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Abstract Chemical imaging, especially mid-infrared spectroscopic microscopy, enables label-free biomedical analyses while achieving expansive molecular sensitivity. However, its slow speed and poor image quality impede widespread adoption. We present a microscope that provides high-throughput recording, low noise, and high spatial resolution where the bottom-up design of its optical train facilitates dual-axis galvo laser scanning of a diffraction-limited focal point over large areas using custom, compound, infinity-corrected refractive objectives. We demonstrate whole-slide, speckle-free imaging in ~3 min per discrete wavelength at 10× magnification (2 μm/pixel) and high-resolution capability with its 20× counterpart (1 μm/pixel), both offering spatial quality at theoretical limits while maintaining high signal-to-noise ratios (>100:1). The data quality enables applications of modern machine learning and capabilities not previously feasible – 3D reconstructions using serial sections, comprehensive assessments of whole model organisms, and histological assessments of disease in time comparable to clinical workflows. Distinct from conventional approaches that focus on morphological investigations or immunostaining techniques, this development makes label-free imaging of minimally processed tissue practical. 

The effect of input doses of 60Co γ-radiation from 80 to 12,000 kGy on the thermophysical properties and thermal stability of samples of polypropylene granules and powder obtained by high temperature shear grinding of irradiated granules, as well as on the tensile strength properties of a plate made from irradiated granules and their corresponding powders, was studied. The thermophysical properties of the powder are determined by the changes introduced by radiation into the initial polymer granules. The effects of radiation in air (environments with oxygen) were studied. Grinding redistributes oxygen-containing functional groups from the surface layer of irradiated granules throughout the entire volume of the obtained powder leading to the destruction of polymer chains as there is a component due to thermal destruction of radiolyzed polymer chains. High-temperature shear grinding of irradiated granules has a significant effect on the product powder, reducing its thermal stability but increasing the tensile strength of plates pressed from it at low absorbed doses. The current work shows that radiation treatment coupled with high temperature shear grinding could be a method for modifying the properties of polymers so that polypropylene waste can be processed for other applications. 

The effect of γ-irradiation in vacuum and air followed by HTSG of polypropylene (PP) is studied using both infrared (IR) spectroscopy and computational chemistry at the correlated G3(MP2)B3 molecular orbital theory level. γ-irradiation of PP in vacuum was found to primarily induce unsaturation and hydroxyl formation from residual system water whereas γ-irradiation of PP in air oxidizes the polymer and degrades the backbone in a thin layer due to oxygen permeability limitations as supported by the computational thermodynamics results. HTSG of the irradiated PP produced smaller particles than un-irradiated PP. HTSG of the irradiated PP led to a decrease in the IR band intensity from degradation due to a nominal homogenization of the pellet. HTSG of air irradiated PP led to a reduction in IR vibrational band intensity from oxidation due to thermal degradation. High-temperature shear grinding of γ-irradiated PP produces variable chemical and physical composition depending on irradiation input dose and environmental conditions. The combination of γ-irradiation and HTSG may be of benefit in recycling polypropylene. 

Acid gases including CO2, OCS, CS2, and SO2 are emitted by industrial processes such as natural gas production or power plants, leading to the formation of acid rain and contributing to global warming as greenhouse gases. An important technological challenge is to capture acid gases and transform them into useful products. The capture of CO2, CS2, SO2, and OCS by ring expansion of saturated and unsaturated substituted nitrogen-strained ring heterocycles was computationally investigated at the G3(MP2) level. The effects of fluorine, methyl, and phenyl substituents on N and/or C were explored. The reactions for the capture CO2, CS2, SO2, and OCS by 3- and 4-membered N-heterocycles are exothermic, whereas ring expansion reactions with 5-membered rings are thermodynamically unfavorable. Incorporation of an OCS into the ring leads to the amide product being thermodynamically favored over the thioamide. CS2 and OCS capture reactions are more exothermic and exergonic than the corresponding CO2 and SO2 capture reactions due to bond dissociation enthalpy differences. Selected reaction energy barriers were calculated and correlated with the reaction thermodynamics for a given acid gas. The barriers are highest for CO2 and OCS and lowest for CS2 and SO2. The ability of a ring to participate in acid gas capture via ring expansion is correlated to ring strain energy but is not wholly dependent upon it. The expanded N-heterocycles produced by acid gas capture should be polymerizable, allowing for upcycling of these materials. 

The formation of carbon-carbon bonds by pinacol coupling of aldehydes and ketones requires a large negative reduction potential, often realized with a stoichiometric reducing reagent. Here, we use solvated electrons generated via a plasma-liquid process. Parametric studies with methyl-4-formylbenzoate reveal that selectivity over the competing reduction to the alcohol requires careful control over mass transport. The generality is demonstrated with benzaldehydes, benzyl ketones, and furfural. A reaction-diffusion model explains the observed kinetics, and ab initio calculations provide insight into the mechanism. This study opens the possibility of a metal-free, electrically-powered, sustainable method for reductive organic reactions.