Division of Surgery & Interventional Science, Charles Bell House, University College London, London, W1W 7EJ, UK.
Small. 2014 Dec 29;10(24):5106-15. doi: 10.1002/smll.201401209. Epub 2014 Aug 28.
Photocatalytic generation of reactive oxygen species (ROS) from quantum dots (QDs) has been widely reported yet quantitative studies of ROS formation and their quantum yields are lacking. This study investigates the generation of ROS by water soluble PEGylated CdSe/ZnS QDs with red emission. PEGylation of QDs is commonly used to confer water solubility and minimise uptake by organs of the reticuloendothelial system; therefore studies of ROS formation are of biomedical relevance. Using non-photolytic visible wavelength excitation, the superoxide anion radical is shown to be the primary ROS species generated with a quantum efficiency of 0.35%. The yield can be significantly enhanced in the presence of the electron donor, nicotinamide adenine dinucleotide (NADH), as demonstrated by oxygen consumption measurements and electron paramagnetic resonance spectroscopy with in situ illumination. Direct production of singlet oxygen is not detectable from the QDs alone. A comparison is made with ROS generation by the same QDs complexed with a sulfonated phthalocyanine which can generate singlet oxygen via Förster resonance energy transfer between the QDs and the phthalocyanine.
量子点(QD)光催化产生的活性氧(ROS)已被广泛报道,但对 ROS 形成及其量子产率的定量研究仍很缺乏。本研究考察了具有红色发射的水溶性 PEG 化 CdSe/ZnS QD 产生 ROS 的情况。QD 的 PEG 化通常用于赋予水溶性并最小化被网状内皮系统器官摄取;因此,ROS 形成的研究具有生物医学相关性。使用非光解可见波长激发,表明超氧阴离子自由基是主要的 ROS 种类,其量子效率为 0.35%。如通过氧消耗测量和原位光照下的电子顺磁共振波谱法所示,在电子供体烟酰胺腺嘌呤二核苷酸(NADH)存在下,产率可显著增强。单独的 QD 不能直接产生单线态氧。将其与与磺化酞菁复合的相同 QD 产生的 ROS 进行了比较,后者可通过 QD 和酞菁之间的Förster 共振能量转移产生单线态氧。