Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 117, Issue 11, Pages 5982-5992Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp312416d
Keywords
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Funding
- U.S. Department of Energy [DE-SC0002456]
- Emerging Technologies Continuing Umbrella of Research Grant from the National Cancer Institute [3U54CA132378-02S1]
- NIH [R01CA55349, P01CA33049]
- MSKCC Experimental Therapeutics Center
- MSKCC Nanotechnology Center
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1041832] Funding Source: National Science Foundation
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Carbon nanotubes internalize into cells and are potential molecular platforms for siRNA and DNA delivery. A comprehensive understanding of the identity and stability of ammonium-functionalized carbon nanotube (f-CNT)-based nucleic acid constructs is critical to deploying them in vivo as gene delivery vehicles. This work explored the capability of f-CNT to bind single- and double-strand oligonucleotides by determining the thermodynamics and kinetics of assembly and the stoichiometric composition in aqueous solution. Surprisingly, the binding affinity of f-CNT and short oligonucleotide sequences was in the nanomolar range, kinetics of complexation were extremely rapid, and from one to five sequences were loaded per nanotube platform. Mechanistic evidence for an assembly process that involved electrostatic, hydrogen bonding, and pi-stacking bonding interactions was obtained by varying nanotube functionalities, oligonucleotides, and reaction conditions. P-31 NMR and spectrophotometric fluorescence emission data described the conditions required to assemble and stably bind a DNA or RNA cargo for delivery in vivo and the amount of oligonucleotide that could be transported. The soluble oligonucleic acid-f-CNT supramolecular assemblies were suitable for use in vivo. Importantly, key evidence in support of an elegant mechanism by which the bound nucleic acid material can be off-loaded from the f-CNT was discovered.
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