4.8 Article

Single-Molecule Tracking of Reagent Diffusion during Chemical Reactions

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 145, 期 19, 页码 10512-10521

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c13172

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Recent experiments show that the diffusion of reagent molecules during a chemical reaction does not match the predictions of the Stokes-Einstein equation. Single-molecule tracking was used to observe the diffusion of reactive reagents, and it was found that the diffusion coefficient remained unchanged in the DA reaction. However, in the click reaction, the diffusion of reagent molecules is faster than predicted when certain concentrations are exceeded. Further analysis suggests that this fast diffusion is due to the reaction itself, rather than the involvement of the tracer.
Recent experiments have shown that the diffusion of reagent molecules is inconsistent with what the Stokes-Einstein equation predicts during a chemical reaction. Here, we used singlemolecule tracking to observe the diffusion of reactive reagent that the diffusion coefficient of the reagents remained unchanged within the experimental uncertainty upon the DA reaction. Yet, diffusion of reagent molecules is faster than predicted during the click reaction when the reagent concentration and catalyst concentration exceed a threshold. A stepwise analysis suggested that the fast diffusion scenario is due to the reaction but not the involvement of the tracer with the reaction itself. The present results provide experimental evidence on the faster-than-expected reagent diffusion during a CuAAC reaction in specific conditions and propose new insights into understanding this unexpected behavior.

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