Preparation and characterization of Basil essential oil nanoparticles/polyvinylpyrrolidone-polyvinyl alcohol hydrogel wound dressing
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摘要: 罗勒精油(Basil essential oil，BEO)是一种绿色、安全的抑菌剂。然而，BEO的强挥发性限制了其在抑菌伤口敷料领域的应用。本文采用纳米沉淀法制备了纳米罗勒精油(BEO@Zein(玉米醇溶蛋白))，然后将其负载在以聚乙烯吡咯烷酮(PVP)和聚乙烯醇(PVA)为基材的水凝胶上，通过冻融循环形成了BEO@Zein/PVP-PVA水凝胶伤口敷料，对BEO@Zein和水凝胶的微观形貌和结构进行表征，对水凝胶的抑菌性能、力学性能、溶胀保湿性、降解性、血液相容性进行研究。结果表明：BEO@Zein形成了以BEO为核、Zein为壳的纳米球形结构(平均粒径为56.3 nm)，显著降低了BEO挥发性。BEO@Zein/PVP-PVA水凝胶可以缓慢释放BEO，从而表现出优异的缓释抑菌性能。因此，BEO@Zein/PVP-PVA水凝胶具有良好的抑菌持久性(超过72 h)。此外，水凝胶还表现出显著的抗细菌生物膜性能。BEO@Zein/PVP-PVA水凝胶的力学性能、溶胀保湿性、降解性和血液相容性均表现良好。研究表明：BEO@Zein/PVP-PVA水凝胶是一种良好的伤口敷料材料。Abstract: Basil essential oil (BEO) is a green and safe antibacterial agent. However, the high volatility of BEO has limited its application in the field of antibacterial wound dressings. BEO nanoparticles (BEO@Zein) were prepared by nanoprecipitation method. They were then loaded on the hydrogel based on polyvinylpyrrolidone (PVP) and polyvinyl alcohol (PVA) to form BEO@Zein/PVP-PVA hydrogel wound dressing by freeze-thaw cycle. The microscopic morphology and structure of BEO@Zein and hydrogel were characterized. The antibacterial property, mechanical property, swelling and moisturizing, degradability and blood compatibility of hydrogel were studied. The results show that BEO@Zein forms a nano-spherical structure with BEO as core and Zein as shell (mean particle size is 56.3 nm), which significantly reduces the volatility of BEO. BEO@Zein/PVP-PVA hydrogel can release BEO slowly, thus exhibiting excellent slow-release antibacterial property. Therefore, BEO@Zein/PVP-PVA hydrogel has excellent antimicrobial persistence (over 72 h). In addition, the hydrogel shows remarkable antibacterial biofilm property. BEO@Zein/PVP-PVA hydrogel has good mechanical property, swelling and moisturizing, degradability, and blood compatibility. Studies have shown that BEO@Zein/PVP-PVA hydrogel can be used as a good wound dressing material.
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图 1 罗勒精油(BEO)@玉米醇溶蛋白(Zein)/聚乙烯吡咯烷酮(PVP)-聚乙烯醇(PVA)水凝胶的制备示意图
V—Volum
Figure 1. Schematic diagram of basil essential oil (BEO)@Zein/polyvinylpyrrolidone (PVP)-polyvinyl alcohol (PVA) hydrogel preparation
图 2 纳米Zein和不同质量比BEO@Zein纳米粒子的平均粒径
Figure 2. Average particle size of Zein nanoparticles and BEO@Zein nanoparticles with different mass ratios
图 3 纳米Zein和不同质量比的BEO@Zein纳米粒子悬浮液对E. coli和S. aureus的抑菌性
Figure 3. Bacteriostasis of Zein nanoparticle suspensions and BEO@Zein nanoparticle suspensions with different mass ratios against E. coli and S. aureus
图 4 纳米Zein的TEM (a)和SEM图像(c)；BEO@Zein的TEM (b)和SEM图像(d)；PVA水凝胶(e)、PVP-PVA水凝胶(f)、BEO@Zein/PVP-PVA水凝胶((g), (h))的SEM图像
Figure 4. SEM (a) and TEM (c) images of Zein nanoparticles; SEM (b) and TEM (d) images of BEO@Zein nanoparticles; SEM images of PVA hydrogel (e), PVP-PVA hydrogel (f) and BEO@Zein/PVP-PVA hydrogel ((g), (h))
图 5 水凝胶的FTIR图谱(a)、XRD图谱(b) 、DSC曲线(c)和TG曲线(d)
Figure 5. FTIR spectra (a), XRD patterns (b), DSC curves (c) and TG curves (d) of hydrogel
图 6 (a) BEO和BEO@Zein在37℃空气中的挥发率；(b) BEO@Zein/PVP-PVA水凝胶在磷酸盐缓冲溶液(PBS)中对BEO的释放；(c) BEO (以滤纸为载体)和BEO@Zein/PVP-PVA水凝胶在37℃空气中挥发36 h和72 h后对E. coli的抑菌性；(d) BEO@Zein/PVP-PVA水凝胶在模拟体液中释放BEO对E. coli和S. aureus的抑菌性
***—Significant difference (p<0.001, n =3); CFU—Colony forming units
Figure 6. (a) Volatilization ratio of BEO and BEO@Zein in 37℃ air; (b) BEO release of BEO@Zein/PVP-PVA hydrogel in phosphate buffer saline (PBS); (c) Antibacterial activity of BEO (filter paper as carrier) and BEO@Zein/PVP-PVA hydrogel on E. coli after volatilization in 37℃ air for 36 h and 72 h; (d) Bacteriostasis of BEO@Zein/PVP-PVA hydrogel releasing BEO in simulated body fluids on E. coli and S. aureus
图 7 PVP-PVA水凝胶和BEO@Zein/PVP-PVA水凝胶对E. coli (a)和S. aureus (b)持续抑菌24 h和72 h后的抑菌性；BEO@Zein/PVP-PVA水凝胶抗E. coli生物膜(c)和S. aureus生物膜(d)性能
Figure 7. Antibacterial activity of PVP-PVA hydrogel and BEO@Zein/PVP-PVA hydrogel against E. coli (a) and S. aureus (b) after 24 h and 72 h of sustained bacteriostasis; BEO@Zein/PVP-PVA hydrogel against E. coli biofilms (c) and S. aureus biofilms (d)
图 8 BEO@Zein/PVP-PVA水凝胶的缓释抑菌机制示意图
Figure 8. Schematic diagram of slow-release bacteriostatic mechanism of BEO@Zein/PVP-PVA hydrogel
图 9 (a) PVA水凝胶、8.5wt%PVA水凝胶、PVP-PVA水凝胶、PVP-8.5wt%PVA水凝胶、BEO@Zein/PVP-PVA水凝胶的应力-应变曲线；(b) PVA水凝胶、PVP-PVA水凝胶、BEO@Zein/PVP-PVA水凝胶在PBS溶液中的溶胀率曲线；(c) BEO@Zein/PVP-PVA水凝胶在37℃和25℃下的失水率曲线；(d) PVP-PVA水凝胶和BEO@Zein/PVP-PVA水凝胶在土壤和PBS溶液中的降解率曲线
Figure 9. (a) Stress-strain curves of PVA hydrogel, 8.5wt%PVA hydrogel, PVP-PVA hydrogel, PVP-8.5wt%PVA hydrogel, and BEO@Zein/PVP-PVA hydrogel; (b) Swelling ratio curves of PVA hydrogel, PVP-PVA hydrogel, and BEO@Zein/PVP-PVA hydrogel in PBS solution; (c) Water loss ratio curves of BEO@Zein/PVP-PVA hydrogel at 37℃ and 25℃; (d) Degradation ratio curves of PVP-PVA hydrogel and BEO@Zein/PVP-PVA hydrogel in soil and PBS solution
图 10 水、PBS和BEO@Zein/PVP-PVA水凝胶处理的红细胞的溶血率(a)和图像(b)；PBS (c)和BEO@Zein/PVP-PVA水凝胶(d)处理的红细胞的光学图像
*—Significant difference (** p<0.01, *** p<0.001, n = 3)
Figure 10. Hemolysis ratio (a) and pictures (b) of red blood cells treated with water, PBS and BEO@Zein/PVP-PVA hydrogel; Optical images of red blood cells treated with PBS (c) and BEO@Zein/PVP-PVA hydrogel (d)
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