Quantitatively Modeling the Equilibrium Properties of Thiol-Decorated Gold Nanoparticles

Tambasco, Michael; Kumar, Sanat K.; Szleifer, Igal

doi:10.1021/la8008046

Cited by 15 publications

(31 citation statements)

References 20 publications

(22 reference statements)

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“…However, every particle and displacement scheme is different. We stress that any measurements of ligand concentrations that are made by displacing the ligands from the docosyl mercaptan Electron Diffraction 2.14 2.5-12.5 [58] S -( C H 2 ) n -CH 3 , n=7, 11, 16 Theory 1.6-2.7…”

Section: Discussionmentioning

confidence: 99%

Determination of the surface density of polyethylene glycol on gold nanoparticles by use of microscale thermogravimetric analysis

Sebby

Mansfield

2015

Anal Bioanal Chem

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The widespread integration of nanoparticle technologies into biomedicine will depend on the ability to repeatedly create particles with well-defined properties and predictable behaviors. For this to happen, fast, reliable, inexpensive, and widely available techniques to characterize nanomaterials are needed. Characterization of the surface molecules is particularly important since the surface, including the surface molecule density, plays a dominant role in determining how nanoparticles interact with their surroundings. Here, 10 and 30 nm gold nanoparticle NIST Standard Reference Materials were functionalized with fluorescently labeled polyethylene glycol (PEG) with either thiolate or lipoic acid anchoring groups to evaluate analytical techniques for determining surface coverage. The coating of the nanoparticles was confirmed with dynamic light scattering, microscale thermogravimetric analysis (μ-TGA), and ultraviolet-visible (UV-vis) spectroscopy. A UV-vis method for determining gold nanoparticle concentrations that takes into account spectral broadening upon functionalization was developed. The amount of bound PEG was quantified with μ-TGA, a technique analogous to thermogravimetric analysis that uses quartz crystal microbalances, and fluorescence spectroscopy of displaced ligands. It is shown that μ-TGA is a convenient technique for the quantification of ligands bound to inorganic particles while sacrificing a minimal amount of sample, and the treatment of the functionalized nanoparticle dispersions with dithiothreitol may be insufficient to achieve complete displacement of the surface ligands for quantification by fluorescence measurements. The μ-TGA and fluorescence results were used to determine ligand footprint sizes-average areas occupied by each ligand on the particles' surface. The lipoic acid bound ligands had footprint sizes of 0.21 and 0.25 nm(2) on 10 and 30 nm particles, respectively while the thiolate ligands had footprint sizes of 0.085 and 0.18 nm(2).

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Section: Discussionmentioning

confidence: 99%

Determination of the surface density of polyethylene glycol on gold nanoparticles by use of microscale thermogravimetric analysis

Sebby

Mansfield

2015

Anal Bioanal Chem

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“…These results are consistent with our findings that degradation rate correlates inversely with DNA density. Because of the high curvature of nanoparticles, DNA density drops rapidly away from the nanoparticle surface (9,23). Therefore, longer DNA strands experience lower density-dependent protective effect than their shorter counterpart.…”

Section: Resultsmentioning

confidence: 99%

Controlling DNA–nanoparticle serum interactions

Zagorovsky

Chou

Chan

2016

Proc. Natl. Acad. Sci. U.S.A.

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Understanding the interaction of molecularly assembled nanoparticles with physiological fluids is critical to their use for in vivo delivery of drugs and contrast agents. Here, we systematically investigated the factors and mechanisms that govern the degradation of DNA on the nanoparticle surface in serum. We discovered that a higher DNA density, shorter oligonucleotides, and thicker PEG layer increased protection of DNA against serum degradation. Oligonucleotides on the surface of nanoparticles were highly resistant to DNase I endonucleases, and degradation was carried out exclusively by protein-mediated exonuclease cleavage and full-strand desorption. These results enabled the programming of the degradation rates of the DNA-assembled nanoparticle system from 0.1 to 0.7 h −1 and the engineering of superstructures that can release two different preloaded dye molecules with distinct kinetics and half-lives ranging from 3.3 to 9.8 h. This study provides a general framework for investigating the serum stability of DNA-containing nanostructures. The results advance our understanding of engineering principles for designing nanoparticle assemblies with controlled in vivo behavior and present a strategy for storage and multistage release of drugs and contrast agents that can facilitate the diagnosis and treatment of cancer and other diseases.nanoparticle assembly | DNA nanostructures | serum stability | serum resistance | controlled cargo release

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“…Thorough evaluation of these factors requires in-depth molecular dynamic simulations and is beyond the scope of this article. Although the influence of curvature of thiol layers on gold particle size has been studied theoretically from a thermodynamic aspect [20], to our knowledge the influence of curvature on transport properties through surfactant layers is very limited.…”

Section: Modelmentioning

confidence: 99%

“…The experimentally observed narrowing of the size distribution cannot be explained by previously published models [2,12,19,20]. Therefore, we have developed a simple model that considers the effect of the capping surfactant layer on the growth rate.…”

Section: Introductionmentioning

confidence: 96%

“…The influence of thiol monolayers on gold nanoparticles was modeled by assuming that thermodynamic equilibrium applies [20]. An important finding was that the entropic contributions from the alkyl tails together with the adsorption equilibrium of the thiols between the solution and the surface atoms of the gold core give rise to a well-defined particle size, set by the gold to thiol ratio.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Evolution of size distribution in pressure drop induced decomposition synthesis of cobalt nanoparticles

Huuppola¹,

Doan²,

Kontturi³

et al. 2010

Journal of Colloid and Interface Science

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Quantitatively Modeling the Equilibrium Properties of Thiol-Decorated Gold Nanoparticles

Cited by 15 publications

References 20 publications

Determination of the surface density of polyethylene glycol on gold nanoparticles by use of microscale thermogravimetric analysis

Determination of the surface density of polyethylene glycol on gold nanoparticles by use of microscale thermogravimetric analysis

Controlling DNA–nanoparticle serum interactions

Evolution of size distribution in pressure drop induced decomposition synthesis of cobalt nanoparticles

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