Surface Curvature and Aminated Side-Chain Partitioning Affect Structure of Poly(oxonorbornenes) Attached to Planar Surfaces and Nanoparticles of Gold

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dc.contributor.authorRahnamoun, Ali
dc.contributor.authorDeline, Alyssa
dc.contributor.authorZienkiewicz, Joanna
dc.contributor.authorBei, Ronghua
dc.contributor.authorZheng, Zheng
dc.contributor.authorRosenzweig, Zeev
dc.contributor.authorFairbrother, Howard
dc.contributor.authorHernandez, Rigoberto
dc.date.accessioned2022-05-27T20:36:44Z
dc.date.available2022-05-27T20:36:44Z
dc.date.issued2020-08-05
dc.description.abstractCationic amphiphilic polymers are often used to coat nanoparticles as they increase chemical stability in solution and exhibit membrane disruption activities. Among these, poly(oxonorbornenes) (PONs) are tunable membrane disruptors. They can be constructed with either one amine-terminated side chain and one hydrophobic alkyl side chain (PON-50) or two amine-terminated side chains (PON-100) on each repeat unit and can then be conjugated to gold nanoparticles using O-(2-carboxyethyl)-O′-(2-mercaptoethyl) heptaethylene glycol (HEG) spacers. While the amine content and membrane disruption activity of PONs can be controlled, the detailed structural properties of PONs conjugated to gold nanoparticles remain less understood. To address this, we performed molecular dynamics simulations of PON-50 and PON-100 to determine the nonbonded energies of PON structures as a function of amine composition. We found increasing energetic stabilization with decreasing amine composition. These results were consistent with experimental observations obtained with X-ray photoelectron spectroscopy (XPS) in which PON-100 was found to have the lowest conjugation efficiency to gold surfaces out of a range of PON amination ratios. Computationally obtained energetics suggest that replacing the aliphatic amine groups with aromatic amine groups can reverse this behavior and lead to more stable PON structures with increasing amine content. We also found that the curvature of the gold nanoparticle surface affects interactions between the surface and the amine groups of PON-50. Increasing curvature decreased these interactions, resulting in a smaller effective footprint of the HEG-PON-50 structure.en_US
dc.description.sponsorshipWe thank Dr. Karen Lienkamp for many fruitful discussions. This work was supported by National Science Foundation under the Center for Sustainable Nanotechnology (CSN), CHE-1503408. The CSN is part of the Centers for Chemical Innovation Program. Computing resources were provided in part by the National Science Foundation through XSEDE resources under Grant CTS090079 and by the Maryland Advanced Research Computing Center (MARCC).en_US
dc.description.urihttps://pubs.acs.org/doi/abs/10.1021/acs.langmuir.0c01567en_US
dc.format.extent29 pagesen_US
dc.genrejournal articlesen_US
dc.genrepostprintsen_US
dc.identifierdoi:10.13016/m2mqin-psdl
dc.identifier.citation"Rahnamoun, Ali et al. Surface Curvature and Aminated Side-Chain Partitioning Affect Structure of Poly(oxonorbornenes) Attached to Planar Surfaces and Nanoparticles of Gold. Langmuir 2020, 36, 35, 10412–10420 Publication Date:August 5, 2020. https://doi.org/10.1021/acs.langmuir.0c01567en_US
dc.identifier.urihttps://doi.org/10.1021/acs.langmuir.0c01567
dc.identifier.urihttp://hdl.handle.net/11603/24757
dc.language.isoen_USen_US
dc.publisherACSen_US
dc.relation.isAvailableAtThe University of Maryland, Baltimore County (UMBC)
dc.relation.ispartofUMBC Chemistry & Biochemistry Department Collection
dc.relation.ispartofUMBC Faculty Collection
dc.relation.ispartofUMBC Student Collection
dc.rightsThis document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Langmuir, copyright ©2020 American Chemical Society after peer review. To access the final edited and published work see https://doi.org/10.1021/acs.langmuir.0c01567en_US
dc.titleSurface Curvature and Aminated Side-Chain Partitioning Affect Structure of Poly(oxonorbornenes) Attached to Planar Surfaces and Nanoparticles of Golden_US
dc.typeTexten_US
dcterms.creatorhttps://orcid.org/0000-0001-6098-3932en_US

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