Nanostructured electrode materials have been extensively studied with the aim of enhancing lithium ion and electron transport and lowering the stress caused by their volume changes during the charge–discharge processes of electrodes in lithium-ion batteries.
Bioorthogonal chemistry, referring to the rapid and selective synthesis of imaging and/or therapeutic molecules in live animals via transition metal‐mediated non‐natural chemical transformation without disrupting endogenous reactions, has greatly expanded the tools and techniques for biomedicine. However, owing to safety concerns associated with metal toxicity, selectivity, sensitivity and stability, efficient bioorthogonal reactions that can be reliably executed in complex biological environments remain challenging. In this study, an intelligent, versatile bioorthogonal catalyst based on ultrasmall poly(acrylic acid)‐modified copper nanocomplexes (Cu@PAA NCs) to achieve high spatiotemporal catalytic efficacy is established. The catalytic activity of the Cu@PAA NCs can be reversibly regulated via valence state interconversion between Cu(II) and Cu(I) under exogenous ultrasound irradiation, promoting off‐target prodrug activation in lesion sites through the Cu(I)‐catalyzed azide–alkyne cycloaddition reaction. Moreover, ultrasound‐triggered electron–hole separation endows the Cu@PAA NCs with robust sonosensitizing ability for sonodynamic therapy. Furthermore, the Cu@PAA NCs exhibit enhanced contrast in magnetic resonance and photoacoustic imaging. Notably, the renal‐clearable Cu@PAA NCs exhibit intrinsically benign biocompatibility. This spatiotemporally ultrasound‐mediated bioorthogonal catalysis not only expands the repertoire of in situ therapeutic agents but also provides a new avenue for disease theranostics.
The effective deployment of reactive oxygen species (ROS)-mediated oncotherapy in practice remains challenging, mired by uncontrollable catalytic processes, stern reaction conditions and safety concerns. Herein, we develop a copper nanodot integrating sonodynamic and catalytic effects within one active center, which responds to exogenous ultrasound (US) and endogenous H 2 O 2 stimuli. US irradiation induces the valence conversion from Cu II to Cu I catalyzing H 2 O 2 into * OH for chemodynamic therapy. Meanwhile, valence transformation results in electron-hole pairs separation, promoting ROS generation for sonodynamic therapy. Notably, copper nanodots not only block lysosome fusion and degradation leading to autophagy flux blockage, but also interfere with the glutathione peroxidase 4 and cystine-glutamate antiporter SLC7A11 function achieving ferroptosis. Furthermore, reversible valence changes, inherent hydrophilicity and renal clearance ultrasmall size guarantee biosafety.
The emerging chemodynamic therapy employs an iron‐based catalytic Fenton reaction to transform less‐reactive endogenous hydrogen peroxide within the tumor microenvironment (TME) into a highly toxic hydroxyl radical for killing cancer cells. However, the effective deployment of chemodynamic modality remains challenging, mired by a paucity of Fenton agents and overexpressed antioxidant glutathione (GSH) in cancer cells. Herein, a clay‐based 2D vermiculite nanosheet as a self‐reinforcing chemodynamic nanoagent for efficient lung cancer treatment is engineered. The engineered 2D vermiculite nanosheets are not only biocompatible with normal cells but also capable of regulating the TME through depleting GSH, which ameliorates the antioxidant activity of cancer cells. Meanwhile, GSH consumption results in increased intracellular reactive oxygen species content and enhanced lipid peroxidation level, thus inducing ferroptosis and augmenting chemodynamic cell‐killing efficacy. In particular, the ferrous oxidase hephaestin is the direct therapeutic target for 2D vermiculite nanosheets to fight against lung cancer cells. Systematic in vivo evaluations on a xenografted tumor model verify the favorable biosafety and effective tumor suppression capacity of the engineered 2D vermiculite nanosheets‐mediated chemodynamic tumor therapy by inducing desirable ferroptosis. Therefore, the developed vermiculite nanosheets represent the paradigm of 2D ferroptosis‐inducing nanomedicine for synergistic and efficient cancer treatment.
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