Synergistic Interaction between Metal Single-Atoms and Defective WO3- x Nanosheets for Enhanced Sonodynamic Cancer Therapy.

Although metal single-atom (SA)-based nanomaterials are explored as sonosensitizers for sonodynamic therapy (SDT), they normally exhibit poor activities and need to combine with other therapeutic strategies. Herein, the deposition of metal SAs on oxygen vacancy (OV)-rich WO3- x nanosheets to generate a synergistic effect for efficient SDT is reported. Crystalline WO3 and OV-rich WO3- x nanosheets are first prepared by simple calcination of the WO3·H2O nanosheets under an air and N2 atmosphere, respectively. Pt, Cu, Fe, Co, and Ni metal SAs are then deposited on WO3- x nanosheets to obtain metal SA-decorated WO3- x nanocomposites (M-WO3- x). Importantly, the Cu-WO3- x sonosensitizer exhibits a much higher activity for ultrasound (US)-induced production of reactive oxygen species than that of the WO3- x and Cu SA-decorated WO3, which is also higher than other M-WO3- x nanosheets. Both the experimental and theoretical results suggest that the excellent SDT performance of the Cu-WO3- x nanosheets should be attributed to the synergistic effect between Cu SAs and WO3- x OVs. Therefore, after polyethylene glycol modification, the Cu-WO3- x can quickly kill cancer cells in vitro and effectively eradicate tumors in vivo under US irradiation. Transcriptome sequencing analysis and further molecular validation suggest that the Cu-WO3- x-mediated SDT-activated apoptosis and TNF signaling pathways are potential drivers of tumor apoptosis induction.

Catalyzing Generation and Stabilization of Oxygen Vacancies on CeO2-x Nanorods by Pt Nanoclusters as Nanozymes for Catalytic Therapy.

Although CeO2 nanomaterials have been widely explored as nanozymes for catalytic therapy, they still suffer from relatively low activities. Herein, the catalyzing generation and stabilization of oxygen vacancies on CeO2 nanorods by Pt nanoclusters via H2 gas reduction under mild temperature (350 °C) to obtain Pt/CeO2- x , which can serve as a highly efficient nanozyme for catalytic cancer therapy, is reported. The deposited Pt on CeO2 by the atomic layer deposition technique not only can serve as the catalyst to generate oxygen vacancies under mild temperature reduction through the hydrogen spillover effect, but also can stabilize the generated oxygen vacancies. Meanwhile, the oxygen vacancies also provide anchoring sites for Pt forming strong metal-support interactions and thus preventing their agglomerations. Importantly, the Pt/CeO2- x reduced at 350 °C (Pt/CeO2- x -350R) exhibits excellent enzyme-mimicking catalytic activity for generation of reactive oxygen species (e.g., ·OH) as compared to other control samples, including CeO2 , Pt/CeO2 , and Pt/CeO2- x reduced at other temperatures, thus achieving excellent performance for tumor-specific catalytic therapy to efficiently eliminate cancer cells in vitro and ablate tumors in vivo. The excellent enzyme-mimicking catalytic activity of Pt/CeO2- x -350R originates from the good catalytic activities of oxygen vacancy-rich CeO2- x and Pt nanoclusters.

Peroxidase-like MoS2/Ag nanosheets with synergistically enhanced NIR-responsive antibacterial activities.

Pathogenic microbial infections have been threatening public health all over the world, which makes it highly desirable to develop an antibiotics-free material for bacterial infection. In this paper, molybdenum disulfide (MoS2) nanosheets loaded with silver nanoparticles (Ag NPs) were constructed to inactive bacteria rapidly and efficiently in a short period under a near infrared (NIR) laser (660 nm) in the presence of H2O2. The designed material presented favorable features of peroxidase-like ability and photodynamic property, which endowed it with fascinating antimicrobial capacity. Compared with free MoS2 nanosheets, the MoS2/Ag nanosheets (denoted as MoS2/Ag NSs) exhibited better antibacterial performance against Staphylococcus aureus by the generated reactive oxygen species (ROS) from both peroxidase-like catalysis and photodynamic, and the antibacterial efficiency of MoS2/Ag NSs could be further improved by increasing the amount of Ag. Results from cell culture tests proved that MoS2/Ag3 nanosheets had a negligible impact on cell growth. This work provided new insight into a promising method for eliminating bacteria without using antibiotics, and could serve as a candidate strategy for efficient disinfection to treat other bacterial infections.

Growth of Cu2O Nanoparticles on Two-Dimensional Zr-Ferrocene-Metal-Organic Framework Nanosheets for Photothermally Enhanced Chemodynamic Antibacterial Therapy.

Two-dimensional (2D) metal-organic framework (MOF) nanosheets have been demonstrated to be promising templates for the growth of various kinds of nanomaterials on their surfaces to construct novel 2D composites, thus realizing enhanced performance in various applications. Herein, we report the growth of Cu2O nanoparticles on 2D Zr-ferrocene (Zr-Fc)-MOF (Zr-Fc-MOF) nanosheets to prepare 2D composites for near-infrared (NIR) photothermally enhanced chemodynamic antibacterial therapy. The uniform Zr-Fc-MOF nanosheets are synthesized using the solvothermal method, followed by ultrasound sonication, and Cu2O nanoparticles are then deposited on its surface to obtain the Cu2O-decorated Zr-Fc-MOF (denoted as Cu2O/Zr-Fc-MOF) 2D composite. Promisingly, the Cu2O/Zr-Fc-MOF composite shows higher chemodynamic activity for producing ·OH via Fenton-like reaction than that of the pristine Zr-Fc-MOF nanosheets. More importantly, the chemodynamic activity of the Cu2O/Zr-Fc-MOF composite can be further enhanced by the photothermal effect though NIR laser (808 nm) irradiation. Thus, the Cu2O/Zr-Fc-MOF composite can be used as an efficient nanoagent for photothermally enhanced chemodynamic antibacterial therapy.