Optical Fingerprinting of Dynamic Interfacial Reaction Pathways Using Liquid Crystals

Reactions at interfaces between fluid phases are widely used to synthesize small molecules, polymers, and nanoparticles. In situ monitoring of the underlying dynamic reaction pathways remains challenging. Liquid crystals (LCs) have been used to detect simple chemical transformations at interfaces in...

Ausführliche Beschreibung

Bibliographische Detailangaben
Veröffentlicht in:Langmuir : the ACS journal of surfaces and colloids. - 1992. - 39(2023), 5 vom: 07. Feb., Seite 1793-1803
1. Verfasser: Wang, Xin (VerfasserIn)
Weitere Verfasser: Krishna, Jithu, Fernandez, Ann, Thayumanavan, S, Abbott, Nicholas L
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2023
Zugriff auf das übergeordnete Werk:Langmuir : the ACS journal of surfaces and colloids
Schlagworte:Journal Article
Beschreibung
Zusammenfassung:Reactions at interfaces between fluid phases are widely used to synthesize small molecules, polymers, and nanoparticles. In situ monitoring of the underlying dynamic reaction pathways remains challenging. Liquid crystals (LCs) have been used to detect simple chemical transformations at interfaces in situations where interface-bound reactants and products trigger distinct equilibrium orientations of LCs. However, whether or not LCs can be used to report complex reaction pathways via nonequilibrium states generated by reactions has not been explored. Here we explore this question using SN2' nucleophilic substitution reactions that involve a synthetic amphiphile and a series of amine-based nucleophiles with one to four reaction sites. Although all reactants and products generate the same equilibrium LC orientation, we find that each nucleophile defines a distinct set of possible reaction pathways with a characteristic spatial and temporal LC optical response unique to the nucleophile. Additional experiments reveal that the nonequilibrium orientational states of the LCs arise from a combination of dynamic interfacial processes that include adsorption/desorption of reactants, the presence of reaction intermediates on the LC interface, and the generation of interfacial tension gradients (Marangoni stresses). Overall, our results reveal that the spatiotemporal optical outputs of LCs ("optical fingerprints") can be a rich source of information regarding interfacial reactions
Beschreibung:Date Completed 07.02.2023
Date Revised 07.02.2023
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1520-5827
DOI:10.1021/acs.langmuir.2c02622