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Spatial reorganization of analytes in charged aqueous microdroplets.

ABSTRACT: Imprinted charged aqueous droplets of micrometer dimensions containing spherical gold and silver nanoparticles, gold nanorods, proteins and simple molecules were visualized using dark-field and transmission electron microscopies. With such studies, we hoped to understand the unusual chemistry exhibited by microdroplets. These droplets with sizes in the range of 1-100 μm were formed using a home-built electrospray source with nitrogen as the nebulization gas. Several remarkable features such as mass/size-selective segregation and spatial localization of solutes in nanometer-thin regions of microdroplets were visualized, along with the formation of micro-nano vacuoles. Electrospray parameters such as distance between the spray tip and surface, voltage and nebulization gas pressure influenced particle distribution within the droplets. We relate these features to unusual phenomena such as the enhancement of rates of chemical reactions in microdroplets.

SUBMITTER: Basuri P

PROVIDER: S-EPMC9682915 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature

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Spatial reorganization of analytes in charged aqueous microdroplets.

Basuri Pallab P Chakraborty Amrita A Ahuja Tripti T Mondal Biswajit B Kumar Jenifer Shantha JS Pradeep Thalappil T

Chemical science 20221011 45

Imprinted charged aqueous droplets of micrometer dimensions containing spherical gold and silver nanoparticles, gold nanorods, proteins and simple molecules were visualized using dark-field and transmission electron microscopies. With such studies, we hoped to understand the unusual chemistry exhibited by microdroplets. These droplets with sizes in the range of 1-100 μm were formed using a home-built electrospray source with nitrogen as the nebulization gas. Several remarkable features such as m ...[more]

PMID: 36507174

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Project description:Multiphasic buffer systems have been of greatest interest in electrophoresis and liquid-liquid electrotransfer; this study extends that foundation by exploring the interplay of the geometric and viscous properties of an interleaving oil layer on the electrotransfer of a charged analyte from an aqueous solution into a hydrogel. We utilized finite element analysis to examine two complementary configurations: one being electrotransfer of a charged analyte (protein) in an aqueous phase into a surrounding hydrogel layer and another being electrotransfer of the protein from that originating aqueous phase-through an interleaving oil layer of predetermined viscosity and thickness-and into a surrounding hydrogel layer. Results indicate that the presence of an oil layer leads to increased skew of the injected peak. To explain this difference in injection dispersion, we utilize Probstein's framework and compare the Péclet (Pe) number with the ratio between length scales characteristic to the axial and radial dispersion, respectively. The formulation assigns electrotransfer conditions into six different dispersion regimes. We show that the presence or absence of an interleaving oil layer moves the observed peak dispersion into distinct electrotransfer regimes; the presence of an oil layer augments the electrophoretic mobility mismatch among the different phases, resulting in a five-fold increase in Pe and a six-fold increase in the ratio between the axial to radial dispersion characteristic lengths. We further show that oil viscosity significantly influences resultant injection dispersion. A decrease in oil-layer viscosity from 0.08 to 0.02 Pa s results in a >100% decrease in injection dispersion. Our theoretical predictions were experimentally validated by comparing the electrotransfer regimes of three different mineral oil samples. We show that lowering the oil viscosity to 0.0039 Pa s results in an injection regime similar to that of the absence of an oil layer. Understanding of the impact of electrotransfer of charged species across multiple immiscible fluid layers on peak dispersion informs the design of multiphasic electrophoresis systems.

Dataset Information

Spatial reorganization of analytes in charged aqueous microdroplets.

Publications

Spatial reorganization of analytes in charged aqueous microdroplets.

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