Journal
ACS NANO
Volume 16, Issue 11, Pages 18232-18243Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c05710
Keywords
Nanozyme; DNA nanotechnology; Peroxidase; Oxidase; Reactive oxygen species (ROS); Chemodynamic cancer therapy
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Funding
- Israel Ministry of Science and Technology
- Shanghai Jiao Tong University, Shanghai, China-The Hebrew University of Jerusalem cooperation program
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Polyadenine-stabilized Au nanoparticles (pA-AuNPs) exhibit dual nanozyme catalytic activities for the oxidation reactions of dopamine and glucose. The conjugation of a dopamine-binding aptamer (DBA) to pA-AuNPs enhances the catalytic activity. The aptananozymes can also be targeted to cancer cells and demonstrate selective cytotoxicity.
Polyadenine-stabilized Au nanoparticles (pA-AuNPs) reveal dual nanozyme catalytic activities toward the H2O2-mediated oxidation of dopamine to aminochrome and toward the aerobic oxidation of glucose to gluconic acid and H2O2. The conjugation of a dopamine-binding aptamer (DBA) to the pA-AuNPs yields aptananozyme structures catalyzing simultaneously the H2O2-mediated oxidation of dopamine to aminochrome through the aerobic oxidation of glucose. A set of aptananozymes consisting of DBA conjugated through the 5'- or 3'-end directly or spacer bridges to pA-AuNPs were synthesized. The set of aptananozymes revealed enhanced catalytic activities toward the H2O2-catalyzed oxidation of dopamine to dopachrome, as compared to the separated pA-AuNPs and DBA constituents, and structure-function relationships within the series of aptananozymes were demonstrated. The enhanced catalytic function of the aptananozymes was attributed to the concentration of the dopamine at the catalytic interfaces by means of aptamer-dopamine complexes. The dual catalytic activities of aptananozymes were further applied to design bioreactors catalyzing the effective aerobic oxidation of dopamine in the presence of glucose. Mechanistic studies demonstrated that the aptananozymes generate reactive oxygen species. Accordingly, the AS1411 aptamer, recognizing the nucleolin receptor associated with cancer cells, was conjugated to the pA-AuNPs, yielding a nanozyme for the chemodynamic treatment of cancer cells. The AS1411 aptamer targets the aptananozyme to the cancer cells and facilitates the selective permeation of the nanozyme into the cells. Selective cytotoxicity toward MDA-MB-231 breast cancer cells (ca. 70% cell death) as compared to MCF-10A epithelial cells (ca. 2% cell death) is demonstrated.
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