Isolation Methods Influence the Protein Corona Composition on Gold-Coated Iron Oxide Nanoparticles

Hoang, Khoi Nguyen L.; Wheeler, Korin E.; Murphy, Catherine J.

doi:10.1021/acs.analchem.1c05243

Cited by 13 publications

(18 citation statements)

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“…Spectral images reproduced from refs , , , , and , respectively. Copyright 2019 (refs and ,), and 2015 (ref ), and 2022 (ref ), American Chemical Society. Copyright 2022 (ref ), Royal Society of Chemistry.…”

Section: Advanced Characterization Methods For Ligand Density and Lig...mentioning

confidence: 99%

“…(d) Numbers of distinct proteins discovered after NP retrieval from a total protein extract after isolation by centrifugation once or twice (C1 and C2), magnetic retrieval once or twice (M1 and M2), and that in the total protein extract (displayed as PE here). Reproduced from (d) ref . Copyright 2022, American Chemical Society.…”

Section: Categories Of Soft Surface Coatings and Ligandsmentioning

confidence: 99%

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The Landscape of Gold Nanocrystal Surface Chemistry

et al. 2023

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Conspectus Gold nanoparticles (AuNPs) exhibit unique size- and shape-dependent properties not obtainable at the macroscale. Gold nanorods (AuNRs), with their morphology-dependent optical properties, ability to convert light to heat, and high surface-to-volume ratios, are of great interest for biosensing, medicine, and catalysis. While the gold core provides many fascinating properties, this Account focuses on AuNP soft surface coatings, which govern the interactions of nanoparticles with the local environments. Postmodification of AuNP surface chemistry can greatly alter NP colloidal stability, nano-bio interactions, and functionality. Polyelectrolyte coatings provide controllable surface-coating thickness and charge, which impact the composition of the acquired corona in biological settings. Covalent modification, in which covalently bound ligands replace the original capping layer, is often performed with thiols and disulfides due to their ability to replace native coatings. N-heterocyclic carbenes and looped peptides expand the possible functionalities of the ligand layer. The characterization of surface ligands bound to AuNPs, in terms of ligand density and dynamics, remains a challenge. Nuclear magnetic resonance (NMR) spectroscopy is a powerful tool for understanding molecular structures and dynamics. Our recent NMR work on AuNPs demonstrated that NMR data were obtainable for ligands on NPs with diameters up to 25 nm for the first time. This was facilitated by the strong proton NMR signals of the trimethylammonium headgroup, which are present in a distinct regime from other ligand protons’ signals. Ligand density analyses showed that the smallest AuNPs (below 4 nm) had the largest ligand densities, yet spin–spin T2 measurements revealed that these smallest NPs also had the most mobile ligand headgroups. Molecular dynamics simulations were able to reconcile these seemingly contradictory results. While NMR spectroscopy provides ligand information averaged over many NPs, the ligand distribution on individual particles’ surfaces must also be probed to fully understand the surface coating. Taking advantage of improvements in electron energy loss spectroscopy (EELS) detectors employed with scanning transmission electron microscopy (STEM), a single-layer graphene substrate was used to calibrate the carbon K-edge EELS signal, allowing quantitative imaging of the carbon atom densities on AuNRs with sub-nanometer spatial resolution. In collaboration with others, we revealed that the mean value for surfactant-bilayer-coated AuNRs had 10–30% reduced ligand density at the ends of the rods compared to the sides, confirming prior indirect evidence for spatially distinct ligand densities. Recent work has found that surface ligands on nanoparticles can, somewhat surprisingly, enhance the selectivity and efficiency of the electrocatalytic reduction of CO2 by controlling access to the active site, tuning its electronic and chemical environment, or denying entry to impurities that poison the nanoparticle surface to facilitate ...

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Section: Advanced Characterization Methods For Ligand Density and Lig...mentioning

confidence: 99%

Section: Categories Of Soft Surface Coatings and Ligandsmentioning

confidence: 99%

The Landscape of Gold Nanocrystal Surface Chemistry

et al. 2023

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“…Other ex situ studies have used the notion of a soft corona to describe the fraction of proteins that remain on the NPs upon separation from the solvent, but come off more easily in the ensuing (repetitive) washing steps to remove the proteins (see, e.g., ref. [175]). A minireview by Weber et al [176] gives an overview of different sample treatments (centrifugation, magnetism, chromatography) for the analysis of the protein corona and evaluates their influence on the outcome, especially with regard to binding persistence.…”

Section: Soft Coronamentioning

confidence: 99%

Mechanistic Understanding of Protein Corona Formation around Nanoparticles: Old Puzzles and New Insights

Nienhaus

2023

Small

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Although a wide variety of nanoparticles (NPs) have been engineered for use as disease markers or drug delivery agents, the number of nanomedicines in clinical use has hitherto remained small. A key obstacle in nanomedicine development is the lack of a deep mechanistic understanding of NP interactions in the bio‐environment. Here, the focus is on the biomolecular adsorption layer (protein corona), which quickly enshrouds a pristine NP exposed to a biofluid and modifies the way the NP interacts with the bio‐environment. After a brief introduction of NPs for nanomedicine, proteins, and their mutual interactions, research aimed at addressing fundamental properties of the protein corona, specifically its mono‐/multilayer structure, reversibility and irreversibility, time dependence, as well as its role in NP agglomeration, is critically reviewed. It becomes quite evident that the knowledge of the protein corona is still fragmented, and conflicting results on fundamental issues call for further mechanistic studies. The article concludes with a discussion of future research directions that should be taken to advance the understanding of the protein corona around NPs. This knowledge will provide NP developers with the predictive power to account for these interactions in the design of efficacious nanomedicines.

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“…Initially, the gold coating served as a protective coating for the magnetic core, as well as an active layer for attaching bioactive molecules, as illustrated in Figure 1BI . However, even to date, not many reports on Au-coated iron oxide nanoparticles for biomedical applications have provided conclusive evidence, e.g., TEM images, that the magnetic cores were completely encapsulated in a non-porous gold coating (e.g., Hoang et al, 2022 ). Indeed, such a continuous but thin gold coating is difficult to achieve.…”

Section: Gold-iron Oxide (Au/fe 3 O 4 ...mentioning

confidence: 99%

Gold-iron oxide (Au/Fe3O4) magnetic nanoparticles as the nanoplatform for binding of bioactive molecules through self-assembly

Lau

Åhlén²,

Cheung³

et al. 2023

Front. Mol. Biosci.

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Nanomedicine plays a crucial role in the development of next-generation therapies. The use of nanoparticles as drug delivery platforms has become a major area of research in nanotechnology. To be effective, these nanoparticles must interact with desired drug molecules and release them at targeted sites. The design of these “nanoplatforms” typically includes a functional core, an organic coating with functional groups for drug binding, and the drugs or bioactive molecules themselves. However, by exploiting the coordination chemistry between organic molecules and transition metal centers, the self-assembly of drugs onto the nanoplatform surfaces can bypass the need for an organic coating, simplifying the materials synthesis process. In this perspective, we use gold-iron oxide nanoplatforms as examples and outline the prospects and challenges of using self-assembly to prepare drug-nanoparticle constructs. Through a case study on the binding of insulin on Au-dotted Fe3O4 nanoparticles, we demonstrate how a self-assembly system can be developed. This method can also be adapted to other combinations of transition metals, with the potential for scaling up. Furthermore, the self-assembly method can also be considered as a greener alternative to traditional methods, reducing the use of chemicals and solvents. In light of the current climate of environmental awareness, this shift towards sustainability in the pharmaceutical industry would be welcomed.

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Isolation Methods Influence the Protein Corona Composition on Gold-Coated Iron Oxide Nanoparticles

Cited by 13 publications

References 58 publications

The Landscape of Gold Nanocrystal Surface Chemistry

The Landscape of Gold Nanocrystal Surface Chemistry

Mechanistic Understanding of Protein Corona Formation around Nanoparticles: Old Puzzles and New Insights

Gold-iron oxide (Au/Fe3O4) magnetic nanoparticles as the nanoplatform for binding of bioactive molecules through self-assembly

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