Simultaneous Sustained Drug Delivery, Tracking, and On-Demand Photoactivation of DNA–Hydrogel Formulated from a Biomass-Derived DNA Nanoparticle

Abstract

Conversion of biomass into nanoparticles for meaningful biomedical applications is a formidable proposition with excellent prospects but fewer patrons. A lack of general methodology for upscaled production and limited versatility of those nanoparticles are the main drawbacks. Herein, we report the creation of a DNA nanoparticle (DNA Dots) from onion genomic DNA (gDNA), a plant biomass source, through controlled hydrothermal pyrolysis in water without any chemicals. The DNA Dots are further formulated into a stimuli-responsive hydrogel through hybridization-mediated self-assembly with untransformed precursor gDNA. The versatility of the DNA Dots is recognized through its crosslinking ability with gDNA through its dangling DNA strands on the surface resulting from incomplete carbonization during annealing without the need for any external organic, inorganic, or polymeric crosslinkers. The gDNA–DNA Dots hybrid hydrogel is shown to be an excellent drug delivery vehicle for sustained release trackable through the inherent fluorescence of the DNA Dots. Interestingly, the DNA Dots are photoexcited with normal visible light to generate on-demand reactive oxygen species, making them exciting candidates for combination therapeutics. Most importantly, the ease with which the hydrogel is internalized in fibroblast cells with minimal cytotoxicity should encourage the nanotization of biomass as a tool for interesting sustainable biomedical applications.

A biomass-derived dual crosslinked DNA-nanoparticle hydrogel for visible light-induced photodynamic bacterial inactivation

“…By trapping the ROS with different radical scavengers, the feasible mechanism of ROS formation by the DNA-NP in the presence of visible light was determined. 16,27 Surface-generated holes (h + ) were captured using Na 2 -EDTA, superoxide (O 2 − ) was captured using p -BZQ, and hydroxyl (HO˙) radicals were captured using methanol (MeOH). When a specific radical scavenger is present, the reduction in the ROS-induced fluorescence emission of rhodamine 123 confirms the existence of that particular radical.…”

“…The decrease in the ROS induced fluorescence emission of rhodamine 123 in the presence of a particular radical scavenger indicates the presence of that radical. 16,27…”

“…This shows the importance of adding untransformed genomic DNA as a filler or a matrix material to obtain the hydrogel. 15,16…”

“…The major advantage of using DNA-NP as a material for hydrogels is the possibility of further crosslinking through hybridization-mediated self-assembly. 15,16 Such self-assembled crosslinking could be achieved through simple thermal annealing. The resulting hydrogel becomes temperature sensitive since the hydrogen bonds created during the self-assembly are heat labile.…”

Intelligent DNA-Based Hydrogels for Bioanalysis and Therapeutics

“…More importantly, biomass-derived DNA hydrogels can also be used as drug delivery carriers. Das's group 60 found that the hydrogel can easily penetrate human cells, is traceable because of its inherent fluorescence, shows excellent drug delivery properties, and produces visible lightinduced ROS, suggesting its potential application in combination therapy.…”