Probing Nanoparticle Reactivity at the Single-Molecule Level

摘要

This final report summarizes our achievements in developing and using single-molecule fluorescence microscopy techniques to interrogate and understand the surface reactivity of individual metal nanoparticles at an unprecedented level. The report covers: (1) Study of size-dependent catalytic activity and dynamics of Au nanoparticles at the single-molecule level (JACS 2010). (2) Quantitative superresolution imaging of catalytic reactivity of single Au nanorods (Nat. Nanotechnol. 2012). (3) Site-specific activity mapping and discovery of radial activity gradients on single 2D nanocrystal catalysts (JACS 2013). (4) Development of a massively scalable, parallel method for screening catalyst activity at the single-particle level and sub-diffraction spatial resolution (i.e., super-optical resolution) (ACS Catal. 2013). (5) Quantification of the catalytic activity and dynamics of single Pt nanoparticles in two different reactions (Nano Lett. 2012). (6) Discovery of long-range catalytic communication within single 1-D and 2-D nanocrystal catalysts. (7) Review of the theory and experiments as well as of the scientific insights from single-molecule nanoparticle catalysis studies (Nano Res. 2009, Phys. Chem. Chem. Phys. 2010, Chemical Society Reviews, 2010 & 2014). The report also describes our progress in the new direction of imaging catalytic reactivity at nanoscale metal-metal junctions.