Department of Chemistry and ‡Department of Biology, University of Konstanz , Konstanz D-78457, Germany.
J Am Chem Soc. 2016 Mar 9;138(9):3076-84. doi: 10.1021/jacs.5b12073. Epub 2016 Feb 25.
Colonization of surfaces by microorganisms is an urging problem. In combination with the increasing antibiotic resistance of pathogenic bacteria, severe infections are reported more frequently in medical settings. Therefore, there is a large demand to explore innovative surface coatings that provide intrinsic and highly effective antibacterial activity. Materials containing silver nanoparticles have been developed in the past for this purpose, but this solution has come into criticism due to various disadvantages like notable toxicity against higher organisms, the high price, and low abundance of silver. Here, we introduce a new, sunlight-mediated organosilica nanoparticle (NP) system based on silver-free antibacterial activity. The simultaneous release of nitric oxide (NO) in combination with singlet oxygen and superoxide radicals (O2(•-)) as reactive oxygen species (ROS) leads to the emergence of highly reactive peroxynitrite molecules with significantly enhanced biocidal activity. This special cooperative effect can only be realized, if the ROS-producing moieties and the functional entities releasing NO are spatially separated from each other. In one type of particle, Rose Bengal as an efficient singlet oxygen ((1)O2) producer was covalently bound to SH functionalities applying thiol-ene click chemistry. "Charging" the second type of particles with NO was realized by quantitatively transferring the thiol groups into S-nitrosothiol functionalities. We probed the oxidation power of ROS-NP alone and in combination with NO-NP using sunlight as a trigger. The high antibacterial efficiency of dual-action nanoparticles was demonstrated using disinfection assays with the pathogenic bacterium Pseudomonas aeruginosa.
微生物对表面的定殖是一个紧迫的问题。结合致病菌对抗生素耐药性的增加,医疗环境中更频繁地报告了严重的感染。因此,迫切需要探索提供固有和高效抗菌活性的创新表面涂层。过去为此目的开发了含有银纳米粒子的材料,但由于对高等生物的明显毒性、高价格和银的低丰度等各种缺点,这种解决方案受到了批评。在这里,我们介绍了一种新的、基于阳光介导的无银抗菌活性的有机硅纳米粒子(NP)系统。一氧化氮(NO)的同时释放与单线态氧和超氧自由基(O2(•-))结合,产生具有显著增强杀菌活性的高反应性过氧亚硝酸盐分子。如果 ROS 产生部分和释放 NO 的功能实体彼此空间分离,则只能实现这种特殊的协同作用。在一种粒子中,Rose Bengal 作为一种有效的单线态氧((1)O2)产生剂,通过硫醇-烯点击化学与 SH 官能团共价结合。通过定量将巯基转化为 S-亚硝酰硫醇官能团,为第二种粒子“充电”NO。我们使用阳光作为触发,单独和组合使用 ROS-NP 来探测 ROS 的氧化能力。使用假单胞菌的消毒实验证明了双功能纳米粒子的高抗菌效率。