Buildup and Consumption of Species in Emulsion Droplets during Aqueous Suzuki Coupling Correlate with Yield.

J Org Chem

Department of Chemistry, University of California, Irvine, Irvine, California 92697-2025, United States.

Published: August 2024

Fluorescence lifetime imaging microscopy (FLIM) provides spatiotemporal resolution of the changing composition of emulsion droplets during aqueous-surfactant Suzuki coupling. In contrast to previous investigations, the present experiments characterize the full course of a catalytic chemical reaction, addressing key questions about reaction species buildup and correlating these microscale behaviors with bench-scale product yields. At low concentrations of (active) catalyst, droplet environments are stable; however, at higher concentrations, emulsion droplet environments change markedly. These changes are consistent with the buildup and consumption of reaction species inside the droplets. A combination of FLIM and bright-field imaging pinpoints limitations in catalyst solubility as controlling rate and degree of buildup of species in droplets. These solubility limitations are also identified as the cause of a reaction induction period and an origin of the rate-and-reproducibility advantage obtained by adding THF cosolvent. The subsequent mechanistic model from these data led to a bench-scale reaction optimization, wherein premixing the catalyst components bypasses the catalyst induction period, resulting in a faster reaction. The understanding generated by FLIM thus provides an early example of how visualizing changes in droplet compositions on the microscale during ongoing aqueous-organic reactions can be leveraged for enhancing efficiencies in bench-scale reactions.

Download full-text PDF

Source
http://dx.doi.org/10.1021/acs.joc.4c00918DOI Listing

Publication Analysis

Top Keywords

buildup consumption
8
emulsion droplets
8
suzuki coupling
8
reaction species
8
droplet environments
8
induction period
8
reaction
6
buildup
4
species
4
consumption species
4

Similar Publications

The Synthesis, Crystal Structure, Modification, and Cytotoxic Activity of α-Hydroxy-Alkylphosphonates.

Molecules

January 2025

Department of Organic Chemistry and Technology, Faculty of Chemical Technology and Biotechnology, Budapest University of Technology and Economics, Műegyetem rkp. 3., 1111 Budapest, Hungary.

A series of α-hydroxy-alkylphosphonates and α-hydroxy-alkylphosphine oxides were synthesized by the Pudovik reaction of acetaldehyde and acetone with dialkyl phosphites or diarylphosphine oxides. The additions were performed in three different ways: in liquid phase using triethylamine as the catalyst (1), on the surface of AlO/KF solid catalyst (2), or by a MW-assisted NaCO-catalyzed procedure (3). In most of the cases, our methods were more efficient and more robust than those applied in the literature.

View Article and Find Full Text PDF

and mosquitoes, known for spreading arboviruses like dengue and West Nile, thrive in cities, posing health risks to urban populations. Climate change can create suitable climatic conditions for these vectors to spread further in Europe. Cities contain numerous landscape and infrastructure elements, such as storm drains, that allow stagnant water build-up facilitating mosquito breeding.

View Article and Find Full Text PDF

Patient: A 26-year-old man with localized tooth wear and demand for aesthetic rehabilitation of the anterior teeth presented to our department. The patient reported excessive consumption of energy drinks. Furthermore, multiple trauma and tooth fractures have occurred in the past.

View Article and Find Full Text PDF

Common salt (NaCl) causes developmental, behavioral, and physiological defects in .

Nutr Neurosci

January 2025

Neural Developmental Biology Lab, Department of Life Science, NIT Rourkela, Rourkela, Odisha, India.

Article Synopsis
  • The study investigates the toxicity of salt on obesity using Drosophila larvae and adult flies, testing varying salt concentrations (50-800 µM).
  • At lower concentrations (50 and 200 µM), significant weight gain and increased feeding behavior were observed, with larvae and adult flies displaying abnormal responses to temperature and light stimuli.
  • The findings reveal that while lower salt concentrations induce stronger adverse effects, higher concentrations deter feeding, suggesting a complex relationship between salt intake and obesity-related behaviors.
View Article and Find Full Text PDF

Hydroxylamine, nitrous acid, and nitric oxide are obligate intermediates or side metabolites in different nitrogen-converting microorganisms. These compounds are unstable and susceptible to the formation of highly reactive nitrogen species, including nitrogen dioxide, dinitrogen trioxide, nitroxyl, and peroxynitrite. Due to the high reactivity and cytotoxicity, the buildup of reactive nitrogen can affect the interplay of microorganisms/microbial processes, stimulate the reactions with organic compounds like organic micropollutants (OMP) and act as the precursors of nitrous oxide (NO).

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!