Center for Electrochemistry and Department of Chemistry and Biochemistry, The University of Texas at Austin, Austin, Texas 78712, USA.
J Am Chem Soc. 2011 Sep 21;133(37):14675-85. doi: 10.1021/ja203731n. Epub 2011 Aug 26.
We report the electrochemical characterization and the observation of excimer emission from a series of 9-naphthylanthracene-based dimer- and trimer-bridged high steric hindrance aromatic groups during photoluminescence (PL) measurements in the solid state and in solution electrogenerated chemiluminescence (ECL) measurements. Cyclic voltammetry of 4,4'-bis(9-(1-naphthyl)anthracen-10-yl)biphenyl (4A) and 1,3,5-tris(9-(1-naphthyl)anthracen-10-yl)benzene (4C) showed two or three reversible, closely spaced one-electron transfers on oxidation in dichloromethane. The ECL emission spectra of 4A and 4C resulting from the annihilation reaction in benzonitrile showed two bands: one at the same wavelength as the PL peak in the solution state, and a broad band at longer wavelength. With a coreactant, such as peroxydisulfate, ECL spectra showed a single peak that was less broad in shape. PL measurement in the solid state and measurement of representative time traces of PL intensity, lifetimes, and picosecond time-correlated single-photon counting confirmed excimer emission at long wavelength. A reprecipitation method was used to prepare well-dispersed organic nanoparticles (NPs) of 4A in both aqueous and acetonitrile solutions. The smallest stable size of NPs produced was ~15 ± 6 nm, as analyzed by transmission electron microscopy. These organic NPs produced stable and weak ECL emission from the annihilation reaction in both aqueous and MeCN solutions. With a coreactant, such as peroxydisulfate, the ECL signal on reduction was sufficiently strong to obtain an ECL spectrum.
我们报告了一系列基于 9-萘基蒽的二聚体和三聚体桥联高空间位阻芳基在固态和溶液电化学发光(ECL)测量中的光电发光(PL)测量中的电化学表征和激基缔合物发射的观察。4,4'-双(9-(1-萘基)蒽-10-基)联苯(4A)和 1,3,5-三(9-(1-萘基)蒽-10-基)苯(4C)的循环伏安法显示在二氯甲烷中氧化时有两个或三个可逆的、紧密间隔的单电子转移。4A 和 4C 在前氰苯中的湮灭反应产生的 ECL 发射光谱显示两个带:一个与溶液状态下的 PL 峰在同一波长,一个在较长波长处的宽带。与核心反应物(如过二硫酸盐)一起,ECL 光谱显示出一个较窄的单峰。固态 PL 测量和代表性 PL 强度、寿命和皮秒时间相关单光子计数的时间轨迹测量证实了长波长处的激基缔合物发射。使用再沉淀方法在水和乙腈溶液中制备了 4A 的良好分散的有机纳米颗粒(NPs)。通过透射电子显微镜分析,所制备的 NPs 的最小稳定尺寸约为 15±6nm。这些有机 NPs 在水和 MeCN 溶液中的湮灭反应中产生稳定且微弱的 ECL 发射。与核心反应物(如过二硫酸盐)一起,还原时的 ECL 信号足够强,可以获得 ECL 光谱。