Abstract
Biotemplated nanomaterials offer versatile functionality for multimodal imaging, biosensing, and drug delivery. There remains an unmet need for traceable and biocompatible nanomaterials that can be synthesized in a precisely controllable manner. Here, we report self-assembled quantum dot DNA hydrogels that exhibit both size and spectral tunability. We successfully incorporate DNA-templated quantum dots with high quantum yield, long-term photostability, and low cytotoxicity into a hydrogel network in a single step. By leveraging DNA-guided interactions, we introduce multifunctionality for a variety of applications, including enzyme-responsive drug delivery and cell-specific targeting. We report that quantum dot DNA hydrogels can be used for delivery of doxorubicin, an anticancer drug, to increase potency 9-fold against cancer cells. This approach also demonstrated high biocompatibility, trackability, and in vivo therapeutic efficacy in mice bearing xenografted breast cancer tumors. This work paves the way for the development of new tunable biotemplated nanomaterials with multiple synergistic functionalities for biomedical applications.
Highlights
Biotemplated nanomaterials offer versatile functionality for multimodal imaging, biosensing, and drug delivery
There are several examples of fluorescent hydrogels that have been developed to date such as silver nanocluster DNA hydrogels, quantum dot (QD) polymers or DNA hydrogel/polymer hybrids; most require complex multi-step fabrication, have low photostabilities or quantum yields (QY), and do not possess many of the features required for biological studies[11, 17, 30,31,32]
While quantum dot DNA hydrogels (QDHs) are stable over a range of physiologically relevant temperatures and pH, they are degraded once they enter cells upon nuclease digestion
Summary
Dynamic light scattering (DLS) was used to monitor the size of QDHs synthesized with different initial concentrations (Supplementary Fig. 1a–f). We found that the diameter of QDHs increased as we increased the initial concentration of DNA-functionalized QD in a precise and predictable manner (Supplementary Fig. 2b). Based on the size of the QDH, we evaluated the various endocytic pathways as potential uptake mechanisms To this end, we pretreated the cells with inhibitors of distinct endocytic pathways with varying diameter of vesicles: dynasore (clathrin-mediated endocytosis, ~120 nm), filipin III (caveolinmediated endocytosis, ~ 60 nm), and cytochalasin D (macropinocytosis, > 1 μm). Consistent with previous reports on toxicity of QDs and other metal complexes, our initial QDHs exhibited significant toxicity in HeLa cells whereas the DNA hydrogel itself was non-toxic (Fig. 4d). We appended a DNA-based aptamer that is specific to a cell-surface receptor on CCL-119 cells to DNA sequences on the surface of QDH-80 nm QDH-100 nm QDH-140 nm b c d
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