Issue 31, 2024

Reaction acceleration at the surface of a levitated droplet by vapor dosing from a partner droplet

Abstract

Chemical reactions in micrometer-sized droplets can be accelerated by up to six orders of magnitude. However, this acceleration factor (ratio of rate constants relative to bulk) drops to less than 10 for millimeter-sized droplets due to the reduction in surface/volume ratio. To enhance the acceleration in millimeter-sized droplets, we use a new synthesis platform that directly doses reagent vapor onto the reaction droplet surface from a second levitated droplet. Using Katritzky transamination as a model reaction, we made quantitative measurements on size-controlled vapor-dosed droplets, revealing a 31-fold increase in reaction rate constants when examining the entire droplet contents. This enhancement is attributed to a greater reaction rate constant in the droplet surface region (estimated as 105 times greater than that for the bulk). The capability for substantial reaction acceleration in large droplets highlights the potential for rapid synthesis of important chemicals at useful scales. For example, we successfully prepared 23 pyridinium salts within minutes. This efficiency positions droplets as an exceptional platform for rapid, in situ catalyst synthesis. This is illustrated by the preparation of pyridinium salts as photocatalysts and their subsequent use in mediation of amine oxidation both within the same droplet.

Graphical abstract: Reaction acceleration at the surface of a levitated droplet by vapor dosing from a partner droplet

Supplementary files

Article information

Article type
Edge Article
Submitted
29 may. 2024
Accepted
30 jun. 2024
First published
02 jul. 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 12277-12283

Reaction acceleration at the surface of a levitated droplet by vapor dosing from a partner droplet

L. Qiu, X. Li, D. T. Holden and R. G. Cooks, Chem. Sci., 2024, 15, 12277 DOI: 10.1039/D4SC03528C

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