Studying single catalyst nanoparticles, during reaction, eliminates averaging effects that are an inherent limitation of ensemble experiments. It enables establishing structure–function correlations beyond averaged properties by including particle-specific descriptors such as defects, chemical heterogeneity and microstructure. Driven by these prospects, several single particle catalysis concepts have been implemented. However, they all have limitations such as low throughput, or that they require very low reactant concentrations and/or reaction rates. In response, we present a nanofluidic device for highly parallelized single nanoparticle catalysis in solution, based on fluorescence microscopy. Our device enables parallel scrutiny of tens of single nanoparticles, each isolated inside its own nanofluidic channel, and at tunable reaction conditions, ranging from the fully mass transport limited regime to the surface reaction limited regime. In a wider perspective, our concept provides a versatile platform for highly parallelized single particle catalysis in solution and constitutes a promising application area for nanofluidics.
Catalyst activity can depend distinctly on nanoparticle
size and
shape. Therefore, understanding the structure sensitivity of catalytic
reactions is of fundamental and technical importance. Experiments
with single-particle resolution, where ensemble-averaging is eliminated,
are required to study it. Here, we implement the selective trapping
of individual spherical, cubic, and octahedral colloidal Au nanocrystals
in 100 parallel nanofluidic channels to determine their activity for
fluorescein reduction by sodium borohydride using fluorescence microscopy.
As the main result, we identify distinct structure sensitivity of
the rate-limiting borohydride oxidation step originating from different
edge site abundance on the three particle types, as confirmed by first-principles
calculations. This advertises nanofluidic reactors for the study of
structure–function correlations in catalysis and identifies
nanoparticle shape as a key factor in borohydride-mediated catalytic
reactions.
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