Investigating the interaction of uranium(VI) with diatoms and their bacterial community: A microscopic and spectroscopic study.

Diatoms and bacteria play a vital role in investigating the ecological effects of heavy metals in the environment. Despite separate studies on metal interactions with diatoms and bacteria, there is a significant gap in research regarding heavy metal interactions within a diatom-bacterium system, which closely mirrors natural conditions. In this study, we aim to address this gap by examining the interaction of uranium(VI) (U(VI)) with Achnanthidium saprophilum freshwater diatoms and their natural bacterial community, primarily consisting of four successfully isolated bacterial strains (Acidovorax facilis, Agrobacterium fabrum, Brevundimonas mediterranea, and Pseudomonas peli) from the diatom culture. Uranium (U) bio-association experiments were performed both on the xenic A. saprophilum culture and on the four bacterial isolates. Scanning electron microscopy and transmission electron microscopy coupled with spectrum imaging analysis based on energy-dispersive X-ray spectroscopy revealed a clear co-localization of U and phosphorus both on the surface and inside A. saprophilum diatoms and the associated bacterial cells. Time-resolved laser-induced fluorescence spectroscopy with parallel factor analysis identified similar U(VI) binding motifs both on A. saprophilum diatoms and the four bacterial isolates. This is the first work providing valuable microscopic and spectroscopic data on U localization and speciation within a diatom-bacterium system, demonstrating the contribution of the co-occurring bacteria to the overall interaction with U, a factor non-negligible for future modeling and assessment of radiological effects on living microorganisms.

Structural Regulation of Au-Pt Bimetallic Aerogels for Catalyzing the Glucose Cascade Reaction.

Bimetallic nanostructures are promising candidates for the development of enzyme-mimics, yet the deciphering of the structural impact on their catalytic properties poses significant challenges. By leveraging the structural versatility of nanocrystal aerogels, this study reports a precise control of Au-Pt bimetallic structures in three representative structural configurations, including segregated, alloy, and core-shell structures. Benefiting from a synergistic effect, these bimetallic aerogels demonstrate improved peroxidase- and glucose oxidase-like catalytic performances compared to their monometallic counterparts, unleashing tremendous potential in catalyzing the glucose cascade reaction. Notably, the segregated Au-Pt aerogel shows optimal catalytic activity, which is 2.80 and 3.35 times higher than that of the alloy and core-shell variants, respectively. This enhanced activity is attributed to the high-density Au-Pt interface boundaries within the segregated structure, which foster greater substrate affinity and superior catalytic efficiency. This work not only sheds light on the structure-property relationship of bimetallic catalysts but also broadens the application scope of aerogels in biosensing and biological detections.

At the Limit of Interfacial Sharpness in Nanowire Axial Heterostructures.

As semiconductor devices approach dimensions at the atomic scale, controlling the compositional grading across heterointerfaces becomes paramount. Particularly in nanowire axial heterostructures, which are promising for a broad spectrum of nanotechnology applications, the achievement of sharp heterointerfaces has been challenging owing to peculiarities of the commonly used vapor-liquid-solid growth mode. Here, the grading of Al across GaAs/AlxGa1-xAs/GaAs heterostructures in self-catalyzed nanowires is studied, aiming at finding the limits of the interfacial sharpness for this technologically versatile material system. A pulsed growth mode ensures precise control of the growth mechanisms even at low temperatures, while a semiempirical thermodynamic model is derived to fit the experimental Al-content profiles and quantitatively describe the dependences of the interfacial sharpness on the growth temperature, the nanowire radius, and the Al content. Finally, symmetrical Al profiles with interfacial widths of 2-3 atomic planes, at the limit of the measurement accuracy, are obtained, outperforming even equivalent thin-film heterostructures. The proposed method enables the development of advanced heterostructure schemes for a more effective utilization of the nanowire platform; moreover, it is considered expandable to other material systems and nanostructure types.

Optical Thin Films in Space Environment: Investigation of Proton Irradiation Damage.

The present work reports a systematic study of the potential degradation of metals and dielectric thin films in different space environments. The mono- and bilayers selected are made of materials commonly used for the realization of optical components, such as reflective mirrors or building blocks of interferential filters. More than 400 samples were fabricated and irradiated with protons at different energies on ground-based facilities. The fluences were selected as a result of simulations of the doses delivered within a long-term space mission considering different orbits (Sun close, Jovian, and Geostationary orbits). In order to stress the samples at different depths and layer interfaces, experiments were carried out with a range of proton energies within 1 and 10 MeV values. An estimate of a safe maximum fluence has been provided for each type of sample at each energy. The damage mechanism, when present, has been investigated with different optical and structural techniques.

Multi-Level Switching of Spin-Torque Ferromagnetic Resonance in 2D Magnetite.

2D magnetic materials hold substantial promise in information storage and neuromorphic device applications. However, achieving a 2D material with high Curie temperature (TC), environmental stability, and multi-level magnetic states remains a challenge. This is particularly relevant for spintronic devices, which require multi-level resistance states to enhance memory density and fulfil low power consumption and multi-functionality. Here, the synthesis of 2D non-layered triangular and hexagonal magnetite (Fe3O4) nanosheets are proposed with high TC and environmental stability, and demonstrate that the ultrathin triangular nanosheets show broad antiphase boundaries (bAPBs) and sharp antiphase boundaries (sAPBs), which induce multiple spin precession modes and multi-level resistance. Conversely, the hexagonal nanosheets display slip bands with sAPBs associated with pinning effects, resulting in magnetic-field-driven spin texture reversal reminiscent of "0" and "1" switching signals. In support of the micromagnetic simulation, direct explanation is offer to the variation in multi-level resistance under a microwave field, which is ascribed to the multi-spin texture magnetization structure and the randomly distributed APBs within the material. These novel 2D magnetite nanosheets with unique spin textures and spin dynamics provide an exciting platform for constructing real multi-level storage devices catering to emerging information storage and neuromorphic computing requirements.

Spin Effect to Regulate the Electronic Structure of Ir─Fe Aerogels for Efficient Acidic Water Oxidation.

"Spin" has been recently reported as an important degree of electronic freedom to promote catalysis, yet how it influences electronic structure remains unexplored. This work reports the spin-induced orbital hybridization in Ir─Fe bimetallic aerogels, where the electronic structure of Ir sites is effectively regulated by tuning the spin property of Fe atoms. The spin-optimized electronic structure boosts oxygen evolution reaction (OER) electrocatalysis in acidic media, resulting in a largely improved catalytic performance with an overpotential of as low as 236 mV at 10 mA cm-2. Furthermore, the gelation kinetics for the aerogel synthesis is improved by an order of magnitude based on the introduction of a magnetic field. Density functional theory calculation reveals that the increased magnetic moment of Fe (3d orbital) changes the d-band structure (i.e., the d-band center and bandwidth) of Ir (5d orbital) via orbital hybridization, resulting in optimized binding of reaction intermediates. This strategy builds the bridge between the electron spin theory with the d-band theory and provides a new way for the design of high-performance electrocatalysts by using spin-induced orbital interaction.

Cobalt-based Co3Mo3N/Co4N/Co Metallic Heterostructure as a Highly Active Electrocatalyst for Alkaline Overall Water Splitting.

Alkaline water electrolysis holds promise for large-scale hydrogen production, yet it encounters challenges like high voltage and limited stability at higher current densities, primarily due to inefficient electron transport kinetics. Herein, a novel cobalt-based metallic heterostructure (Co3Mo3N/Co4N/Co) is designed for excellent water electrolysis. In operando Raman experiments reveal that the formation of the Co3Mo3N/Co4N heterointerface boosts the free water adsorption and dissociation, increasing the available protons for subsequent hydrogen production. Furthermore, the altered electronic structure of the Co3Mo3N/Co4N heterointerface optimizes ΔGH of the nitrogen atoms at the interface. This synergistic effect between interfacial nitrogen atoms and metal phase cobalt creates highly efficient active sites for the hydrogen evolution reaction (HER), thereby enhancing the overall HER performance. Additionally, the heterostructure exhibits a rapid OH- adsorption rate, coupled with great adsorption strength, leading to improved oxygen evolution reaction (OER) performance. Crucially, the metallic heterojunction accelerates electron transport, expediting the afore-mentioned reaction steps and enhancing water splitting efficiency. The Co3Mo3N/Co4N/Co electrocatalyst in the water electrolyzer delivers excellent performance, with a low 1.58 V cell voltage at 10 mA cm-2, and maintains 100 % retention over 100 hours at 200 mA cm-2, surpassing the Pt/C||RuO2 electrolyzer.

Low-temperature diffusion in thin-film Pt-(Au-)-Co heterostructures: a structural and magnetic characterization.

Formation of functional thin films for nanoelectronics and magnetic data storage via thermally induced diffusion-driven structural phase transformations in multilayer stacks is a promising technology-relevant approach. Ferromagnetic thin films based on Co Pt alloys are considered as a material science platform for the development of various applications such as spin valves, spin orbit torque devices, and high-density data storage media. Here, we study diffusion processes in Pt-Co-based stacks with the focus on the effect of layers inversion (Pt/Co/substrate versus Co/Pt/substrate) and insertion of an intermediate Au layer on the structural transitions and magnetic properties. We demonstrate that the layer stacking has a pronounced effect on the diffusion rate at temperatures, where the diffusion is dominated by grain boundaries. We quantify effective diffusion coefficients, which characterize the diffusion rate of Co and Pt through the interface and grain boundaries, providing the possibility to control the homogenization rate of the Pt-Co-based heterostructures. The obtained values are in the range of 10-16-10-13cm2s-1for temperatures of 150 °C-350 °C. Heat treatment of the thin-film samples results in the coercivity enhancement, which is attributed to short-range chemical ordering effects. We show that introducing an additional Au intermediate layer leads to an increase of the coercive field of the annealed samples due to a modification of exchange coupling between the magnetic grains at the grain boundaries.