Degradable iron-rich mesoporous dopamine as a dual-glutathione depletion nanoplatform for photothermal-enhanced ferroptosis and chemodynamic therapy.

Recent progress in MOFs-based nanozymes for biosensing

Despite recent advancements in cancer immunotherapy, challenges have yet to be surmounted to achieve two major goals of magnifying antitumor immunity and remodeling immunosuppressive tumor microenvironment. Here, a nanosystem (ODM-R) that integrates oxygen-deficient molybdenum oxide (ODM) nanosonosensitizers and R7 peptides with tumor metabolism regulation effects is designed and fabricated for synergistic sonodynamic-immunometabolic therapy of spinal-metastasized tumor. The ODM generates reactive oxygen species upon ultrasound irradiation to implement sonodynamic therapy (SDT), inducing cancer cell apoptosis and immunogenic cell death. The R7 attached on ODM markedly inhibits the uptake of glucose and excretion of lactic acid in cancer cells by perturbing the glycolysis process. The combination of SDT and tumor glycolysis obstruction by ODM-R guarantees satisfactory efficacy in synergizing with PD-L1 antibody to eradicate the spinal-metastasized tumors, achieving concurrent sonodynamic-triggered immune activation and immunosuppressive tumor microenvironment remodeling. This work provides a proof-of-concept of nanosonosensitizers for boosting cancer immunotherapy by SDT and tumor metabolic regulation. This article is protected by copyright. All rights reserved.

Peptide-appended Nanosonosensitizers Targeting Tumor Glycolysis for Synergistic Sonodynamic-Immunometabolic Therapy of Spinal-Metastasized Tumor.

Molecular oxygen as a green, non-toxic, and inexpensive oxidant has displayed numerous advantages compared with other oxidants for more sustainable and environmentally benign pollutant degradation. Molecular oxygen activation stands as a groundbreaking approach in advanced oxidation processes, offering efficient environmental remediation with minimal environmental impact with the production of high-oxidation reactive oxygen species (ROS). The adaptability and energy efficiency of molecular oxygen activation significantly contribute to the progression of sustainable water remediation technologies. This review meticulously explores the principles and mechanisms of molecular oxygen activation, shedding light on the diverse ROS production pathways. Subsequently, this review comprehensively details contemporary activation approaches, including photocatalytic activation, electrocatalytic activation, piezoelectric activation, and photothermal activation, explicating their distinct activation mechanisms. Additionally, it delves into the promising applications of molecular oxygen activation in the degradation of water pollutants, primary air pollutants, and volatile organic compounds, providing an in-depth analysis of the associated degradation pathways and mechanisms. Moreover, this review also addresses the imminent challenges and emerging opportunities in environmental remediation. It is envisioned that this comprehensive analysis will spur ongoing exploration and innovation in the use of molecular oxygen activation for environmental remediation and beyond. 

Molecular oxygen activation: Innovative techniques for environmental remediation.

Radiotherapy is inevitably accompanied by some degree of radiation resistance, which leads to local recurrence and even therapeutic failure. To overcome this limitation, herein, we report the room-temperature synthesis of an iodine- and ferrocene-loaded covalent organic framework (COF) nanozyme, termed TADI-COF-Fc, for the enhancement of radiotherapeutic efficacy in the treatment of radioresistant esophageal cancer. The iodine atoms on the COF framework not only exerted a direct effect on radiotherapy, increasing its efficacy by increasing X-ray absorption, but also promoted the radiolysis of water, which increased the production of reactive oxygen species (ROS). In addition, the ferrocene surface decoration disrupted redox homeostasis by increasing the levels of hydroxyl and lipid peroxide radicals and depleting intracellular antioxidants. Both in vitro and in vivo experiments substantiated the excellent radiotherapeutic response of TADI-COF-Fc. This study demonstrates the potential of COF-based multinanozymes as radiosensitizers and suggests a possible treatment integration strategy for combination oncotherapy. 

A Multifunctional Covalent Organic Framework Nanozyme for Promoting Ferroptotic Radiotherapy against Esophageal Cancer.

Piezocatalytic therapy is a new‐emerging reactive oxygen species (ROS)‐enabled therapeutic strategy that relies on built‐in electric field and energy‐band bending of piezoelectric materials activated by ultrasound (US) irradiation. Despite becoming a hot topic, material development and mechanism exploration are still underway. Herein, as‐synthesized oxygen‐vacancy‐rich BiO2−x nanosheets (NSs) demonstrate outstanding piezoelectric properties. Under US, a piezo‐potential of 0.25 V for BiO2−x NSs is sufficient to tilt the conduction band to be more negative than the redox potentials of O2/•O2−, •O2−/H2O2, and H2O2/•OH, which initiates a cascade reaction for ROS generation. Moreover, the BiO2−x NSs exhibit peroxidase and oxidase‐like activities to augment ROS production, especially in the H2O2‐overexpressed tumor microenvironment. Density functional theory calculations show that the generated oxygen vacancies in BiO2−x NSs are favorable for H2O2 adsorption and increasing the carrier density to produce ROS. Furthermore, the quick movement of electrons enables an excellent sonothermal effect, for example, rapid rise in temperature to nearly 65 °C upon US with low power (1.2 W cm−2) and short time (96 s). Therefore, this system realizes a multimode synergistic combination of piezocatalytic, enzymatic, and sonothermal therapies, providing a new direction for defect engineering‐optimized piezoelectric materials for tumor therapy.

Oxygen‐Vacancy‐Rich Piezoelectric BiO2−x Nanosheets for Augmented Piezocatalytic, Sonothermal, and Enzymatic Therapies

Abstract Since the discovery of enzyme-like activity of Fe 3 O 4 nanoparticles in 2007, nanozymes are becoming the promising substitutes for natural enzymes due to their advantages of high catalytic activity, low cost, mild reaction conditions, good stability, and suitable for large-scale production. Recently, with the cross fusion of nanomedicine and nanocatalysis, nanozyme-based theranostic strategies attract great attention, since the enzymatic reactions can be triggered in the tumor microenvironment to achieve good curative effect with substrate specificity and low side effects. Thus, various nanozymes have been developed and used for tumor therapy. In this review, more than 270 research articles are discussed systematically to present progress in the past five years. First, the discovery and development of nanozymes are summarized. Second, classification and catalytic mechanism of nanozymes are discussed. Third, activity prediction and rational design of nanozymes are focused by highlighting the methods of density functional theory, machine learning, biomimetic and chemical design. Then, synergistic theranostic strategy of nanozymes are introduced. Finally, current challenges and future prospects of nanozymes used for tumor theranostic are outlined, including selectivity, biosafety, repeatability and stability, in-depth catalytic mechanism, predicting and evaluating activities. 

Deep Insight of Design, Mechanism, and Cancer Theranostic Strategy of Nanozymes

Responsive nanosystems for tumor treatment with high specificity and sensitivity have aroused great attention. Herein, we develop a tumor microenvironment responsive and near-infrared (NIR)-activatable theranostic nanoreactor for imaging-guided anticancer therapy. The nanoreactor (SnO2-x@AGP) is comprised of poly(vinylpyrrolidine) encapsulated hollow mesoporous black SnO2-x nanoparticles coloaded with glucose oxidase (GOx) and 2,2'-azinobis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS). The constructed nanoreactor can be specifically activated through endogenous H2O2 by an NIR-mediated "bursting-like" process to enhance its imaging and therapeutic functions. Black SnO2-x with abundant oxygen vacancies expedites effective separation of electron-hole pairs from energy-band structure and endows them with strong hyperthermia effect upon NIR laser irradiation. The generating toxic H2O2 with the assistance of GOx provides SnO2-x@AGP with the capacity of oxidative stress therapy. Ascended H2O2 can activate ABTS into ABTS•+. ABTS•+ not only possesses significant NIR absorption properties, but also disrupts intracellular glutathione to generate excessive reactive oxygen species for improved phototherapy, leading to more effective treatment together with oxidative stress therapy. Thus, SnO2-x@AGP with NIR-mediated and H2O2-activated performance presents tumor inhibition efficacy with minimized damage to normal tissues. These outstanding characteristics of SnO2-x@AGP bring an insight into the development of activatable nanoreactors for smart, precise, and non-invasive cancer theranostics.

Tumor-Specific NIR-Activatable Nanoreactor for Self-Enhanced Multimodal Imaging and Cancer Phototherapy.

Tirapazamine-loaded UiO-66/Cu for ultrasound-mediated promotion of chemodynamic therapy cascade hypoxia-activated anticancer therapy.

Tumor Microenvironment Activated Glutathione Self-Depletion Theranostic Nanocapsules for Imaging-Directed Synergistic Cancer Therapy

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