Silk microfibrous mats with long-lasting antimicrobial function

doi:10.1016/j.jmst.2020.02.060

Abstract

Abstract:

The controlled release of antibiotic drugs to injured sites has great advantages over the conventional intravenous administration of antibiotics, which is associated with systemic toxicity, for wound care. Electrospun nanofibrous/microfibrous mats, with a similar structure to the native extracellular matrix, is a promising wound dressing. Herein, drug-loaded halloysite nanotubes (HNTs) incorporated into regenerated silk fibroin (RSF) microfibrous mats were prepared by electrospinning to achieve sustained drug release and long-lasting antimicrobial protection. A broad-spectrum antibiotic, tetracycline hydrochloride (TCH), was selected as the model drug. Transmission electron microscopic images revealed that the TCH-loaded HNTs were homogeneously embedded in the RSF electrospun microfibers without significant changes in morphology. The drug release profiles showed that the RSF microfibrous mats with TCH-loaded HNTs exhibited a significantly reduced burst phase and a long release time over two weeks compared to the pure TCH-loaded HNTs and the TCH-loaded RSF microfibrous mats without HNTs. These results were attributed to the two-step release of TCH first from the HNTs and then RSF matrix in the electrospun mats. Finally, the antimicrobial properties of the RSF microfibrous mats with TCH-loaded HNTs were evaluated using both Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli bacteria. The results demonstrated long-lasting antimicrobial activity for at least one week, showing the great potential of TCH-loaded RSF microfibrous mat as a wound dressing material. Therefore, these TCH-loaded RSF microfibrous mats with excellent biocompatibility and sustained antimicrobial protection are extremely attractive systems for clinical applications.

Key words: Silk protein, Inorganic nanoparticles, Electrospinning, Nano-in-micro, Hybrid materials, Antibacterial materials

Mi Wu, Wen Liu, Jinrong Yao, Zhengzhong Shao, Xin Chen. Silk microfibrous mats with long-lasting antimicrobial function[J]. J. Mater. Sci. Technol., 2021, 63: 203-209.

Figures/Tables 7

Fig. 1. TEM images of (a) the HNTs and (b) the TCH-loaded HNTs.

Fig. 2. SEM images and diameter distribution histogram of (a) pristine RSF, (b) TCH@RSF, (c) TCH@RSF-HNTs, and (d) TCH@RSF/@RSF-HNTs microfibrous mats.

Fig. 3. TEM micrograph of TCH@RSF-HNTs electrospun microfiber (a) and FTIR spectra of TCH, HNTs, TCH@HNTs, pristine RSF electrospun microfibers, and TCH@RSF-HNTs electrospun microfibers (b).

Fig. 4. In vitro drug release profiles of TCH@HNTs (a), TCH@RSF microfibrous mats (b), TCH@RSF-HNTs microfibrous mats (c), and TCH@RSF/@RSF-HNTs microfibrous mats (d). All the samples were incubated in PBS buffer solution (pH = 7.4) at 37 °C.

Fig. 5. Inhibition of E. coli (a) and S. aureus (b) growth on agar plates with TCH-loaded RSF microfibrous mats after one day of cultivation at 37 °C.

Table 1 Diameter of the inhibition zone of E. coli after daily removal of the TCH-loaded RSF microfibrous mats to a new agar plate with bacterial seeding.

Time (day)	TCH@RSF (mm)	TCH@RSF-HNTs (mm)	TCH@RSF/@RSF-HNTs (mm)
1	30.5 ± 0.3	26.8 ± 0.2	29.0 ± 0.9
2	28.1 ± 0.5	25.9 ± 0.7	26.5 ± 0.8
3	20.3 ± 1.2	23.3 ± 0.2	23.6 ± 0.2
4	13.8 ± 0.7	18.6 ± 0.4	17.9 ± 0.5
5	-	16.4 ± 0.9	14.8 ± 1.1
6	-	15.6 ± 0.3	13.6 ± 0.6
7	-	12.9 ± 0.5	12.0 ± 0.3
8	-	11.5 ± 0.7	-

Table 2 Diameter of the inhibition zone of S. aureus after daily removal of the TCH-loaded RSF microfibrous mats to a new agar plate with bacterial seeding.

Time (day)	TCH@RSF (mm)	TCH@RSF-HNTs (mm)	TCH@RSF/@RSF-HNTs (mm)
1	31.5 ± 0.4	24.2 ± 0.3	29.5 ± 0.8
2	24.5 ± 0.7	23.0 ± 0.9	26.7 ± 0.3
3	20.3 ± 0.2	20.1 ± 0.2	22.9 ± 0.7
4	17.1 ± 1.1	16.9 ± 0.5	14.5 ± 0.7
5	-	14.8 ± 0.7	13.8 ± 0.5
6	-	13.5 ± 0.3	12.6 ± 0.3
7	-	12.8 ± 0.7	-

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