Ma Hui, Chen Jian-Fu, Wang Hai-Feng, Hu Pei-Jun, Ma Wei, Long Yi-Tao
School of Chemistry and Molecular Engineering, East China University of Science and Technology, 200237, Shanghai, P. R. China.
State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, 210023, Nanjing, P.R. China.
Nat Commun. 2020 May 8;11(1):2307. doi: 10.1038/s41467-020-16149-0.
With the development of new instruments and methodologies, the highly dynamic behaviors of nanoparticle at the liquid-solid interface have been studied. However, the dynamic nature of the electrochemical behavior of individual nanoparticles on the electrode interface is still poorly understood. Here, we generalize scaling relations to predict nanoparticle-electrode interactions by examining the adsorption energy of nanoparticles at an ultramicroelectrode interface. Based on the theoretical predictions, we investigate the interaction-modulated dynamic electrochemical behaviors for the oxidation of individual Ag nanoparticles. Typically, significantly distinct current traces are observed owing to the adsorption-mediated motion of Ag nanoparticles. Inspired by restraining the stochastic paths of particles in the vicinity of the electrode interface to produce surface-confined current traces, we successfully realize high-resolution size measurements of Ag nanoparticles in mixed-sample systems. This work offers a better understanding of dynamic interactions of nanoparticles at the electrochemical interface and displays highly valuable applications of single-entity electrochemistry.
随着新仪器和方法的发展，人们对纳米颗粒在液固界面的高度动态行为进行了研究。然而，对于电极界面上单个纳米颗粒电化学行为的动态本质仍知之甚少。在此，我们通过研究纳米颗粒在超微电极界面的吸附能，归纳出标度关系以预测纳米颗粒与电极之间的相互作用。基于理论预测，我们研究了单个银纳米颗粒氧化过程中相互作用调制的动态电化学行为。通常，由于银纳米颗粒的吸附介导运动，会观察到明显不同的电流轨迹。受限制电极界面附近颗粒的随机路径以产生表面受限电流轨迹的启发，我们成功实现了混合样品系统中银纳米颗粒的高分辨率尺寸测量。这项工作有助于更好地理解纳米颗粒在电化学界面的动态相互作用，并展示了单实体电化学的高价值应用。
