Journal
ACS APPLIED NANO MATERIALS
Volume 4, Issue 9, Pages 8690-8698Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c00707
Keywords
flocculation; flash nanoprecipitation; FNP; confocal microscopy; nanoparticle concentration; lumefantrine; malaria; polyelectrolyte; pH responsive
Funding
- Bill and Melinda Gates Foundation (BMGF) [OPP1150755]
- National Science Foundation [DGE-1656466]
- Bill and Melinda Gates Foundation [OPP1150755] Funding Source: Bill and Melinda Gates Foundation
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This study presents a reversible pH-driven flocculation technique for concentrating nanoparticles stabilized with a carboxylic acid-bearing cellulose polymer, which significantly reduces the drying time and improves particle retention efficiency. The flocculation process is found to be effective in separating amphiphilic polyelectrolyte-coated nanoparticles from suspension for advanced processing, demonstrating a potential method for nanoparticle concentration and drying.
Nanoformulating poorly water-soluble drugs is attractive for improving oral dissolution kinetics, but concentrating and drying dilute nanoparticle (NP) suspensions is a barrier to translation. This work describes a reversible, pH-driven flocculation technique for concentrating NPs stabilized with a carboxylic acid-bearing cellulose polymer. Lumefantrine NPs 150 nm in diameter stabilized by anionic hydroxypropylmethylcellulose acetate succinate, a Food and Drug Administration-approved pharmaceutical polymer excipient, are prepared using flash nanoprecipitation. Particles are then concentrated 50-fold by acid-induced flocculation at pH 2.0, separation (either filtration or centrifugation), and base-induced redispersion at pH 6.9, reducing the drying time 50-fold. Dried powders retain enhanced lumefantrine dissolution kinetics. Filtration efficiency is assessed, and flocculation is found to improve NP retention from 3 to 85% on a 2.5 mu m filter. The kinetics of flocculation and the fractal nature of the flocs are studied using confocal microscopy and agree closely with a diffusion-limited aggregation model. These results demonstrate a proof of concept that reversible flocculation is a facile method for separating amphiphilic polyelectrolyte-coated NPs from suspension for advanced processing.
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