Search

Taking advantage of the difference between the surface energies of aqueous and organic solvents on a Teflon substrate, a fully automated small-scale strategy is developed on the basis of gas-driven oscillatory motion of a biphasic slug for high-throughput in situ measurement and screening of partition coefficients of organic substances between aqueous and organic phases. The developed oscillatory flow strategy enables single partition coefficient data point measurement within 8 min (including the sample preparation time) which is 360 times faster than the conventional "shake-flask" method, while using less than a 30 μL volume of the two phases and 9 nmol of the target organic substance. The developed multiphase strategy is validated using a conventional shake-flask technique. Finally, the developed strategy is extended to include automated screening of partition coefficients at physiological temperature. [ABSTRACT FROM AUTHOR]

Increase in the ionic strength of water that is mediated by the reaction of carbon dioxide (C 0 2) with nitrogenous bases is a promising approach toward phase separation in mixtures of water with organic solvents and potentially water purification. Conventional macroscale studies of this complicated process are challenging, due to its occurrence via several consecutive and concurrent steps, mass transfer limitation, and lack of control over gas—liquid interfaces. We report a new microfluidic strategy for fundamental studies of liquid—liquid phase separation mediated by CO2 as well as screening of the efficiency of nitrogenous agents. A single set of microfluidic experiments provided qualitative and quantitative information on the provided qualitative and quantitative information on the kinetics and completeness of water—tetrahydrofuran phase separation, the minimum amount of CO2 required to complete phase separation, the total CO2 uptake, and the rate of CO2 consumption by the liquid mixture. The efficiency of tertiary diamines with different lengths of alkyl chain was examined in a time- and labor-efficient manner and characterized with the proposed efficiency parameter. A wealth of information obtained using the MF methodology can facilitate the development of new additives for switchable solvents in green chemistry applications. [ABSTRACT FROM AUTHOR]

To develop an understanding of thenature of complex, spatiotemporalinteractions between cells and the extracellular matrix (ECM), artificialECMs formed from hydrogels with a particular spectrum of propertiesare being developed at a rapid pace. We report the microfluidic generationof small, monodisperse composite agarose–gelatin hydrogel modules(microgel particles) that can be used for cell encapsulation and canserve as instructive cellular microenvironments. The agarose componentof the microgels gelled under reduced temperature, while gelatin modifiedwith phenolic hydroxyl groups underwent peroxidase-catalyzed gelation.Microgel composition, structure, morphology, and rigidity were tunedin a high-throughput manner. The results of this work are importantfor the generation of libraries of cell-laden polymer microgels forsingle-cell analysis, tissue engineering, and fundamental studiesof the role of local microenvironments in cell fate. [ABSTRACT FROM AUTHOR]

Frustrated Lewis pairs (FLPs) comprising sterically hindered Lewis acids and bases offer the capability to reversibly capture CO2 under mild reaction conditions. The determination of equilibrium constants and thermodynamic properties of these reactions should enable assessment of the efficiency of a particular FLP system for CO2sequestration and provide insights for design of new, efficient formulations of FLP catalysts for CO2capture. We have developed a microfluidic approach to studies of FLP–CO2reactions, which provides their thermodynamic characterization that is not accessible otherwise. The approach enables the determination of the equilibrium reaction constants at different temperatures, the enthalpy, the entropy, and the Gibbs energy of these reactions, as well as the enhancement factor. The microfluidic methodology has been validated by applying it to the well-characterized reaction of CO2with a secondary amine. The microfluidic approach can be applied for fundamental thermodynamic studies of other gas–liquid reactions. [ABSTRACT FROM AUTHOR]

In this work, we present a facile and scalable hydrolysis-based route for the synthesis of copper-doped TiO 2 particles for highly effective light-activated antiviral and antibacterial applications. The performance of the synthesized Cu-doped TiO 2 particles is then evaluated using solution-phase antimicrobial photodynamic inactivation assays. We demonstrate that the Cu-doped TiO 2 particles can successfully inactivate a wide range of pathogens with exposure to light for 90 min, including bacteria ranging from methicillin-resistant Staphylococcus aureus (99.9999%, ∼6 log units) to Klebsiella pneumoniae (99.93%, ∼3.3 log units), and viruses including feline calicivirus (99.94%, ∼3.4 log units) and HCoV-229E (99.996%, ∼4.6 log units), with the particles demonstrating excellent robustness toward photobleaching. Furthermore, a spray-coated polymer film, loaded with the synthesized Cu-doped TiO 2 particles achieves inactivation of methicillin-resistant S. aureus up to 99.998% (∼4.8 log units). The presented results provide a clear advance forward in the use of metal-doped TiO 2 for aPDI applications, including the scalable synthesis (kg/day) of well-characterized and robust particles, their facile incorporation into a nontoxic, photostable coating that may be easily and cheaply applied to a multitude of surfaces, and a broad efficacy against drug-resistant Gram-positive and Gram-negative bacteria, as well as against enveloped and nonenveloped viruses., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Although the pharmaceutical and fine chemical industries primarily utilize batch homogeneous reactions to carry out chemical transformations, emerging platforms seek to improve existing shortcomings by designing effective heterogeneous catalysis systems in continuous flow reactors. In this work, we present a versatile network-supported palladium (Pd) catalyst using a hybrid polymer of poly(methylvinylether- alt -maleic anhydride) and branched polyethyleneimine for intensified continuous flow synthesis of complex organic compounds via heterogeneous Suzuki-Miyaura cross-coupling and nitroarene hydrogenation reactions. The hydrophilicity of the hybrid polymer network facilitates the reagent mass transfer throughout the bulk of the catalyst particles. Through rapid automated exploration of the continuous and discrete parameters, as well as substrate scope screening, we identified optimal hybrid network-supported Pd catalyst composition and process parameters for Suzuki-Miyaura cross-coupling reactions of aryl bromides with steady-state yields up to 92% with a nominal residence time of 20 min. The developed heterogeneous catalytic system exhibits high activity and mechanical stability with no detectable Pd leaching at reaction temperatures up to 95 °C. Additionally, the versatility of the hybrid network-supported Pd catalyst is demonstrated by successfully performing continuous nitroarene hydrogenation with short residence times (<5 min) at room temperature. Room temperature hydrogenation yields of >99% were achieved in under 2 min nominal residence times with no leaching and catalyst deactivation for more than 20 h continuous time on stream. This catalytic system shows its industrial utility with significantly improved reaction yields of challenging substrates and its utility of environmentally-friendly solvent mixtures, high reusability, scalable and cost-effective synthesis, and multi-reaction successes., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

Frustrated Lewis pairs (FLPs) comprising sterically hindered Lewis acids and bases offer the capability to reversibly capture CO2 under mild reaction conditions. The determination of equilibrium constants and thermodynamic properties of these reactions should enable assessment of the efficiency of a particular FLP system for CO2 sequestration and provide insights for design of new, efficient formulations of FLP catalysts for CO2 capture. We have developed a microfluidic approach to studies of FLP-CO2 reactions, which provides their thermodynamic characterization that is not accessible otherwise. The approach enables the determination of the equilibrium reaction constants at different temperatures, the enthalpy, the entropy, and the Gibbs energy of these reactions, as well as the enhancement factor. The microfluidic methodology has been validated by applying it to the well-characterized reaction of CO2 with a secondary amine. The microfluidic approach can be applied for fundamental thermodynamic studies of other gas-liquid reactions.