阳离子光敏抗菌型水凝胶的制备及性能表征
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摘要
利用蒙脱土(MMT)分别吸附3种阳离子光敏剂(meso-四(1-甲基吡啶嗡-4-基)卟吩对甲苯磺酸盐(TMPyP)、meso-四(N-甲基-4-吡啶)卟吩四氯化锌(Zn-TMPyP)、亚甲基蓝(MB)),然后均匀分散在聚乙烯醇-苯乙烯基吡啶盐缩合物(PVA-SbQ)的水溶液中,通过紫外光交联法制备出相应的光敏MMT/PS水凝胶。借助透射电子显微镜(TEM)对MMT和MMT/PS形貌结构进行分析,利用扫描电子显微镜(SEM)、热重分析仪(TGA)对3种光敏水凝胶的内部形貌、热学性能进行分析,研究其溶胀性能及对金黄色葡萄球菌的抗菌效果。结果表明:3种光敏MMT/PS水凝胶均具有良好的溶胀性能。抗菌结果显示,三者对金黄色葡萄球菌均具有一定的杀灭效果,其中负载Zn-TMPyP的水凝胶在光照条件下对金黄色葡萄球菌的杀菌率达到98.49%。
Montmorillonite(MMT) was utilized to absorb three types of cationic photosensitizers, namely, meso-tetra(4-N-methylpyridyl)porphyrine tetratosylate(TMPyP), Zn(Ⅱ) meso-tetra(N-methyl-4-pyridyl) porphine tetrachloride(Zn-TMPyP) and methylene blue(MB), the as-obtained mixtures were then evenly dispersed in aqueous polyvinyl alcohol-styrylpyridine salt condensate(PVA-SbQ) solution, corresponding photoactive MMT/PS hydrogels were prepared by the assay of UV cross-linking eventually. Transmission electron microscopy(TEM) was employed to analyse morphology of MMT and one as-prepared MMT/PS hydrogel. Scanning electron microscopy(SEM) and thermogravimetric analysis(TGA) were applied to analyse the internal morphology and thermal properties of the as-prepared hydrogels. Finally, swelling properties and antibacterial effect against staphylococcus aureus(S. aureus) were investigated. The results show that three photoactive MMT/PS hydrogels are successfully prepared with good swelling properties. The as-prepared hydrogels exhibit inactivation against S. aureus to some extent, furthermore, the hydrogel which immobilizes Zn-TMPyP reveals best inactivation efficacy, with a sterilization rate of 98.49%.
Montmorillonite(MMT) was utilized to absorb three types of cationic photosensitizers, namely, meso-tetra(4-N-methylpyridyl)porphyrine tetratosylate(TMPyP), Zn(Ⅱ) meso-tetra(N-methyl-4-pyridyl) porphine tetrachloride(Zn-TMPyP) and methylene blue(MB), the as-obtained mixtures were then evenly dispersed in aqueous polyvinyl alcohol-styrylpyridine salt condensate(PVA-SbQ) solution, corresponding photoactive MMT/PS hydrogels were prepared by the assay of UV cross-linking eventually. Transmission electron microscopy(TEM) was employed to analyse morphology of MMT and one as-prepared MMT/PS hydrogel. Scanning electron microscopy(SEM) and thermogravimetric analysis(TGA) were applied to analyse the internal morphology and thermal properties of the as-prepared hydrogels. Finally, swelling properties and antibacterial effect against staphylococcus aureus(S. aureus) were investigated. The results show that three photoactive MMT/PS hydrogels are successfully prepared with good swelling properties. The as-prepared hydrogels exhibit inactivation against S. aureus to some extent, furthermore, the hydrogel which immobilizes Zn-TMPyP reveals best inactivation efficacy, with a sterilization rate of 98.49%.
引文
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[2] 高党鸽,陈琛,吕斌,等. 原位制备季铵盐聚合物/纳米ZnO复合抗菌剂[J]. 材料工程,2015,43(6):38-45. GAO D G,CHEN C,LYU B,et al. Synthesis polymer quaternary ammonium salt/nano-ZnO composite antibacterial agent via in-situ method[J]. Journal of Materials Engineering,2015,43(6):38-45.
[3] 吕生华,李莹,杨文强,等. 氧化石墨烯/壳聚糖生物复合材料的制备及应用研究进展[J]. 材料工程,2016,44(10):119-128. LYU S H,LI Y,YANG W Q,et al. Research progress on preparation and application of graphene oxide/chitosan biocomposites[J]. Journal of Materials Engineering,2016,44(10):119-128.
[4] WAINWRIGHT M. Photodynamic antimicrobial chemotherapy (PACT)[J]. J Antimicrob Chemother,1998,42(1):13-28.
[5] SPAGNUL C,TURNER L C,BOYLE R W. Immobilized photosensitizers for antimicrobial applications[J]. J Photochem Photobiol B-Biol,2015,150:11-30.
[6] SCHLACHET I,SOSNIK A. Protoporphyrin IX-modified chitosan-g-oligo (NiPAAm) polymeric micelles: from physical stabilization to permeability characterization in vitro[J]. Biomater Sci,2017,5(1):128-140.
[7] ALVES E,FAUSTINO M A F,NEVES M,et al. Potential applications of porphyrins in photodynamic inactivation beyond the medical scope[J]. J Photochem Photobiol C-Photochem Rev,2015,22:34-57.
[8] CAVALLARO A,TAHERI S,VASILEV K. Responsive and "smart" antibacterial surfaces: common approaches and new developments (review)[J]. Biointerphases,2014,9(2):10-19.
[9] BUJDAK J,KOMADEL P. Interaction of methylene blue with reduced charge montmorillonite[J]. J Phys Chem B,1997,101(44):9065-9068.
[10] BETTANIN F,FONTINELLES T A D,MACIEL C D,et al. Aggregation of photosensitizers: the role of dispersion and solvation on dimer formation energetics[J]. Theoretical Chemistry Accounts,2015,134(12):11-23.
[11] ZHANG H F,HUSSAIN I,BRUST M,et al. Aligned two- and three-dimensional structures by directional freezing of polymers and nanoparticles[J]. Nat Mater,2005,4(10):787-793.
[12] WU J,MEREDITH J C. Assembly of chitin nanofibers into porous biomimetic structures via freeze drying[J]. ACS Macro Lett,2014,3(2):185-190.
[13] CUI J,WANG Q,WEI Q. Synthesis and characterization of cross-linked SbQ/montmorillonite composites[J]. Polymer Materials Science & Engineering,2015,31(7):159-162.
[14] ROTOMSKIS R,STRECKYTE G,BAGDONAS S. Phototransformations of sensitizers 1. significance of the nature of the sensitizer in the photobleaching process and photoproduct formation in aqueous solution[J]. J Photochem Photobiol B-Biol,1997,39:167-171.
[15] HORVATH O,HUSZANK R,VALICSEK Z,et al. Photophysics and photochemistry of kinetically labile,water-soluble porphyrin complexes[J]. Coordination Chemistry Reviews,2006,250(13/14):1792-1803.
[16] 许凤兰,李玉宝,李吉东,等. 纳米羟基磷灰石/聚乙烯醇复合水凝胶的溶胀性[J]. 材料工程,2005(7):15-18. XU F L,LI Y B,LI J D,et al.Swelling properties of nano-hydroxyaptite/polyvinyl alcohol hydrogel composite[J]. Journal of Materials Engineering,2005(7):15-18.
[17] 崔晓彤,刘金龙,张德坤,等. 不同接触尺度下PVA/HA复合水凝胶的滑动摩擦行为[J]. 材料工程,2016,44(5):59-64. CUI X T,LIU J L,ZHANG D K,et al. Sliding friction behavior of PVA/HA composite hydrogels under different contacting scales[J]. Journal of Materials Engineering,2016,44(5):59-64.
[18] GOMEZ I,OTAZO E M,HERNANDEZ H,et al. Thermal degradation study of PVA derivative with pendant phenylthionecarbamate groups by DSC/TGA and GC/MS[J]. Polym Degrad Stabil,2015,112:132-136.
[19] XU J,BAI H Y,WANG M,et al. Properties of hyaluronan/PVA-SbQ composite films processed by casting[J]. Polymers & Polymer Composites,2013,21(1):55-60.
[20] REDMOND R W,GAMLIN J N. A compilation of singlet oxygen yields from biologically relevant molecules[J]. Photochem Photobiol,1999,70(4):391-475.
[21] ZHAO Z,LI Y,MENG S,et al. Susceptibility of methicillin-resistant staphylococcus aureus to photodynamic antimicrobial chemotherapy with α-d-galactopyranosyl zinc phthalocyanines:in vitro study[J]. Lasers in Medical Science,2014,29(3):1131-1138.
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