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MacGregor Milne posted an update 6 months, 3 weeks ago
An-O → An-N substitutions marginally improve the barriers by 1-4 kcal/mol and more substantially improve the reaction energies by 9-15 kcal/mol. For H2 capture and hydride transfer, the reaction energies for the U and Np species are similar. For both actinides, like-for-like An-O → An-N substitutions lead to improved reaction energies. Interestingly, in a recent report, it seemingly appears that U-O (siloxide) → U-N (silylamide) leads to complete shutdown of reactivity for H2 capture and hydride transfer. This observation is reproduced and explained with calculations. The ligand environments of the siloxide and silylamide that were compared are vastly different. The steric environment of the siloxide is conducive for reactivity while the particular silylamide is not. We conclude that small-molecule activation with organometallic neptunium species is achievable with a guided choice of ligands. Additional emphasis should be placed on ligands that can allow for improved transition state barriers.Additive manufacturing (also known as three-dimensional (3D) printing) is being extensively utilized in many areas of electrochemistry to produce electrodes and devices, as this technique allows for fast prototyping and is relatively low cost. Furthermore, there is a variety of 3D-printing technologies available, which include fused deposition modeling (FDM), inkjet printing, select laser melting (SLM), and stereolithography (SLA), making additive manufacturing a highly desirable technique for electrochemical purposes. In particular, over the last number of years, a significant amount of research into using 3D printing to create electrodes/devices for electrochemical energy conversion and storage has emerged. Strides have been made in this area; however, there are still a number of challenges and drawbacks that need to be overcome in order to 3D print active and stable electrodes/devices for electrochemical energy conversion and storage to rival that of the state-of-the-art. In this Review, we will give an overview of the reasoning behind using 3D printing for these electrochemical applications. We will then discuss how the electrochemical performance of the electrodes/devices are affected by the various 3D-printing technologies and by manipulating the 3D-printed electrodes by post modification techniques. N-acetylcysteine in vitro Finally, we will give our insights into the future perspectives of this exciting field based on our discussion through this Review.Structural, electrical, and thermal properties of CdSnAs2, with analyses from temperature-dependent transport properties over a large temperature range, are reported. Phase-pure microcrystalline powders were synthesized that were subsequently densified to a high-density homogeneous polycrystalline specimen for this study. Temperature-dependent transport indicates n-type semiconducting behavior with a very high and nearly temperature independent mobility over the entire measured temperature range, attributed to the very small electron effective mass of this material. The Debye model was successfully applied to model the thermal conductivity and specific heat. This work contributes to the fundamental understanding of this material, providing further insight and allowing for investigations into altering this and related physical properties of these materials for technological applications.X-ray radio-luminescence materials have potential application in radiotherapy (RT) and biomedical imaging. Considering that lutecium ions (Lu3+) with high atomic number (Z) have high X-ray attenuation coefficients, Ce3+-doped A-type Lu2SiO5@SiO2 (A-LSOCe3+@SiO2) core-shell nanospheres with size in the range of 200-250 nm were prepared through coprecipitation method. The growth mechanism of A-LSOCe3+@SiO2 core-shell nanospheres was investigated through determining the phase transition and morphology evolution by XRD, FT-IR, and TEM. The emission spectra, decay profile, and X-ray excited luminescence spectra (XEL) of the obtained samples were collected. The results show that a new type of lutecium silicate core-shell nanospheres A-LSOCe3+@SiO2 can be fabricated and exhibit efficient radio-luminescence under X-ray radiation, which has potential application in the diagnosis and therapy of cancer.B-F σ-bond activation of a fluoroborate has been experimentally achieved through reactions with electron-rich iridium(I) and palladium(0) complexes. The selectivity of B-F σ-bond cleavage by iridium complexes was improved through the high nucleophilicity of the iridium center, implying that a different pathway from that of well-accepted F- abstraction was in effect. The palladium(0) complex was found to promote exclusive B-F σ-bond cleavage even at ambient temperature. Density functional theory (DFT) calculations suggested that B-F σ-bond activation occurred through an SN2-type pathway, which is, to our knowledge, the first proposal of SN2-type borate-fluorine σ-bond cleavage mediated by a transition metal complex. The high feasibility of the SN2-type pathway appears to be attributed to the relatively low deformation energy of the transition state. It was also found that countercation Cs+ effectively stabilized the transition state and product by serving as a F- acceptor.Therapy for intracerebral hemorrhage (ICH) remains elusive, in part dependent on the severity of the hemorrhage itself as well as multiple deleterious effects of blood and its breakdown products such as hemin and free iron. While oxidative injury and genomic damage have been seen following ICH, the details of this injury and implications remain unclear. Here, we discovered that, while free iron produced mostly reactive oxygen species (ROS)-related single-strand DNA breaks, hemin unexpectedly induced rapid and persistent nuclear and mitochondrial double-strand breaks (DSBs) in neuronal and endothelial cell genomes and in mouse brains following experimental ICH comparable to that seen with γ radiation and DNA-complexing chemotherapies. Potentially as a result of persistent DSBs and the DNA damage response, hemin also resulted in senescence phenotype in cultured neurons and endothelial cells. Subsequent resistance to ferroptosis reported in other senescent cell types was also observed here in neurons. While antioxidant therapy prevented senescence, cells became sensitized to ferroptosis.
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