10 research outputs found

    Quantification of Hybrid Topological Spin Textures and Their Nanoscale Fluctuations in Ferrimagnets

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    Noncolinear spin textures, including chiral stripes and skyrmions, have shown great potential in spintronics. Basic configurations of spin textures are either Bloch or Néel types, and the intermediate hybrid type has rarely been reported. A major challenge in identifying hybrid spin textures is to quantitatively determine the hybrid angle, especially in ferrimagnets with weak net magnetization. Here, we develop an approach to quantify magnetic parameters, including chirality, saturation magnetization, domain wall width, and hybrid angle with sub-5 nm spatial resolution, based on Lorentz four-dimensional scanning transmission electron microscopy (Lorentz 4D-STEM). We find strong nanometer-scale variations in the hybrid angle and domain wall width within structurally and chemically homogeneous FeGd ferrimagnetic films. These variations fluctuate during different magnetization circles, revealing intrinsic local magnetization inhomogeneities. Furthermore, hybrid skyrmions can also be nucleated in FeGd films. These analyses demonstrate that the Lorentz 4D-STEM is a quantitative tool for exploring complex spin textures

    Synthesis of Pincer Hydrido Ruthenium Olefin Complexes for Catalytic Alkane Dehydrogenation

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    A series of new hydrido Ru­(II) olefin complexes supported by isopropyl-substituted pincer ligands have been synthesized and characterized. These complexes are thermally robust and active for catalytic transfer and acceptorless alkane dehydrogenation. Notably, the alkane dehydrogenation catalysts are tolerant of a number of polar functional species

    Influence of the concentration of seawater on the early hydration properties of calcium sulphoaluminate (CSA) cement: A preliminary study

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    This research investigates the effect of seawater of different concentrations on the hydration process and microstructure of calcium sulphoaluminate (CSA) cement. It studies the CSA cement pastes via experiments carried out to determine the initial and final setting times, mechanical strength and chemical shrinkage with X-ray diffraction (XRD), scanning electron microscopy (SEM) and simultaneous differential thermal-thermogravimetric (DTA-TG) analysis. The DTA-TG and XRD results showed that the main hydration products were ettringite (AFt) and aluminum hydroxide in the CSA cement paste mixed with both freshwater and seawater, while a small amount of ettringite (AFt) became monosulfate (AFm) in the freshwater-mixed CSA cement. The SEM results demonstrate that seawater can improve the microstructure of CSA cement paste in the early stage of hydration (1 d) but impairs the microstructure of the CSA cement matrix in the later stage of hydration (7 d). The experimental results also indicate that a high concentration of seawater can extend the setting time, increase the chemical shrinkage and decrease the mechanical strength of CSA cement

    Point-of-Use SERS Approach for Efficient Determination and Removal of Phthalic Acid Esters Based on a Metal–Organic Framework-Coated Melamine Sponge

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    Phthalic acid esters (PAEs) are ubiquitous environmental contaminants, and their real-time monitoring and removal remain challenging. Herein, a point-of-use (POU) device integrating adsorption, surface-enhanced Raman spectroscopy (SERS), and removal strategy was developed and realized ultrafast on-site determination of PAEs and cleanup of them from water. A piece of flexible melamine sponge (MS) was coated with gold nanostars (AuNSs) and metal–organic frameworks (MOFs), thus obtaining SERS activity and adsorption capacity. Based on this multifunctional AuNSs@MOFs/MS composite, clear trends were observed between SERS signal intensity and concentration of di(2-ethylhexyl)phthalate (DEHP) and dibutyl phthalate (DBP). The method detection limits of DEHP and DBP were calculated to be 0.75 × 10–7 and 0.67 × 10–7 M in water, respectively, proving good sensitivity. Furthermore, this POU device exhibited satisfactory adsorption capacity (∌82.3 g/g for DBP and ∌90.0 g/g for DEHP), high adsorption efficiency (equilibrium in 100 s), and good regeneration capability (removal efficiency >70% after 5 cycles). The applicability of this device was verified by its good determination and removal performance in real environmental water matrices. The whole process could be completed within 5 min. This approach provides a new POU alternative for real-time monitoring and removal of PAEs in water

    Sulfur-Doped NiFe Hydroxide Nanobowls with Wrinkling Patterns for Photothermal Cancer Therapy

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    Hierarchical multiscale wrinkling nanostructures have shown great promise for many biomedical applications, such as cancer diagnosis and therapy. However, synthesizing these materials with precise control remains challenging. Here, we report a sulfur doping strategy to synthesize sub-1 nm NiFe hydroxide ultrathin nanosheets (S-NiFe HUNs). The introduction of sulfur affects the reduction of the band gap and the adjustment of the electronic structure, thereby improving the light absorption ability of the S-NiFe HUNs. Additionally, S-NiFe HUNs show a multilayered nanobowl-like structure that enables multiple reflections of incident light inside the nanostructure, which improved the utilization of incident light and achieved high photothermal conversion. As a result, the as-prepared product with hydrophilic modification (dS-NiFe HUNs) demonstrated enhanced tumor-killing ability in vitro. In a mouse model of breast cancer, dS-NiFe HUNs combined with near-infrared light irradiation greatly inhibited tumor growth and prolonged the mice survival. Altogether, our study demonstrates the great potential of dS-NiFe HUNs for cancer photothermal therapy applications

    Exploring the Complex Impact of Proteins on Dopamine Polymerization: Mechanisms and Strategies for Modulation

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    Polydopamine (pDA) is a valuable material with wide-ranging potential applications. However, the complex and debated nature of dopamine polymerization complicates our understanding. Specifically, the impact of foreign substances, especially proteins, on pDA formation adds an additional layer of subtlety and complexity. This study delves into specific surface features of proteins that predominantly shape their impact on dopamine polymerization. Notably, the biotin-binding site emerges as a critical region responsible for the pronounced inhibitory effect of avidin and neutravidin on the dopamine polymerization process. The binding of biotin successfully mitigates these inhibitory effects. Moreover, several nucleases demonstrated a significant hindrance to pDA formation, with their impact substantially alleviated through the introduction of DNA. It is speculated that hydrogen bonding, electrostatic, cation−π, and/or hydrophobic interactions may underlie the binding between protein surfaces and diverse oligomeric intermediates formed by the oxidation products of dopamine. Additionally, we observed a noteworthy blocking effect on the dopamine polymerization reaction induced by erythropoietin (EPO), a glycoprotein hormone known for its role in stimulating red blood cell production and demonstrating neuroprotective effects. The inhibitory influence of EPO persisted even after deglycosylation. These findings not only advance our comprehension of the mechanisms underlying dopamine polymerization but also provide strategic insights for manipulating the reaction to tailor desired biomaterials

    Density Measurements of Various Molten Sodium, Magnesium, Potassium, and Uranium Chloride Salt Compositions Using Neutron Imaging

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    With an increased interest in the use of molten salts for energy generation, obtaining thermophysical properties of salt mixtures becomes critical for the understanding of salt performance and behavior. Density is one of the significant thermophysical properties of salt systems. This work presents the density measurement of molten chloride salt mixtures using neutron imaging. This work was performed at the Oak Ridge National Laboratory High-Flux Isotope Reactor. Resulting densities as a function of temperature for different molten chloride salts from this work were compared with calculated values using Redlich–Kister modeling. Agreement between the calculated and measured values was within 1–10%, with the exception of the ternary UCl3–NaCl–KCl salt that showed a 32% discrepancy between several literature reports; however, the results did align well with another neutron radiography article. Analysis of the radiographs suggests that microbubbles in the ternary mixture might have biased the density measurements

    Expanding the Scope of Polymerization-Induced Self-Assembly: Z‑RAFT-Mediated Photoinitiated Dispersion Polymerization

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    In this communication, we developed the first well-controlled Z-RAFT (RAFT = reversible addition–fragmentation chain transfer) mediated polymerization-induced self-assembly (PISA) formulation based on photoinitiated RAFT dispersion polymerization of <i>tert</i>-butyl acrylate (<i>t</i>BA) in ethanol/water (60/40, w/w) at room temperature using a Z-type macromolecular chain transfer agent (macro-CTA). Polymerizations proceeded rapidly via the exposure of visible-light irradiation (405 nm, 0.45 mW/cm<sup>2</sup>) with high monomer conversion (>95%) being achieved within 1 h. A variety of polymer nano-objects (spheres, worms, and vesicles) with narrow molar mass distributions were prepared by this Z-RAFT mediated PISA formulation. Silver nanoparticles were loaded with the vesicles via in situ reduction, which can be used as a catalyst for the reduction of methylene blue (MB) in the presence of NaBH<sub>4</sub>. Finally, gel permeation chromatography (GPC) analysis demonstrated that the corona block and the core-forming block could be cleaved by treating with excess initiator. This novel PISA formulation will greatly expand the scope of PISA and provide more mechanistic insights into the PISA research

    Multimodal Encapsulation to Selectively Permeate Hydrogen and Engineer Channel Conduction for p‑Type SnO<sub><i>x</i></sub> Thin-Film Transistor Applications

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    It has been challenging to synthesize p-type SnOx (1 x < 2) and engineer the electrical properties such as carrier density and mobility due to the narrow processing window and the localized oxygen 2p orbitals near the valence band. Herein, we report on the multifunctional encapsulation of p-SnOx to limit the surface adsorption of oxygen and selectively permeate hydrogen into the p-SnOx channel for thin-film transistor (TFT) applications. Time-of-flight secondary ion mass spectrometry (ToF-SIMS) measurements identified that ultrathin SiO2 as a multifunctional encapsulation layer effectively suppressed the oxygen adsorption on the back channel surface of p-SnOx and selectively diffused hydrogen across the entire thickness of the channel. Encapsulated p-SnOx-based TFTs demonstrated much enhanced channel conductance modulation in response to the gate bias applied, featuring higher on-state current and lower off-state current (on/off ratio > 103), field effect mobility of 3.41 cm2/(V s), and threshold voltages of ∌5–10 V. The fabricated devices show minimal deviations as small as ±6% in the TFT performance parameters, which demonstrates good reproducibility of the fabrication process. The relevance between the TFT performance and the effects of hydrogen permeation is discussed in regard to the intrinsic and extrinsic doping mechanisms. Density functional theory calculations reveal that hydrogen-related impurity complexes are in charge of the enhanced channel conductance with gate biases, which further supports the selective permeation of hydrogen through a thin SiO2 encapsulation
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