期刊
ANALYTICAL CHEMISTRY
卷 87, 期 21, 页码 11013-11021出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.5b02968
关键词
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资金
- National Science Foundation [CHE-1111518]
- Welch Foundation [F-0021]
- National Science Foundation of China [21375102, 21005061, 20975079]
- Natural Science Basic Research Plan in Shaanxi Province of China [2012KJXX-25]
- National Scholarship Fund of China Scholarship Council [201208615034]
- National Science Foundation Graduate Research Fellowship [DGE-1110007]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1405248] Funding Source: National Science Foundation
We report the collisions of single emulsion oil droplets with extremely low dielectric constants (e.g., benzene, epsilon of 2.27, or cyclohexane, epsilon of 2.02) as studied via emulsion droplet reactor (EDR) on an ultramicroelectrode (UME). By applying appropriate potentials to the UME, we observed the electrochemical effects of single-collision signals from the bulk electrolysis of single emulsion droplets. Different hydrophobic redox species (ferrocene, decamethyl-ferrocene, or metalloporphyrin) were trapped in a mixed benzene (or cyclohexane) oil-in-water emulsion using an ionic liquid as the supporting electrolyte and emulsifier. The emulsions were prepared using ultrasonic processing. Spike-like responses were observed in each i-t response due to the complete electrolysis of all of the above-mentioned redox species within the droplet. On the basis of these single-particle collision results, the collision frequency, size distribution, i-t decay behavior of the emulsion droplets, and possible mechanisms are analyzed and discussed. This work demonstrated that bulk electrolysis can be achieved in a few seconds in these attoliter reactors, suggesting many applications, such as analysis and electrosynthesis in low dielectric constant solvents, which have a much broader potential window.
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