Bacteriostatic performance and mechanism of Ag quantum dots synergistic tetracycline
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摘要: 四环素类抗生素因具有高效、低毒、广谱抑菌性等优点而被广泛使用，但随着抗生素的滥用致使大量的耐药菌出现，使四环素类抗生素的药用价值逐渐降低。超小粒径的纳米Ag虽可使细菌甚至耐药菌失活，但单独使用毒性较强，且易团聚。为此，本研究利用Ag的d轨道为满电子结构，可与供电子基团配位的原理，设计了核壳型介孔Fe3O4@SiO2@mTiO2@Ag-四环素(FSmTA-T)复合材料用以解决抗生素耐药和纳米Ag团聚、强毒性问题。研究结果显示，制备的复合材料中纳米Ag量子点的粒径约为2.84 nm，可与四环素环3中的羰基键合，同时，相比四环素，复合材料对大肠杆菌，金黄色葡萄球菌，耐四环素沙门氏菌和白色念珠菌均具有较高的抑菌活性，并可有效破坏细菌细胞壁而使其死亡，且对哺乳细胞的毒性降低为原来的1/3。因此，其优越的抑菌活性可应用于污水处理领域。Abstract: Tetracycline antibiotics are widely used because of their high efficiency, low toxicity and broad-spectrum bacteriostasis, but with the abuse of antibiotics leading to the emergence of a large number of resistant bacteria, the medicinal value of tetracycline antibiotics gradually decreases. Although the ultra-small particle size of Ag can inactivate bacteria and even drug-resistant bacteria, it is highly toxic and easy to agglomerate when used alone. Therefore, in this study, the core-shell mesoporous Fe3O4@SiO2@mTiO2@Ag-tetracycline (FSmTA-T) composite was designed to solve the problems of antibiotic resistance, Ag nanoparticles agglomeration and strong toxicity by using the principle that the d orbital of Ag is a full electron structure and can be coordinated with the electron donor group. The results showed that the particle size of the Ag quantum dots in the prepared composite was 2.84 nm, which could be bonded with the carbonyl group in tetracycline ring 3, and compared with tetracycline, the composite material had high bacteriostatic activity against Escherichia coli, Staphylococcus aureus, tetracycline-resistant Salmonella and Candida albicans, and could effectively destroy the bacterial cell wall and make it die, while the toxicity was reduced to 1/3 of the original. Therefore, its superior bacteriostatic activity can be applied to sewage treatment.
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Key words:
- bacteriostasis /
- nanocomposite material /
- antibacterial mechanism /
- tetracycline /
- drug resistance /
- Ag quantum dots
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图 1 Fe3O4@SiO2@mTiO2@Ag-四环素(FSmTA-T)的制备原理示意图
Figure 1. Schematic diagram of the preparation principle of the Fe3O4@SiO2@mTiO2@Ag-tetracycline (FSmTA-T)
图 2 F(a)、FS (b)、FST (c)、FSmT (d)、FSmTA-T (e)和Ag (f)的TEM图
Figure 2. TEM image of F (a)，FS (b)，FST (c)，FSmT (d)，FSmTA-T (e) and Ag
图 3 (a)为Ag量子点的粒径分布，(b)是EDX分析结果，(c)和(d)为XRD和VSM分析结果，(e)是不同样品的紫外分析结果，(f)是FSmTA-T的XPS全谱
Figure 3. The particle size distribution of Ag quantum dots (a), EDX spectrum result (b), XRD (c) and VSM (d) spectrum, UV absorption spectra of different samples (e), XPS spectrum of the FSmTA-T (f)
图 4 (a-f)依次为C 1s, Fe 2p, N 1s, O 1s, Si 2p和Ti 2p的XPS图谱
Figure 4. XPS spectra of C 1s (a), Fe 2p (b), N 1s (c), O 1s (d), Si 2p (e) and Ti 2p (f)
图 5 (a)为 Ag XPS图谱，(b)、(c)为材料的Zeta和FT-IR谱图结果，(d)、(e)为Ag量子点结合T的MS计算和对应的数据分析
Figure 5. XPS spectra of Ag 3 d (a), the Zeta (b) and FT-IR (c) spectra of different materials, MS theoretical calculation results of the Ag quantum dot bonding T (d) and corresponding data (e)
图 6 (a-d)是FSmTA-T对E. coli、S. aureus、T-Salm和C. albicans的最小抑菌浓度测试照片
Figure 6. MIC test photos of FSmTA-T on E. coli (a), S. aureus (b), T-Salm (c) and C. albicans (d)
图 7 (a-d)是不同材料对E. coli、S. aureus、T-Salm和C. albicans的滤纸片扩散照片，O为对照，A，B，C和D依次为Ag、T、FSmTA和FSmTA-T
Figure 7. Paper diffusion photos of of different samples on E. coli (a), S. aureus (b), T-Salm (c) and C. albicans (d). O is the control, A, B, C and D are Ag、T、FSmTA and FSmTA-T, respectively
a1~e1: 25 µg/mL; a2~e2: 50 µg/mL; a3~e3: 100 µg/mL; a4~e4: 150 µg/mL; a5~e5: 200 µg/mL
图 8 (a-d)是FSmTA-T对E. coli、S. aureus、T-Salm和C. albicans的菌落计数实验结果，O为对照，A，B，C和D依次为10、20、30和40 min
Figure 8. Photographs of the results of colony counting experiments of FSmTA-T on E. coli (a), S. aureus (b), T-Salm (c) and C. albicans (d). O is the control, A, B, C and D are 10、20、30 and 40 min
图 9 (a)为MIC抑菌数据结果，(b-e)为材料对E. coli、S. aureus、T-Salm和C. albicans滤纸片扩散分析结果数据，(f)为 FSmTA-T对菌的菌落计数分析结果
Figure 9. Antibacterial data results of MIC (a)，The results of filter paper diffusion analysis of E. coli (b), S. aureus (c), T-Salm (d) and C. albicans (d) by materials. The FSmTA-T on bacterial colony count analysis data results (f)
图 10 (a1-a4)，(b1-b4)分别为FSmTA-T对E. coli、S. aureus、T-Salm 和C. albicans 的PI染色结果，(c)为Zeta电势分析结果，(d)为GDC-0941、T、Ag和FSmTA-T对MCF-7细胞活力的影响
Figure 10. PI staining analysis of FSmTA-T on E. coli (a1, b1), S. aureus (a2, b2), T-salm (a3, b3) and C. albican (a4, b4). Zeta potential analysis results (c). Viability of MCF-7 cells exposed to GDC-0941, T, Ag and FSmTA-T (d)
图 11 FSmTA-T对E. coli、S. aureus、T-Salm和C. albicans的核酸泄露(a-d)分析结果
Figure 11. DNA leakage analysis of FSmTA-T on E. coli (a), S. aureus (b), T-Salm (c) and C. albicans (d)
图 12 (a-d)是FSmTA-T对E. coli、S. aureus、T-Salm和C. albicans的微量热分析
Figure 12. Microcalorimetric analysis of E. coli (a), S. aureus (b), T-Salm (c) and C. albicans (d)
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