsion between adsorbed particles on the bilayer surface determined the final extent of PAH-DNP attachment. Upon attachment, NPs attract lipids by the contact ion pairing between the ammonium groups on PAH and phosphate and glycerol groups on the lipids and acquire a lipid corona. Lipid corona formation on the PAH-DNP reduces the effective charge density of the particle and is in fact a key factor determining the final extent of NP attachment to the bilayer. Incorporation of DOPG to the bilayer leads to a decrease in efficiency and final extent of attachment compared to DOPC alone. The reduction in PAH-DNP attachment in the presence of DOPG is attributed to the adsorption of free PAH in equilibrium with bound PAH in the nanoparticle solution, thus reducing electrostatic attraction between PAH-DNPs and SLBs. This leads to an increase in hydrogen bonding interactions between lipid headgroups that limits extraction of phospholipids from the bilayer by PAH-DNP, lessening the reduction in interparticle repulsion achieved by acquisition of a lipid corona. Our results indicate that the inclusion of charged phospholipids in SLBs changes bilayer rigidity and stability and hinders the attachment of PAH-DNPs by preventing lipid extraction from the bilayer.

Graphical abstract: Interaction of supported phospholipid bilayers with diamond nanoparticles non-covalently functionalized with a cationic polyelectrolyte

Supplementary files

Article information

Article type
Paper
Submitted
31 Mot 2023
Accepted
24 Leo 2023
First published
27 Leo 2023

Environ. Sci.: Nano, 2024,11, 601-613

Author version available

Interaction of supported phospholipid bilayers with diamond nanoparticles non-covalently functionalized with a cationic polyelectrolyte

T. R. Kuech, N. Ganji, C. Anastasia, M. D. Torelli, E. S. Melby, A. C. Mensch, E. R. Caudill, R. Zimmermann, R. J. Hamers and J. A. Pedersen, Environ. Sci.: Nano, 2024, 11, 601 DOI: 10.1039/D3EN00349C

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