Metal–organic frameworks (MOFs) have become a promising accommodation for enzyme immobilization and protection. However, the integration of multienzymes into MOFs may result in compromise of individual enzymatic activity. In this work, we report an iron mineralization strategy to facilely construct a mesoporous MOF, possessing excellent peroxidase-mimic bioactivity. Furthermore, the feasibility of in situ encapsulating natural enzymes within the developed mesoporous MOF nanozymes endows these natural/nanomimic enzyme hybrids with remarkably enhanced synergistic catalysis ability. Such activity enhancement is mainly due to (1) the fast flux rate of substances through the interconnected mesoporous channels and (2) the simultaneously increased loading amount of enzymes and iron within the MOFs caused by the iron mineralization process.
Chemodynamic therapy (CDT) by triggering Fenton reaction or Fenton-like reaction to generate hazardous hydroxyl radical (•OH), is a promising strategy to selectively inhibit tumors with higher H2O2 levels and relatively acidic microenvironment. Current Fe-based Fenton nanocatalysts mostly depend on slowly releasing iron ions from Fe or Fe oxide-based nanoparticles, which leads to a limited rate of Fenton reaction. Herein, we employed black phosphorene nanosheets (BPNS), a biocompatible and biodegradable photothermal material, to develop iron-mineralized black phosphorene nanosheet (BPFe) by in situ deposition method for chemodynamic and photothermal combination cancer therapy. This study demonstrated that the BPFe could selectively increase cytotoxic ·OH in tumor cells whereas having no influence on normal cells. The IC50 of BPFe for tested tumor cells was about 3–6 μg/mL, which was at least one order of magnitude lower than previous Fe-based Fenton nanocatalysts. The low H2O2 level in normal mammalian cells guaranteed the rare cytotoxicity of BPFe. Moreover, the combination of photothermal therapy (PTT) with CDT based on BPFe was proved to kill tumors more potently with spatiotemporal accuracy, which exhibited excellent anti-tumor effects in xenografted MCF-7 tumor mice models.
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