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  1. Free, publicly-accessible full text available December 3, 2023
  2. Free, publicly-accessible full text available November 10, 2023
  3. Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active metal center can greatly improve the stability without compromising the activity. Using an Ir dinuclear heterogeneous catalyst (DHC) as a study platform, we identify two types of oxygen species, interfacial and bridge, that work in concert to enable both activity and stability. The work sheds important light on the synergistic effect between the active metal center and the supporting substrate and may find broad applications for the use of atomically dispersed catalysts.
    Free, publicly-accessible full text available January 3, 2024
  4. McCartney, J.S. ; Tomac, I. (Ed.)
    Immiscible multiphase flow in porous media is largely affected by interfacial properties, manifested in contact angle and surface tension. The gas-liquid surface tension can be significantly altered by suspended particles at the interface. Particle-laden interfaces have unique properties, for example, a lower surface tension of interfaces laden with surfactants or nanoparticles. This study investigates the impacts of a motile bacterium Escherichia coli ( E. coli , strain ATCC 9637) on the air-water surface tension. Methods of the maximum bubble pressure, the du Noüy ring, and the pendant droplet are used to measure the surface tension of the motile-bacteria-laden interfaces. Measured surface tension remains independent to the E. coli concentration when using the maximum bubble pressure method, decreases with increased E. coli concentration in the du Noüy ring method, and presents time-dependent changes by the pendant drop method. The analyses show that the discrepancies may come from the different convection-diffusion processes of E. coli in the flow among various testing methods.
  5. McCartney, J.S. ; Tomac, I. (Ed.)
    Multiphase flow patterns in porous media largely depend on the properties of the fluids and interfaces such as viscosity, surface tension, and contact angle. Microorganisms in soils change the fluid and interfacial properties, and thus can alter multiphase fluid flow in porous media. This study investigates the impact of motile bacterium Escherichia coli ( E. coli ) on fluid displacement patterns in a microfluidic chip. The fluid displacement is observed during the saturation and the desaturation processes of the microfluidic chip with and without E.coli suspension. Time-lapse photography results show that the presence of E.coli alters the displacement patterns during the wetting and drying process and changes the residual saturation of the chip. Although studies of the impacts of motility on interfacial properties remain elusive, these results bring the expectation to the manipulation of multiphase transport in porous media and the adaptive control of industrial and environmental flow processes using active particles.
  6. Abstract

    Three-dimensional bicontinuous porous materials formed by dealloying contribute significantly to various applications including catalysis, sensor development and energy storage. This work studies a method of molten salt dealloying via real-time in situ synchrotron three-dimensional X-ray nano-tomography. Quantification of morphological parameters determined that long-range diffusion is the rate-determining step for the dealloying process. The subsequent coarsening rate was primarily surface diffusion controlled, with Rayleigh instability leading to ligament pinch-off and creating isolated bubbles in ligaments, while bulk diffusion leads to a slight densification. Chemical environments characterized by X-ray absorption near edge structure spectroscopic imaging show that molten salt dealloying prevents surface oxidation of the metal. In this work, gaining a fundamental mechanistic understanding of the molten salt dealloying process in forming porous structures provides a nontoxic, tunable dealloying technique and has important implications for molten salt corrosion processes, which is one of the major challenges in molten salt reactors and concentrated solar power plants.