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Abstract
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.
Single-entity electrochemistry has been proposed for studying properties of single nanoparticles (NPs). Here, the authors make use of adsorption-mediated motion of Ag NPs to take individual NP size measurements using electrochemical impacts with excellent agreement to standard imaging techniques.
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1 East China University of Science and Technology, School of Chemistry and Molecular Engineering, Shanghai, P. R. China (GRID:grid.28056.39) (ISNI:0000 0001 2163 4895); Nanjing University, State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing, P.R. China (GRID:grid.41156.37) (ISNI:0000 0001 2314 964X)
2 East China University of Science and Technology, State Key Laboratory of Chemical Engineering, Centre for Computational Chemistry & Research Institute of Industrial Catalysis, Shanghai, P. R. China (GRID:grid.28056.39) (ISNI:0000 0001 2163 4895)
3 East China University of Science and Technology, State Key Laboratory of Chemical Engineering, Centre for Computational Chemistry & Research Institute of Industrial Catalysis, Shanghai, P. R. China (GRID:grid.28056.39) (ISNI:0000 0001 2163 4895); The Queen’s University of Belfast, School of Chemistry and Chemical Engineering, Belfast, UK (GRID:grid.4777.3) (ISNI:0000 0004 0374 7521)
4 East China University of Science and Technology, School of Chemistry and Molecular Engineering, Shanghai, P. R. China (GRID:grid.28056.39) (ISNI:0000 0001 2163 4895)