Molecular Interactions at the Interface of Engineered Nanoparticles and Biological Membranes
EMSL Project ID
47975
Abstract
The proposed project focuses on applying EMSL's outstanding capabilities in super resolution and single-molecule fluorescence microscopy (Galya Orr), high-resolution vibrational spectroscopy (hr-SFG) (Hongfei Wang), and all-atom molecular dynamics (MD) simulations (Ping Yang) to conduct molecular scale studies of nanoparticle (NP) interaction with model lipid membranes. This research will lead to a fundamental understanding of molecular interactions at the interface between nanomaterials and living cells and provide guiding rules to enable innovative and safe nanotechnology. The proposed studies build on on-going work in the laboratories of Pedersen (model cell membranes) and Geiger (SFG) on NP-membrane interaction that employ NPs with precisely controlled sizes, shapes, and sophisticated surface ligands, synthesized by the Hamers and Murphy groups. The specific aims of the proposed project are to (1) determine the influence of NP properties, in particular charge and charge density, on co-localization with membrane domains/components and penetration through the bilayer; (2) examine the extent to which interaction with NPs cause structural rearrangement of lipid membranes; and (3) investigate the energetics and atomic-level interactions between NPs and membrane lipids. We hypothesize that NP binding to lipid bilayers is driven primarily by electrostatic attraction between the lipid head groups and the termini of functionalizing ligands on the NP surfaces and that the degree of lipid bilayer penetration increases with increasing NP charge density. In addition, we expect NPs bearing amphiphilic ligands to be able to penetrate lipid bilayers. We further hypothesize that interaction of NPs with lipid bilayers alters membrane order and that membrane penetration is larger in regions of higher intrinsic disorder. The proposed integrated experimental and computational studies will provide new understanding of the interactions that occur between highly reactive nano-surfaces and complex biological systems, directly addressing the focus topic under Science of Interfacial Phenomena, seeking to "advance the fundamental understanding of chemical processes at complex interfaces associated with advanced materials including materials/biological interfaces." We expect this research to yield increased molecular understanding of NP localization in lipid membranes and accompanying lipid rearrangements and/or membrane disruption, ultimately enabling nanotechnological discoveries and innovations.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2015-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Dogangun M, MN Hang, J Troiano, AC McGeachy, ES Melby, JA Pedersen, RJ Hamers, and FM Geiger. 2015. "Alteration of Membrane Compositional Asymmetry by LiCoO? Nanosheets." ACS Nano 9(9):8755–8765. doi:10.1021/acsnano.5b01440
Dominguez GA, SE Lohse, M Torelli, C Murphy, RJ Hamers, G Orr, and RD Klaper. 2015. "Effects of charge and surface ligand properties of nanoparticles on oxidative stress and gene expression within the gut of Daphnia magna." Aquatic Toxicology 162:1-9. doi:10.1016/j.aquatox.2015.02.015
Gunsolus IL, D Hu, C Mihai, SE Lohse, CS Lee, M Torelli, RJ Hamers, C Murphy, G Orr, and CL Haynes. 2014. "Facile method to stain the bacterial cell surface for super-resolution fluorescence microscopy." Analyst 139(12):3174-3178. doi:10.1039/c4an00574k
Jacobson KH, IL Gunsolus, TR Kuech, JM Troiano, ES Melby, SE Lohse, D Hu, WB Chrisler, C Murphy, G Orr, FM Geiger, CL Haynes, and JA Pedersen. 2015. "Lipopolysaccharide density and structure governs the extent and distance of nanoparticle interaction with actual and model bacterial outer membranes." Journal of Environmental Science and Technology. doi:10.1021/acs.est.5b01841
Melby ES, AC Mensch, SE Lohse, D Hu, G Orr, C Murphy, RJ Hamers, and JA Pedersen. 2015. "Formation of supported lipid bilayers containing phase-segregated domains and their interaction with gold nanoparticles." Environmental Science: Nano. doi:10.1039/C5EN00098J
Murphy C, AM Vartanian, FM Geiger, RJ Hamers, JA Pedersen, Q Cui, CL Haynes, EE Carlson, R Hernandez, RD Klaper, G Orr, and Z Rosenzweig. 2015. "Biological Responses to Engineered Nanomaterials: Needs for the Next Decade." ACS Central Science 1(3):117-123. doi:10.1021/acscentsci.5b00182
Troiano J, LL Olenick, TR Kuech, ES Melby, D Hu, SE Lohse, AC Mensch, M Dogangun, AM Vartanian, M Torelli, E Ehimiaghe, SR Walter, L Fu, CR Anderton, Z Zhu, C Murphy, H Wang, G Orr, RJ Hamers, JA Pedersen, and FM Geiger. 2014. "Direct Probes of 4-nm Diameter Gold Nanoparticles Interacting with Supported Lipid Bylayers." Journal of Physical Chemistry C. doi:10.1021/jp512107z