Single-molecule fluorescence imaging of nanocatalytic processes

Abstract

This tutorial review covers recent developments in using single-molecule fluorescence microscopy to study nanoscale catalysis. The single-molecule approach enables following catalytic and electrocatalytic reactions on nanocatalysts, including metal nanoparticles and carbon nanotubes, at single-reaction temporal resolution and nanometer spatial precision. Real-time, in situ, multiplexed measurements are readily achievable under ambient solution conditions. These studies provide unprecedented insights into catalytic mechanism, reactivity, selectivity, and dynamics in spite of the inhomogeneity and temporal variations of catalyst structures. Prospects, generality, and limitations of the single-molecule fluorescence approach for studying nanocatalysis are also discussed.

High‐Resolution Single‐Molecule Fluorescence Imaging of Zeolite Aggregates within Real‐Life Fluid Catalytic Cracking Particles

“…[12–17] The single-molecule sensitivity of fluorescence detection is used to enhance the spatial resolution down to the nanometer scale, making it an ideal candidate for assessing the reactivity of catalytic solids. The technique has been used for studies on well-defined heterogeneous catalysts; for example, single-molecule kinetics of nanoparticle catalysts,[18–20] and high-resolution imaging of catalytic activity in porous heterogeneous catalysts.…”

A new silver nanorod SPR probe for detection of trace benzoyl peroxide

“…Precious metal nanoparticles, especially nanogold and nanosilver have become research focus in many fields such as physics, chemistry, materials and sensing since they have novel physicochemical properties and good stability12. Compared with nanogold, nanosilver (AgNP) has advantages of low-cost, higher molar extinction coefficient3 and more excellent optical properties such as the AgNP aggregates being of low molar extinction coefficient and strong SERS effects, it provide the foundation for their applications45678.…”

Copper nanoparticle heterogeneous catalytic ‘click’ cycloaddition confirmed by single-molecule spectroscopy

“…Hofkens and co-workers 29,30 utilized single-molecule techniques to map the catalytic activity of zeolites and mesoporous materials. Single-molecule techniques have also been used to observe crystal-face-dependent catalysis of layered double hydroxides 31 , and face-dependent catalysis of gold nanoparticles [32][33][34] and has also been the subject of recent reviews [35][36][37][38] . Chen and co-workers 39 have also taken a singlemolecule approach to high-throughput catalyst screening, which uses single-molecule catalysis to identify high activity catalyst particles in mixtures of catalysts and activity correlations to assess reactions that do not involve fluorescence.…”

“…In this study, we combine mole scale reactions with singlemolecule studies utilizing total internal reflection fluorescence microscopy (TIRFM), an effective tool in studying heterogeneous nanoscale catalyst surface dynamics and reactivity 27,[29][30][31][32][33][34][35][36][37][38][39][40][41] . The success of TIRFM as a single-molecule technique hinges on the generation of an evanescent wave at the glass-sample interface that only allows irradiation of the sample within approximately 100 nm from the glass support surface 42 .…”