Knoblauch Rachael, Harvey Amanda, Ra Estelle, Greenberg Ken M, Lau Judy, Hawkins Elizabeth, Geddes Chris D
Institute of Fluorescence and Department of Chemistry and Biochemistry, University of Maryland Baltimore County, 701 East Pratt Street, Baltimore, Maryland 21202, USA.
Nanoscale. 2021 Jan 7;13(1):85-99. doi: 10.1039/d0nr06842j. Epub 2020 Nov 19.
The evolving threat of antibiotic resistance development in pathogenic bacteria necessitates the continued cultivation of new technologies and agents to mitigate associated negative health impacts globally. It is no surprise that infection prevention and control are cited by the Centers for Disease Control and Prevention (CDC) as two routes for combating this dangerous trend. One technology that has gained great research interest is antimicrobial photodynamic inactivation of bacteria, or APDI. This technique permits controllable activation of antimicrobial effects by combining specific light excitation with the photodynamic properties of a photosensitizer; when activated, the photosensitizer generates reactive oxygen species (ROS) from molecular oxygen via either a type I (electron transfer) or type II (energy transfer) pathway. These species subsequently inflict oxidative damage on nearby bacteria, resulting in suppressed growth and cell death. To date, small molecule photosensitizers have been developed, yet the scalability of these as widespread sterilization agents is limited due to complex and costly synthetic procedures. Herein we report the use of brominated carbon nanodots (BrCND) as new photosensitizers for APDI. These combustion byproducts are easily and inexpensively collected; incorporation of bromine into the nanodot permits photosensitization effects that are not inherent to the carbon nanodot structure alone-a consequence of triplet character gained by the heavy atom effect. BrCND demonstrate both type I and type II photosensitization under UV-A irradiation, and furthermore are shown to have significant antimicrobial effects against both Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus and Listeria monocytogenes as well. A mechanism of "dark" toxicity is additionally reported; the pH-triggered release of reactive nitrogen species is detected from a carbon nanodot structure for the first time. The results described present the BrCND structure as a competitive new antimicrobial agent for controllable sterilization of bacteria.
病原菌中抗生素耐药性不断演变的威胁使得必须持续研发新技术和制剂,以减轻全球范围内相关的负面健康影响。疾病控制与预防中心(CDC)将感染预防和控制列为对抗这一危险趋势的两条途径,这并不奇怪。一种引起广泛研究兴趣的技术是细菌的抗菌光动力灭活(APDI)。该技术通过将特定的光激发与光敏剂的光动力特性相结合,实现对抗菌效果的可控激活;激活后,光敏剂通过I型(电子转移)或II型(能量转移)途径从分子氧产生活性氧(ROS)。这些物质随后对附近的细菌造成氧化损伤,导致生长受抑制和细胞死亡。迄今为止,小分子光敏剂已被开发出来,但由于合成过程复杂且成本高昂,这些光敏剂作为广泛使用的消毒剂的可扩展性有限。在此,我们报告使用溴化碳纳米点(BrCND)作为APDI的新型光敏剂。这些燃烧副产物易于且廉价地收集;将溴掺入纳米点可产生光致敏效果,这并非仅由碳纳米点结构本身所固有,而是重原子效应赋予的三线态特性的结果。BrCND在紫外-A照射下表现出I型和II型光致敏作用,此外还显示出对革兰氏阴性大肠杆菌以及革兰氏阳性金黄色葡萄球菌和单核细胞增生李斯特菌均具有显著的抗菌作用。此外,还报道了一种“暗”毒性机制;首次从碳纳米点结构中检测到pH触发的活性氮物质释放。所描述的结果表明,BrCND结构是一种有竞争力的新型抗菌剂,可用于对细菌进行可控消毒。