ROS Balance Autoregulating Core-Shell CeO2@ZIF-8/Au Nanoplatform for Wound Repair

doi:10.1007/s40820-024-01353-0

Abstract

Abstract:

Reactive oxygen species (ROS) plays important roles in living organisms. While ROS is a double-edged sword, which can eliminate drug-resistant bacteria, but excessive levels can cause oxidative damage to cells. A core-shell nanozyme, CeO₂@ZIF-8/Au, has been crafted, spontaneously activating both ROS generating and scavenging functions, achieving the multi-faceted functions of eliminating bacteria, reducing inflammation, and promoting wound healing. The Au Nanoparticles (NPs) on the shell exhibit high-efficiency peroxidase-like activity, producing ROS to kill bacteria. Meanwhile, the encapsulation of CeO₂ core within ZIF-8 provides a seal for temporarily limiting the superoxide dismutase and catalase-like activities of CeO₂ nanoparticles. Subsequently, as the ZIF-8 structure decomposes in the acidic microenvironment, the CeO₂ core is gradually released, exerting its ROS scavenging activity to eliminate excess ROS produced by the Au NPs. These two functions automatically and continuously regulate the balance of ROS levels, ultimately achieving the function of killing bacteria, reducing inflammation, and promoting wound healing. Such innovative ROS spontaneous regulators hold immense potential for revolutionizing the field of antibacterial agents and therapies.

Key words: Metal-organic framework (MOF), Reactive oxygen species (ROS), Cerium dioxide, Au nanoparticles, Wound healing

Xi Zhou, Quan Zhou, Zhaozhi He, Yi Xiao, Yan Liu, Zhuohang Huang, Yaoji Sun, Jiawei Wang, Zhengdong Zhao, Xiaozhou Liu, Bin Zhou, Lei Ren, Yu Sun, Zhiwei Chen, Xingcai Zhang. ROS Balance Autoregulating Core-Shell CeO₂@ZIF-8/Au Nanoplatform for Wound Repair[J]. Nano-Micro Letters, 2024, 16(1): 156-.

Xi Zhou, Quan Zhou, Zhaozhi He, Yi Xiao, Yan Liu, Zhuohang Huang, Yaoji Sun, Jiawei Wang, Zhengdong Zhao, Xiaozhou Liu, Bin Zhou, Lei Ren, Yu Sun, Zhiwei Chen, Xingcai Zhang. [J]. Nano-Micro Letters, 2024, 16(1): 156-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01353-0

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/156

Figures/Tables 10

Fig. 1 CeO₂@ZIF-8/Au NPs treatment and healing promoting mechanism of bacterial infected wound in mice and equations of ROS production/clearance

Fig. 2 Characterization of basic material properties. a TEM images of CeO₂, CZ and CZA. SEM images of CZA. b High resolution image of CZA and EDS elemental mapping images (Ce, Zn, N, Au). c XRD of CeO₂, ZIF-8, CZ and CZA. d Hydrodynamic diameter of CZA. e ζ-Potentials of CeO₂, ZIF-8, CZ, and CZA (Dispersed in methanol, pH = 7.0). f FT-IR spectra of CeO₂, ZIF-8, CZ and CZA

Fig. 3 Characterization of materials catalytic properties. a schematic diagram of the corresponding catalytic action of the inner (CeO₂ NPs) and outer layers (Au NPs) of CZA. b ESR spectral of various groups. c UV-vis absorption of TMB in various groups (pH 4.5): TMB, H₂O₂ + TMB, CeO₂ + H₂O₂ + TMB, CZA + TMB, CZ + H₂O₂ + TMB, CZA + H₂O₂ + TMB

Fig. 4 Characterization of catalytic kinetics and acid degradation ability of materials a The absorbance value of TMB chromogram of CZA (100 μg mL⁻¹) at varied pH values (3.5, 4.5, 5.5, and 6.5) when 5 mM H₂O₂ was added. Time-course absorbance of b Time-course absorbance of CZA with different H₂O₂ (50, 25, 12.5, and 5 mM) and Michaelis-Menten c kinetics and Lineweaver-Burk d curves of CZA. TEM images of CZA e, f after PBS treatment (pH = 7) for 4 and 8 h, g, h after acid treatment (pH = 4.5) for 4 and 8 h

Fig. 5 Characterization of antibacterial activity of materials in vitro. MIC of CZA NPs incubated with a E. coli and b S. aureus. c Agar plates photographs with remaining inoculated bacteria (above, E. coli; lower, S.aureus). d, e Bar chart of bacterial survival numbers. f TEM photographs of E. coli and S. aureus. g Protein exudation of bacterial in various group (mean ± SD, n = 3; P values: *P < 0.05, **P < 0.01, ***P < 0.001)

Fig. 6 Live/Dead staining confocal microscopy and SEM photographs of E.coli and S.aureus after different treatments

Fig. 7 Material cytotoxicity data and live and dead cytoskeleton staining In vitro cytotoxicity and apoptosis investigation. a In vitro cytotoxicity assays for different concentrations and incubation times of CZA in L929 cells. b In vitro cytotoxicity assays for different concentrations and incubation times of CZA in 293T cells. c The apoptosis of L929 cells after CZA treatments was detected by calcein AM/PI staining (Green: live cells, Red: dead cells). Scale bars: 50 μm. d Statistical chart of L929 cell survival quantity. e The apoptosis of 293T cells after CZA treatments was detected by calcein AM/PI staining (Green: live cells, Red: dead cells). Scale bars: 50 μm. f Statistical chart of 293T cell survival quantity. g Cytoskeleton staining of L929 and 293T cells (Red: cytoskeleton, Blue: nucleus). Scale bars: 5 μm

Fig. 8 Anti-inflammatory data characterization of materials In vitro CZA enhancing cell antioxidant function investigation. a Cells viabilities of L929 cells after the treatment with PBS, CZA, LPS, CZA + LPS, H₂O₂, and CZA + H₂O₂. b Cells viabilities of 293T cells after the treatment with PBS, CZA, LPS, CZA + LPS, H₂O₂, and CZA + H₂O₂. c The images of H₂O₂ induced L929 cells with oxidized DCFH-DA fluorescence treated with different components. Scale bars: 50 μm. d-f SOD1, SOD2, Caspase-3 gene expression level of L929 cell after treated with H₂O₂ or CZA + H₂O₂. g Caspase-3 gene expression level of L929 cell after treated with LPS or CZA + LPS. h-j SOD1, SOD2, Caspase-3 gene expression level of 293T cell after treated with H₂O₂ or CZA + H₂O₂. k Caspase-3 gene expression level of 293T cell treated with LPS or CZA + LPS. (mean ± SD, n = 3; P values: *P < 0.05, **P < 0.01, ***P < 0.001)

Fig. 9 CZA antibacterial/promote the healing of animal models. a Schematic diagram of anti-infection implementation scenario in vivo for CZA. b Wound area graph treated differently along time points. Scale bars: 5 mm. c Corresponding changes in relative wound area. d Mice body weight. e H&E stained photographs at wound site (gules and yellow arrows mean hair follicles and blood vessels) (mean ± standard deviation, n = 3; P values: *P < 0.05, **P < 0.01, ***P < 0.001)

Fig. 10 Images of H&E-stained heart, liver, spleen, lung, and kidney obtained from mice of PBS, CZA, and CZA + H₂O₂ groups

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