Controlled Synthesis of Nanoscale Icosahedral Gold Particles at Room Temperature
Abstract not provided
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Tracking the Light-Induced Excited-State Dynamics and Structural Configurations of an Extraordinarily Long-Lived Metastable State at Room Temperature
Time-resolved X-ray (Tr-XAS) and optical transient absorption (OTA) spectroscopy in the pico-microsecond time scale coupled with Density Functional theory calculations are applied to study the light-induced spin crossover processes of a Fe-based macrocyclic complex in solution. Tr-XAS analysis after light illumination shows the formation of a seven-coordinated high spin quintet metastable state which relaxes to a six-coordinated high spin configuration before decaying to ground state. Kinetic analysis of the macrocyclic complex reveals an unprecedented long-lived decay lifetime of ~42.6 µs. Comparative studies with a non-macrocyclic counterpart illustrate a significantly shortened ~568-old decay lifetime of ~75 ns, and highlight the importance of the ligand arrangement in stabilizing the reactivity of the excited state. Lastly, OTA analysis shows the seven-coordinated high spin state to be formed within ~6.2 ps. Finally, these findings provide a complete understanding of the spin crossover reaction and relaxation pathways of the macrocyclic complex, and reveal the importance of a flexible coordination environment for their rational design.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Sn-Based Alloys Synthesized in an Ionic Liquid at Room Temperature: Cu6Sn5 as a Case Study
Sn-based alloys are increasingly investigated owing to possible electronic/structural modulations of interest for electrocatalysis and energy storage applications. Here, we report on the use of a chemical system consisting of an ionic liquid (1-ethyl-3- methylimidazolium bis(trifluoromethanesulfonyl)imide: [EMIm(+)][TFSI-]) and Sn-based precursor Sn(TFSI)(2) both featuring similar anionic groups. This strategy increases the solubility of the cationic precursor in the IL and avoids the formation of side-products during the precipitation of Sn-nanoparticles formed upon reaction with a reducing agent (NaBH4). Using NMR relaxometry, we further established that these nanoparticles are stabilized by specific interactions with the cationic group of the IL. Targeting the composition Cu6Sn5, we further demonstrated that this approach can be used to prepare Sn-based alloys which could not be prepared using conventional chloride-based precursors.
cyclic voltammetry↗
New Mechanism for the Reduction of Vanadyl Acetylacetonate to Vanadium Acetylacetonate for Room Temperature Flow Batteries
In this study, a new mechanism for the reduction of vanadyl acetylacetonate, VO(acac)2, to vanadium acetylacetonate, V(acac)3, is introduced. V(acac)3 has been studied for use in redox flow batteries (RFBs) for some time; however, contamination by moisture leads to the formation of VO(acac)2. In previous work, once this transformation occurs, it is no longer reversible because there is a requirement for extreme low potentials for the reduction to occur. Here, we propose that, in the presence of excess acetylacetone (Hacac) and free protons (H+), the reduction can take place between 2.25 and 1.5 V versus Na/Na+ via a one-electron-transfer reduction. This reduction can take place in situ during discharge in a novel hybrid Na-based flow battery (HNFB) with a molten Na–Cs alloy as the anode. The in situ recovery of V(acac)3 during discharge is shown to allow the Coulombic efficiency of the HNFB to be ≈100 % with little or no capacity decay over cycles. In addition, utilizing two-electron-transfer redox reactions (i.e., V3+/V4+ and V2+/V3+ redox couples) per V ion to increase the energy density of RFBs becomes possible owing to the in situ recovery of V(acac)3 during discharge. The concept of in situ recovery of material can lead to more advances in maintaining the cycle life of RFBs in the future.
25 ENERGY STORAGE↗
Room-temperature Synthesis of High-entropy Perovskite Oxide Nanoparticle Catalysts via Ultrasonication-based Method
Currently, a sonochemical-based technique for one-pot synthesis of entropy-stabilized perovskite oxide nanoparticle catalysts with high surface area is reported. The high-entropy perovskite oxides were synthesized as monodispersed, spherical nanoparticles with average crystallite size of ~5.9 nm. Taking advantage of the acoustic cavitation phenomenon in ultrasonication process, the nanoparticles of BaSr(ZrHfTi)O 3 , BaSrBi(ZrHfTiFe)O 3 and Ru/BaSrBi(ZrHfTiFe)O 3 were crystallized as single-phase perovskite structures through ultrasonication exposure without calcination. Of utmost importance, the entropically-driven stability of Ru/BaSrBi(ZrHfTiFe)O 3 with excellent dispersion of Ru in the perovskite phase, bestowed the nanoparticles of Ru/BaSrBi(ZrHfTiFe)O 3 with good catalytic activity for CO oxidation.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Surface Modification of Nickel-Rich Cathode Materials by Ionically Conductive Materials at Room Temperature
Nickel-rich cathode materials (LiNi x Mn y Co 1-x-y O 2 , NMC) are promising to push the limits of lithium-ion batteries to higher energy density. This approach is favored in practical applications including electric vehicles and aviation transportation. However, the instability of the NMC at charged state results in safety concerns and poor cycling stability. Surface coating is a practical and effective strategy to address this. Cubic Li7La3Zr2O12 (LLZO) is an ideal coating material regarding the low electron transfer rate and high Li+ conductivity. Thus, a LLZO coating layer can suppress the parasitic reactions in the electrode/electrolyte interface without deteriorating the lithium migration. However, high-temperature calcination seems to inevitably create the chemical couplings between NMC and LLZO, leading to the interdiffusion and degradation of NMC and LLZO crystal structures. This work presents a simple mechanochemical method to effectively coat LLZO on the NMC particle surface. Furthermore, the coated cathode demonstrates superior electrochemical performance compared with the pristine NMC cathode.
25 ENERGY STORAGE↗
Room temperature crystal structure of the fast switching M159T mutant of the fluorescent protein dronpa
Abstract not provided
Kaucikas, Marius↗
Support-Mediated Reversible Redox Dynamics of Pt and Au on CeO2 at Room Temperature
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36 MATERIALS SCIENCE↗
Template‐Directed Growth of Palladium Nanoparticles in Holey Single‐Layer Graphene for High‐Performance Room‐Temperature Hydrogen Sensing
Holey graphene (HG), formed by introducing nanoscale perforations into graphene sheets, combines the structural advantages of continuous sp 2 conjugation with the beneficial effects of high surface area and enhanced chemical reactivity associated with nanoscopic holes. Conventional HG fabrication methods often rely on harsh oxidative treatments that compromise graphene's intrinsic electronic properties by disrupting its sp 2 conjugation. A new approach is introduced to fabricate HG directly from single-layer graphene (SLG), using two-dimensional covalent organic frameworks (COFs) as a template followed by controlled oxygen plasma etching. This method preserves the integrity of the SLG's sp 2 network while producing well-defined holes with an average diameter of 2.7 nm. These hole edges act as reactive sites that facilitate the confined, autoreductive growth of palladium nanoparticles (PdNPs) without external reducing agents. The confined hole geometry prevents NP agglomeration and ensures a uniform size distribution. The resulting Pd@HG hybrid exhibits exceptional chemiresistive hydrogen sensing characteristics, including ultrahigh sensitivity, low detection limits, rapid response and recovery, and long-term stability under both dry and humid conditions. Mechanistic investigations reveal a two-step sensing process involving surface redox interactions and hydrogen absorption into the PdNP lattices. This strategy presents a scalable platform for integrating metal NPs within conductive carbon frameworks for advanced sensing applications.
chemical vapor deposition↗
Aorta Balloon Occlusion in Trauma: Three Cases Demonstrating Multidisciplinary Approach Already on Patient’s Arrival to the Emergency Room
PurposeTo describe the usage of aortic balloon occlusion (ABO), based on a multidisciplinary approach in severe trauma patients, emphasizing the role of the interventional radiologist in primary trauma care.MethodsWe briefly discuss the relevant literature, the technical aspects of ABO in trauma, and a multidisciplinary approach to the bleeding trauma patient. We describe three severely injured trauma patients for whom ABO was part of initial trauma management.ResultsThree severely injured multi-trauma patients were treated by ABO as a bridge to surgery and embolization. The procedures were performed by an interventional radiologist in the early stages of trauma management.ConclusionsThe interventional radiologist and the multidisciplinary team approach can be activated already on severe trauma patient arrival. ABO usage and other endovascular methods are becoming more widely spread, and can be used early in trauma management, without delay, thus justifying the early activation of this multidisciplinary approach.
62 RADIOLOGY AND NUCLEAR MEDICINE↗
Iron-sulfur clusters: the road to room temperature
Abstract Iron-sulfur proteins perform a wide variety of reactions central to the metabolisms of all living organisms. Foundational to their reaction chemistry are the rich electronic structures of their constituent Fe-S clusters, which differ in important ways from the active sites of mononuclear Fe enzymes. In this perspective, we summarize the essential electronic structure features that make Fe-S clusters unique, and point to the need for studies aimed at understanding the electronic basis for their reactivity under physiological conditions. Specifically, at ambient temperature, both the ground state and a large number of excited states are thermally populated, and thus a complete understanding of Fe-S cluster reactivity must take into account the properties, energies, and reactivity patterns of these excited states. We highlight prior research toward characterizing the low-energy excited states of Fe-S clusters that has established what is now a consensus model of these excited state manifolds and the bonding interactions that give rise to them. In particular, we discuss the low-energy alternate spin states and valence electron configurations that occur in Fe-S clusters of varying nuclearities, and finally suggest that there may be unrecognized functional roles for these states. Graphical abstract
Skeel, Brighton A. (ORCID:000000018458088X)↗
IoT in Radiology: Using Raspberry Pi to Automatically Log Telephone Calls in the Reading Room
The work environment for medical imaging such as distractions, ergonomics, distance, temperature, humidity, and lighting conditions generates a paucity of data and is difficult to analyze. The emergence of Internet of Things (IoT) with decreasing cost of single-board computers like Raspberry Pi makes creating customized hardware to collect data from the clinical environment within the reach of a clinical imaging informaticist. This article will walk the reader through a series of basic project using a variety sensors and devices in conjunction with a Pi to gather data, culminating in a complex example designed to automatically detect and log telephone calls.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Room temperature mechanical properties of natural-mineral-based thermoelectrics
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charge transport↗
Observation of Room-Temperature Range Magnetocaloric Effect in PrSr{sub 1−x}Pb{sub x}Mn{sub 2}O{sub 6} (0.4 ≤ x ≤ 0.6) Double-Perovskite Manganite System
The Pr(Sr{sub 1−x}Pb{sub x})Mn{sub 2}O{sub 6} (0.4 ≤ x ≤ 0.6) double-perovskite manganite samples have been produced by using a sol-gel method. The Rietveld refinement method has been used to analyse the structural properties, and the results show that all samples are crystallized in monoclinic structure with P21/n space group without any impurity phase. The temperature dependence of magnetization measurement shows that samples exhibit paramagnetic to ferromagnetic phase transition by decreasing temperature. The values of the T{sub C} are determined as 286, 280 and 278 K for x= 0.4, 0.5 and 0.6 in Pr(Sr{sub 1−x}Pb{sub x})Mn{sub 2}O{sub 6} samples, respectively. Isothermal applied magnetic field-dependent magnetization curves are used to determine both order of magnetic phase transition and magnetic entropy change (ΔS{sub M}) value. −ΔS{sub M} values are found as 3.68, 3.15 and 2.85 J kg{sup − 1} K{sup − 1} for PSPM-4, PSPM-5 and PSPM-6 samples, respectively. Additionally, magnetic phase transition of the samples is identified as second-order magnetic phase transition that indicates accompanying small thermal and magnetic hysteresis to the samples during the phase transition. Relative cooling power (RCP) values are determined as 282, 233 and 268 J kg{sup − 1} for PSPM-4, PSPM-5 and PSPM-6 samples, respectively.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Large Magnetic Entropy Change in Pr{sub 2/3}Sr{sub 1/3}MnO{sub 3}-CuO Composite at Room Temperature
We report in this paper the impact of copper oxide (CuO) on the structural, magnetic, and magnetocaloric properties of Pr{sub 2/3}Sr{sub 1/3}MnO{sub 3} (PSMO) material. Our samples were synthesized by conventional solid-state reaction. The phase formation with no impurities was verified using the X-ray diffraction (XRD). The magnetic properties measured by Magnetic Properties Measurement System (MPMS) show the impact of the AFM CuO semiconductor on the magnetization and the transition temperature of the composite. The magnetic entropy changes were calculated from the isothermal curve of the magnetization as a function of the magnetic field. It is found that a small amount of copper oxide is enough to enhance the magnetocaloric properties of our materials.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗