Biomedical Engineering Center, College of Chemistry and Chemical Engineering, State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan University, Changsha 410082, People's Republic of China.
Anal Chem. 2010 Oct 15;82(20):8744-9. doi: 10.1021/ac101933y.
Real time observation of chemical reactions of individual noble metal nanoparticles (MNPs) is fundamentally important to their controlled synthesis, chemical sensing and catalysis applications. Here, with a simple and high-throughput single-molecule darkfield spectral imaging technique, we demonstrate that the reaction-induced plasmonic resonance variations of multiple MNPs could be monitored in parallel. Oxidation kinetics of individual gold nanorods (AuNRs), either immobilized on a glass substrate or moving freely in homogeneous solution, was recorded successfully. Heterogeneous reaction pathways and intermediate states unobservable in ensemble UV-visible measurements were revealed. Interestingly, the oxidation rate of individual immobilized AuNRs was much slower than that of the bulk AuNR solution, which implies the existence of a novel self-catalysis mechanism. This high-throughput darkfield spectral imaging technique could be applied to chemical reaction kinetics and heterogeneous catalysis studies of other MNPs at single particle level.
实时观察单个贵金属纳米粒子(MNPs)的化学反应对于其可控合成、化学传感和催化应用具有重要意义。在这里,我们使用一种简单、高通量的单分子暗场光谱成像技术,成功地证明了可以同时监测多个 MNPs 的反应诱导等离子体共振变化。成功地记录了单个金纳米棒(AuNRs)的氧化动力学,这些 AuNRs 要么固定在玻璃基底上,要么在均匀溶液中自由移动。揭示了在整体紫外-可见测量中不可观察的非均相反应途径和中间状态。有趣的是,单个固定 AuNRs 的氧化速率比大块 AuNR 溶液慢得多,这意味着存在一种新的自催化机制。这种高通量暗场光谱成像技术可以应用于其他 MNPs 的化学反应动力学和多相催化研究,达到单颗粒水平。