Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 3, Pages 1254-1264Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b09617
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Funding
- NIH NIDA CEBRA award [R21DA044010]
- Burroughs Wellcome Fund Career Award at the Scientific Interface (CASI)
- Simons Foundation
- Stanley Fahn PDF Junior Faculty Grant [PF-JFA-1760]
- Beckman Foundation Young Investigator Award
- DARPA Young Investigator Award
- NSF [NSF DGE 1752814]
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Noncovalent adsorption of DNA on nanoparticles has led to their widespread implementation as gene delivery tools and optical probes. Yet, the behavior and stability of DNA-nanoparticle complexes once applied in biomolecule-rich, in vivo environments remains unpredictable, whereby biocompatibility testing usually occurs in serum. Here, we demonstrate time-resolved measurements of exchange dynamics between solution-phase and adsorbed corona-phase DNA and protein biomolecules on single-walled carbon nanotubes (SWCNTs). We capture real-time binding of fluorophore-labeled biomolecules, utilizing the SWCNT surface as a fluorescence quencher, and apply this corona exchange assay to study protein corona dynamics on ssDNA-SWCNT-based dopamine sensors. We study exchange of two blood proteins, albumin and fibrinogen, adsorbing to and competitively displacing (GT)(6) vs (GT)(15) ssDNA from ssDNA-SWCNTs. We find that (GT)(15) binds to SWCNTs with a higher affinity than (GT)(6) and that fibrinogen interacts with ssDNA-SWCNTs more strongly than albumin. Albumin and fibrinogen cause a 52.2% and 78.2% attenuation of the dopamine nanosensor response, coinciding with 0.5% and 3.7% desorption of (GT)(6), respectively. Concurrently, the total surface-adsorbed fibrinogen mass is 168% greater than that of albumin. Binding profiles are fit to a competitive surface exchange model which recapitulates the experimental observation that fibrinogen has a higher affinity for SWCNTs than albumin, with a fibrinogen on-rate constant 1.61-fold greater and an off-rate constant 0.563-fold smaller than that of albumin. Our methodology presents a generic route to assess real-time corona exchange on nanoparticles in solution phase and more broadly motivates testing of nanoparticle-based technologies in blood plasma rather than the more ubiquitously tested serum conditions.
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