Issue 4, 2014

Spatiotemporal catalytic dynamics within single nanocatalysts revealed by single-molecule microscopy

Abstract

This review discusses the latest advances in using single-molecule microscopy of fluorogenic reactions to examine and understand the spatiotemporal catalytic behaviors of single metal nanoparticles of various shapes including pseudospheres, nanorods, and nanoplates. Real-time single-turnover kinetics reveal size-, catalysis-, and metal-dependent temporal activity fluctuations of single pseudospherical nanoparticles (<20 nm in diameter). These temporal catalytic dynamics can be related to nanoparticles' dynamic surface restructuring whose timescales and energetics can be quantified. Single-molecule super-resolution catalysis imaging further enables the direct quantification of catalytic activities at different surface sites (i.e., ends vs. sides, or corner, edge vs. facet regions) on single pseudo 1-D and 2-D nanocrystals, and uncovers linear and radial activity gradients within the same surface facets. These spatial activity patterns within single nanocrystals can be attributed to the inhomogeneous distributions of low-coordination surface sites, including corner, edge, and defect sites, among which the distribution of defect sites is correlated with the nanocrystals' morphology and growth mechanisms. A brief discussion is given on the extension of the single-molecule imaging approach to catalysis that does not involve fluorescent molecules.

Graphical abstract: Spatiotemporal catalytic dynamics within single nanocatalysts revealed by single-molecule microscopy

Article information

Article type
Review Article
Submitted
26 Jun 2013
First published
18 Sep 2013

Chem. Soc. Rev., 2014,43, 1107-1117

Spatiotemporal catalytic dynamics within single nanocatalysts revealed by single-molecule microscopy

P. Chen, X. Zhou, N. M. Andoy, K. Han, E. Choudhary, N. Zou, G. Chen and H. Shen, Chem. Soc. Rev., 2014, 43, 1107 DOI: 10.1039/C3CS60215J

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