Improvements in tumor therapy require a combination of strategies where targeted treatment is critical. We developed a new versatile nanoplatform, MA@E, that generates high levels of reactive oxygen species (ROS) with effective photothermal conversions in the removal of tumors. Enhanced stability liposomes were employed as carriers to facilitate the uniform distribution and stable storage of encapsulated gold nanorods (AuNRs) and Mn-MIL-100 metal–organic frameworks, with efficient delivery of MA@E to the cytoplasm. In the targeted phagocytosis of tumor cells, MA@E can effectively deplete the reduced glutathione (GSH) with increased hydroxyl radicals that combine with Mn2+ released from Mn-MIL-100 to trigger Fenton-like reactions, generating ROS that induces cell apoptosis. Exposure to near-infrared (NIR-II) irradiation results in a AuNRs-induced thermogenic effect that expedites the release of Mn2+ and promotes Fenton-like reactions, achieving increased production of •OH. In the murine tumor model, MA@E effectively removed the implanted tumor tissue within 2 days without any obvious toxic effects. This response is attributed to a synergism involving the photothermal capability of AuNRs and ROS chemodynamic treatment. The proposed MA@E provides a new approach to utilizing unstable nanomaterials in effective tumor therapy.
Activating hydrogen peroxide (H 2 O 2 ) to produce hydroxyl radical ( • OH) (Fenton-like process) is of great importance in heterogeneous catalytic oxidations. However, most of transition metal nano-catalysts as well as recently reported carbon supported Fe-N 4 single atom catalysts (SACs) suffer from unsatisfactory catalytic performance. Herein, a novel Fe 1 /C 3 N 4 SAC with Fe-N 5 active site was constructed. Using this SAC, the electron/structure-symmetry of Fe-N 4 site can be broken by axial nitrogen-coordination, which transforms less active Fe-N 4 species into highly active Fe-N 5 species in Fenton-like reaction. Specifically, Fe-N 5 site exhibits an unprecedented activity for 3,3′,5,5′-tetramethylbenzidine oxidation, which is at least one order of magnitude more active than reported Fe-N 4 /C SACs. Mechanism studies reveal that the unique role of axial nitrogen-coordination over Fe-N x sites is to change the adsorption behavior of H 2 O over Fe-N 5 site without influencing H 2 O 2 activation. This discovery provides a new approach for rationally designing efficient catalysts in Fenton-like reactions.
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