pH-Responsive Oxygen and Hydrogen Peroxide Self-Supplying Nanosystem for Photodynamic and Chemodynamic Therapy of Wound Infection

• Published in: ACS applied materials & interfaces 2021-12, Vol.13 (50), p.59720-59730
• Main Authors: Ma, Yunsu, Xu, Huanghuang, Sun, Bo, Du, Silin, Cui, Shuai, Zhang, Li, Ding, Ning, Yang, Dongzhi
• Format: Article
• Language: English
• Subjects: Anti-Bacterial Agents - chemistry; Anti-Bacterial Agents - pharmacology; Biocompatible Materials - chemistry; Biocompatible Materials - pharmacology; Biological and Medical Applications of Materials and Interfaces; Escherichia coli - drug effects; Hydrogen Peroxide - chemistry; Hydrogen Peroxide - pharmacology; Hydrogen-Ion Concentration; Imidazoles - chemistry; Imidazoles - pharmacology; Materials Testing; Microbial Sensitivity Tests; Molecular Structure; Nanoparticles - chemistry; Oxygen - chemistry; Oxygen - pharmacology; Particle Size; Photochemotherapy; Reactive Oxygen Species - metabolism; Staphylococcus aureus - drug effects; Wound Infection - drug therapy; Wound Infection - metabolism; Zeolites - chemistry; Zeolites - pharmacology
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.1c19681

The combination of photodynamic therapy (PDT) and chemodynamic therapy (CDT) has been continuously explored in the antibacterial aspect and has achieved more effective antibacterial effect than a single therapy. We design a pH-responsive O2 and H2O2 self-supplying zeolitic imidazolate framework-67 (ZIF-67) nanosystem for PDT/CDT of wound infection. Under the acidic inflammatory conditions, ZIF-67 can degrade to produce Co2+ and release CaO2 and graphene quantum dots (GQDs). The exposed CaO2 reacted with water to generate H2O2 and O2. The self-supplied O2 alleviates hypoxia at the site of inflammation and enhances external light-initiated GQD-mediated PDT, while H2O2 was catalyzed by endogenous Co2+ to produce hydroxyl radicals for Co2+-triggered CDT. In vitro and in vivo experiments confirm that CaO2/GQDs@ZIF-67 has a combined PDT/CDT effect. The antibacterial mechanism indicates that bacteria post-treated with CaO2/GQDs@ZIF-67 may be sterilized by reactive oxygen species-mediated oxidative stress and the leakage of bacterial contents. The experiments also find that CaO2/GQDs@ZIF-67 may activate the immune response and enhance the therapeutic effect by activating the cyclic GMP–AMP synthase–stimulator of interferon genes signaling pathway.