Jiang Bo, Gu Wenjie, Jiang Wenxuan, Lv Mengqi, Niu Ben, Wu Xue-Jun, Wang Wei, Wang Hui
State Key Laboratory of Analytical Chemistry for Life Science, Chemistry and Biomedicine Innovation Center (ChemBIC), School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu, 210023, China.
Key Laboratory for Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM), Nanjing University of Posts and Telecommunications, Nanjing, Jiangsu, 210023, China.
Angew Chem Int Ed Engl. 2022 Sep 26;61(39):e202209964. doi: 10.1002/anie.202209964. Epub 2022 Aug 25.
The electronic coupling between a metal electrode and single nano-entities is of unfading significance which impacts the heterogeneous electron transfer. Herein, we demonstrated a simple optical technique for directly imaging the transient interfacial electronic coupling events during electrochemical oxidation of single Ag nanoparticles on Au electrode. The electronic coupling brings out a dramatic dip behavior of bright field imaging traces, and is conductive to cross the energy barrier of oxidation for single silver nanoparticles. This dip behavior is further verified by in situ vis-transmission spectroscopy, and the heterogeneity of the Au-Ag electronic coupling down to single-nanoparticle level is uncovered by unifying the morphology and size of individual silver nanoparticles. These results suggest the interfacial electronic coupling facilitates electron transfer of single nanoparticles, and provide important insight into understanding detailed mechanism of nanoelectrochemistry.
金属电极与单个纳米实体之间的电子耦合具有持久的重要性，它会影响异质电子转移。在此，我们展示了一种简单的光学技术，用于直接成像金电极上单个银纳米颗粒电化学氧化过程中的瞬态界面电子耦合事件。电子耦合导致明场成像轨迹出现显著的下降行为，并有助于单个银纳米颗粒跨越氧化的能垒。这种下降行为通过原位可见-透射光谱进一步得到验证，并且通过统一单个银纳米颗粒的形态和尺寸，揭示了金-银电子耦合在单纳米颗粒水平上的异质性。这些结果表明界面电子耦合促进了单个纳米颗粒的电子转移，并为理解纳米电化学的详细机制提供了重要的见解。
