High Throughput Synthesis and Screening of Oxygen Reduction Catalysts in the MTiO₃ (M = Ca, Sr, Ba) Perovskite Phase Diagram

A library of 66 perovskite BaxSryCazTiO3 (x + y + z = 1) samples (ca. three grams per sample) was made in ca. 14 h using a high-throughput continuous hydrothermal flow synthesis system. The as-synthesized samples were collected from the outlet of the process and then cleaned and freeze-dried before being evaluated individually as oxygen reduction catalysts using a rotating disk electrode testing technique. To establish any correlations between physical and electrochemical characterization data, the as-synthesized samples were investigated using analytical methods including BET surface area, powder X-ray diffraction (PXRD) and in selected cases, transmission electron microscopy (TEM). The aforementioned approach was validated as being able to quickly identify oxygen reduction catalysts from new libraries of electrocatalysts

Continuous Hydrothermal Synthesis of Metal Germanates (M₂GeO₄; M=Co, Mn, Zn) for High-Capacity Negative Electrodes in Li-Ion Batteries

Nanosized metal germanates (M2GeO4; M = Co, Mn, Zn) are synthesized using a continuous hydrothermal flow synthesis process for the first time. The electrochemical properties of all samples as active materials for negative electrodes in Li‐ion half cells are explored. The galvanostatic and potentiodynamic testing is conducted in the potential range of 3.00–0.05 V versus Li/Li+. The results suggest that both alloying and conversion reactions associated with Ge contribute to the stored charge capacity; Zn2GeO4 shows a high specific capacity of 600 mAh g−1 (ten cycles at 0.1 A g−1) due to alloying and conversion reactions for both Ge and Zn. Mn2GeO4 is studied for the first time as a potential negative electrode material in a Li‐ion half cell; an excellent specific charge capacity of 510 mAh g−1 (10 cycles per 0.1 A g−1) is obtained with a significant contribution to charge arising from the conversion reaction of Mn to MnO upon delithiation. In contrast, Co2GeO4 only shows a specific capacity of 240 mAh g−1, after ten cycles at the same current rate, which suggests that cobalt has little or no benefit for enhancing stored charge in germanate

Enhanced IL-2 in early life limits the development of TFH and protective antiviral immunity

T follicular helper cell (TFH)-dependent antibody responses are critical for long-term immunity. Antibody responses are diminished in early life, limiting long-term protective immunity and allowing prolonged or recurrent infection, which may be important for viral lung infections that are highly prevalent in infancy. In a murine model using respiratory syncytial virus (RSV), we show that TFH and the high-affinity antibody production they promote are vital for preventing disease on RSV reinfection. Following a secondary RSV infection, TFH-deficient mice had significantly exacerbated disease characterized by delayed viral clearance, increased weight loss, and immunopathology. TFH generation in early life was compromised by heightened IL-2 and STAT5 signaling in differentiating naive T cells. Neutralization of IL-2 during early-life RSV infection resulted in a TFH-dependent increase in antibody-mediated immunity and was sufficient to limit disease severity upon reinfection. These data demonstrate the importance of TFH in protection against recurrent RSV infection and highlight a mechanism by which this is suppressed in early life

From Ligand to Phosphor: Rapid, Machine-Assisted Synthesis of Substituted Iridium(III) Pyrazolate Complexes with Tuneable Luminescence

A first generation machine-assisted approach towards the preparation of hybrid ligand/metal materials has been explored. A comparison of synthetic approaches demonstrates that incorporation of both flow chemistry and microwave heating, can be successfully applied to the rapid synthesis of a range of new phenyl-1H-pyrazoles (ppz) substituted with electron withdrawing groups (-F, -CF3, -OCF3, -SF5), and these, in turn, can be translated in to heteroleptic complexes, [Ir(ppz)2(bipy)]BF4 (bipy = 2,2’-bipyridine). Microwave-assisted syntheses for the IrIII complexes allows isolation of spectroscopically pure species in less than 1 hour of reaction time from IrCl3. All new complexes have been explored photophysically (including nanosecond time-resolved transient absorption spectroscopy), electrochemically and by TD-DFT studies which show that the complexes possess ligand-dependent, and thus, tuneable green-yellow luminescence (500-560 nm), with quantum yields in the range 5-15 %

Functional cardiac MRI in preterm and term newborns.

Published versio

Multiple diffusion pathways in LixNi0.77Co0.14Al0.09O2 (NCA) Li-ion battery cathodes

Experimental evidence for the presence of two computationally theorised diffusion pathways, namely the oxygen dumbbell hop (ODH) and tetrahedral site hop (TSH), has been given for the first time by muon spin relaxation (µSR) on sub-stoichiometric LixNi0.77Co0.14Al0.09O2. µSR has proven to be a powerful tool that is able to discriminate between diffusion pathways that occur on different timescales on a local level, where bulk electrochemical techniques cannot. Whereas the estimated values of DLi at lithium concentrations of 0.87 and 0.71 were found to be on the order of 10-11 by electrochemical impedance spectroscopy, contributions to diffusion from ODH and TSH were determined to be on the order of 10-11 and 10-10 cm2 s-1, and a factor of four decrease in Ea for both samples, in excellent agreement with theoretical calculations on related compounds. Rietveld refinement of both X-ray and neutron diffraction data was also used to interrogate the local structure of the materials where no contribution from Li+/Ni2+ cation mixing was observed

Design of secure coding challenges for cybersecurity education in the industry

To minimize the possibility of introducing vulnerabilities in source code, software developers in the industry may attend security awareness and secure coding training. One promising novel approach to raise awareness is to use cybersecurity challenges in a capture-the-flag event. In order for this to be effective, the types of challenges must be adequately designed to address the target group. In this work we look at how to design challenges for software developers in an industrial context, based on survey given to security experts by gathering their experience on the field. While our results show that traditional methods seem to be adequate, they also reveal a new class of challenges based on code entry and interaction with an automated coach.info:eu-repo/semantics/acceptedVersio

Luminescent properties and reduced dimensional behavior of hydrothermally prepared Y <inf>2</inf>SiO <inf>5</inf>: Ce nanophosphors

Hydrothermally prepared nanophosphor Y2 Si O5: Ce crystallizes in the P 21 c structure, rather than the B2b structure observed in bulk material. Relative to bulk powder, nanophosphors of particle size ∼25-100 nm diameter exhibit redshifts of the photoluminescence excitation and emission spectra, reduced self absorption, enhanced light output, and medium-dependent radiative lifetime. Photoluminescence data are consistent with reduced symmetry of the P 21 c structure and are not necessarily related to reduced dimensionality of the nanophosphor. In contrast, medium-dependent lifetime and enhanced light output are attributed to nanoscale behavior. Perturbation of the Ce ion electric field is responsible for the variable lifetime. © 2006 American Institute of Physics

Filtration‐histogram based magnetic resonance texture analysis (Mrta) for the distinction of primary central nervous system lymphoma and glioblastoma

Primary central nervous system lymphoma (PCNSL) has variable imaging appearances, which overlap with those of glioblastoma (GBM), thereby necessitating invasive tissue diagnosis. We aimed to investigate whether a rapid filtration histogram analysis of clinical MRI data supports the distinction of PCNSL from GBM. Ninety tumours (PCNSL n = 48, GBM n = 42) were analysed using pre‐treatment MRI sequences (T1‐weighted contrast‐enhanced (T1CE), T2‐weighted (T2), and apparent diffusion coefficient maps (ADC)). The segmentations were completed with proprietary texture analysis software (TexRAD version 3.3). Filtered (five filter sizes SSF = 2–6 mm) and unfil-tered (SSF = 0) histogram parameters were compared using Mann‐Whitney U non‐parametric test-ing, with receiver operating characteristic (ROC) derived area under the curve (AUC) analysis for significant results. Across all (n = 90) tumours, the optimal algorithm performance was achieved using an unfiltered ADC mean and the mean of positive pixels (MPP), with a sensitivity of 83.8%, specificity of 8.9%, and AUC of 0.88. For subgroup analysis with >1/3 necrosis masses, ADC permit-ted the identification of PCNSL with a sensitivity of 96.9% and specificity of 100%. For T1CE‐derived regions, the distinction was less accurate, with a sensitivity of 71.4%, specificity of 77.1%, and AUC of 0.779. A role may exist for cross‐sectional texture analysis without complex machine learning models to differentiate PCNSL from GBM. ADC appears the most suitable sequence, especially for necrotic lesion distinction

Synergistic Effect of Co and Mn Co-Doping on SnO2 Lithium-Ion Anodes

The incorporation of transition metals (TMs) such as Co, Fe, and Mn into SnO2 substantially improves the reversibility of the conversion and the alloying reaction when used as a negative electrode active material in lithium-ion batteries. Moreover, it was shown that the specific benefits of different TM dopants can be combined when introducing more than one dopant into the SnO2 lattice. Herein, a careful characterization of Co and Mn co-doped SnO2 via transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy and X-ray diffraction including Rietveld refinement is reported. Based on this in-depth investigation of the crystal structure and the distribution of the two TM dopants within the lattice, an ex situ X-ray photoelectron spectroscopy and ex situ X-ray absorption spectroscopy were performed to better understand the de-/lithiation mechanism and the synergistic impact of the Co and Mn co-doping. The results specifically suggest that the antithetical redox behaviour of the two dopants might play a decisive role for the enhanced reversibility of the de-/lithiation reaction