Facile fabrication of amorphous Al/Fe based metal-organic framework as effective heterogeneous fenton catalyst for environmental remediation.

This study presents a facile preparation and durable amorphous Fe and Al-based MOF nanoplate (AlFe-BTC MOFs) catalyst with notable stability in Fenton reactions. Rigorous characterization using XRD, HR-TEM, and BET confirms the amorphous nature of the synthesized AlFe-BTC MOFs, revealing mesopores (3.4 nm diameter), a substantial surface area (232 m2/g), and a pore volume of 0.69 cc/g. XPS analysis delineates distinct Al2p and Fe2p binding energy values, signifying specific chemical bonding. FE-SEM elemental mapping elucidates the distinctive distribution of Fe and Al within the framework of AlFe-BTC MOFs. In catalytic activity testing, the amorphous AlFe-BTC MOFs exhibited outstanding performance, achieving complete degradation of Methylene blue (MB) dye and 78% TOC removal over 45 min of treatment under mild reaction conditions. The catalyst's durability was assessed, revealing about 75% TOC removal and complete dye decomposition over five successive recycles, with less than 1 mg/L of Fe and Al leaching. UV-Vis spectra revealed the destruction of MB dye over multiple recycling studies. Based on this finding, the amorphous AlFe-BTC MOF nanoplates emerge as a promising solution for efficient dye removal from industrial wastewater, underscoring their potential in advanced environmental remediation processes.

Ultrathin Magnesium-Based Coating as an Efficient Oxygen Barrier for Superconducting Circuit Materials.

Scaling up superconducting quantum circuits based on transmon qubits necessitates substantial enhancements in qubit coherence time. Over recent years, tantalum (Ta) has emerged as a promising candidate for transmon qubits, surpassing conventional counterparts in terms of coherence time. However, amorphous surface Ta oxide layer may introduce dielectric loss, ultimately placing a limit on the coherence time. In this study, a novel approach for suppressing the formation of tantalum oxide using an ultrathin magnesium (Mg) capping layer is presented. Synchrotron-based X-ray photoelectron spectroscopy studies demonstrate that oxide is confined to an extremely thin region directly beneath the Mg/Ta interface. Additionally, it is demonstrated that the superconducting properties of thin Ta films are improved following the Mg capping, exhibiting sharper and higher-temperature transitions to superconductive and magnetically ordered states. Moreover, an atomic-scale mechanistic understanding of the role of the capping layer in protecting Ta from oxidation is established based on computational modeling. This work provides valuable insights into the formation mechanism and functionality of surface tantalum oxide, as well as a new materials design principle with the potential to reduce dielectric loss in superconducting quantum materials. Ultimately, the findings pave the way for the realization of large-scale, high-performance quantum computing systems.

Investigating Anisotropic Magnetoresistance in Epitaxially Strained CoFe Thin Films on a Flexible Mica.

This study investigates the crystal structure, epitaxial relation, and magnetic properties in CoFe thin films deposited on a flexible mica substrate. The epitaxial growth of CoFe thin films was successfully achieved by DC magnetron sputtering, forming three CoFe(002) domains exhibiting four-fold symmetry on the mica substrate. A notable achievement of this work was the attainment of the highest anisotropic magnetoresistance (AMR) value reported to date on a flexible substrate. Additionally, it was observed that the magnetic characteristics of the CoFe films on the flexible mica substrate display reversibility upon strain release. More importantly, the AMR effect of epitaxial CoFe films on flexible mica shows lesser dependence on the crystalline orientation and remains the same under different bending states. These findings demonstrate the potential of utilizing CoFe films on flexible substrates to develop wearable magnetoresistance sensors with diverse applications.

Phase/Interfacial-Engineered Two-Dimensional-Layered WSe2 Films by a Plasma-Assisted Selenization Process: Modulation of Oxygen Vacancies in Resistive Random-Access Memory.

Here, we propose phase and interfacial engineering by inserting a functional WO3 layer and selenized it to achieve a 2D-layered WSe2/WO3 heterolayer structure by a plasma-assisted selenization process. The 2D-layered WSe2/WO3 heterolayer was coupled with an Al2O3 film as a resistive switching (RS) layer to form a hybrid structure, with which Pt and W films were used as the top and bottom electrodes, respectively. The device with good uniformity in SET/RESET voltage and high low-/high-resistance window can be obtained by controlling a conversion ratio from a WO3 film to a 2D-layered WSe2 thin film. The Pt/Al2O3/(2D-layered WSe2/WO3)/W structure shows remarkable improvement to the pristine Pt/Al2O3/W and Pt/Al2O3/2D-layered WO3/W in terms of low SET/RESET voltage variability (-20/20)%, multilevel characteristics (uniform LRS/HRS distribution), high on/off ratio (104-105), and retention (∼105 s). The thickness of the obtained WSe2 was tuned at different gas ratios to optimize different 2D-layered WSe2/WO3 (%) ratios, showing a distinctive trend of reduced and uniform SET/RESET voltage variability as 2D-layered WSe2/WO3 (%) changes from 90/10 (%) to 45/55 (%), respectively. The electrical measurements confirm the superior ability of the metallic 1T phase of the 2D-layered WSe2 over the semiconducting 2H phase. Through systemic studies of RS behaviors on the effect of 1T/2H phases and 2D-layered WSe2/WO3 ratios, the low-temperature plasma-assisted selenization offers compatibility with the temperature-limited 3D integration process and also provides much better thickness control over a large area.

Gamma-Ray Irradiation Induced Ultrahigh Room-Temperature Ferromagnetism in MoS2 Sputtered Few-Layered Thin Films.

Defect engineering is of great interest to the two-dimensional (2D) materials community. If nonmagnetic transition-metal dichalcogenides can possess room-temperature ferromagnetism (RTFM) induced by defects, then they will be ideal for application as spintronic materials and also for studying the relation between electronic and magnetic properties of quantum-confined structures. Thus, in this work, we aimed to study gamma-ray irradiation effects on MoS2, which is diamagnetic in nature. We found that gamma-ray exposure up to 9 kGy on few-layered (3.5 nm) MoS2 films induces an ultrahigh saturation magnetization of around 610 emu/cm3 at RT, whereas no significant changes were observed in the structure and magnetism of bulk MoS2 (40 nm) films even after gamma-ray irradiation. The RTFM in a few-layered gamma-ray irradiated sample is most likely due to the bound magnetic polaron created by the spin interaction of Mo 4d ions with trapped electrons present at sulfur vacancies. In addition, density functional theory (DFT) calculations suggest that the defect containing one Mo and two S vacancies is the dominant defect inducing the RTFM in MoS2. These DFT results are consistent with Raman, X-ray photoelectron spectroscopy, and ESR spectroscopy results, and they confirm the breakage of Mo and S bonds and the existence of vacancies after gamma-ray irradiation. Overall, this study suggests that the occurrence of magnetism in gamma-ray irradiated MoS2 few-layered films could be attributed to the synergistic effects of magnetic moments arising from the existence of both Mo and S vacancies as well as lattice distortion of the MoS2 structure.

Consequences of gamma-ray irradiation on structural and electronic properties of PEDOT:PSS polymer in air and vacuum environments.

In this work, the effects of gamma-ray irradiation (up to 3 kGy) on the structural and electronic properties of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), irradiated in air and vacuum environments are systematically investigated. Raman spectroscopy indicates that there is no significant change in structural conformation of PEDOT:PSS film after gamma-ray irradiation. However, the conductivity of the film decreases as a function of dose in both air and vacuum environments, which can be deduced as a result of defects created in the structure. Hall effect measurements showed higher carrier concentration when the samples are irradiated under vacuum in comparison to the air environment, whereas mobility decreases as a function of dose irrespective of the environment. Furthermore, the electron spin resonance spectra provided evidence of the evolution of polaron population after gamma-ray exposure of 3 kGy, due to the decrease in charge delocalization and molecular ordering of the molecules. This decrease in conductivity and mobility of the PEDOT:PSS films irradiated in air and vacuum environments can be mainly ascribed to the defects and radical formation after gamma-ray exposure, favoring chain scission or cross-linking of the polymers.

Correction: Consequences of gamma-ray irradiation on structural and electronic properties of PEDOT:PSS polymer in air and vacuum environments.

[This corrects the article DOI: 10.1039/D1RA03463D.].

Gamma Ray Irradiation Enhances the Linkage of Cotton Fabrics Coated with ZnO Nanoparticles.

In this work, we aim to study zinc oxide (ZnO)-based functional materials over cotton fabrics and their effects after gamma ray exposure of 9 kGy. We found that the binding of the nanoparticles with cotton fabrics can be enhanced after irradiation. This could be due to the oxygen deficiency or defects created in the interface between ZnO and cotton fabrics after irradiation. Near-edge X-ray absorption fine structure and X-ray photoelectron spectroscopy (XPS) were used to detect the oxygen inadequacies generated in the interior and at the surface of the ZnO nanoparticles after gamma ray exposure. XPS results showed that the binding energy of Zn shifts by 2 eV at 1.5 kGy and by 4 eV at 9 kGy. This huge shift of about 4 eV is completely different from other works due to the reaction that takes place on the interface between ZnO nanostructures and cotton fabrics after gamma ray irradiation. Overall, this work suggests that after gamma ray irradiation, there is an enhanced level of binding between the coated functional nanoparticles and cotton fabrics, which can be advantageous for the textile industries.

Stoichiometry-Controlled MoxW1-xTe2 Nanowhiskers: A Novel Electrocatalyst for Pt-Free Dye-Sensitized Solar Cells.

Novel polymorphic MoxW1-xTe2-based counter electrodes possess high carrier mobility, phase-dependent lattice distortion, and surface charge density wave to boost the charge-transfer kinetics and electrocatalytic activity in dye-sensitized solar cells (DSSCs). Here, we report the syntheses of stoichiometry-controlled binary and ternary MoxW1-xTe2 nanowhiskers directly on carbon cloth (CC), denoted by MoxW1-xTe2/CC, with an atmospheric chemical vapor deposition technique. The synthesized MoxW1-xTe2/CC samples, including 1T'-MoTe2/CC, Td-WTe2/CC, Td-Mo0.26W0.73Te2.01/CC, and 1T'- & Td-Mo0.66W0.32Te2.02/CC, were then employed as different counter electrodes to study their electrochemical activities and efficiencies in DSSCs. The photovoltaic parameter analysis manifests that MoxW1-xTe2/CCs are more stable than a standard Pt/CC in the I-/I3- electrolyte examined by cyclic voltammetry over 100 cycles. A 1T'- & Td-Mo0.66W0.32Te2.02/CC-based DSSC can achieve a photocurrent density of 16.29 mA cm-2, a maximum incident photon-to-electron conversion efficiency of 90% at 550 nm excitation, and an efficiency of 9.40%, as compared with 8.93% of the Pt/CC counterpart. Moreover, the 1T'- & Td-Mo0.66W0.32Te2.02/CC shows lower charge-transfer resistance (0.62 Ω cm2) than a standard Pt/CC (1.19 Ω cm2) in electrocatalytic reactions. Notably, MoxW1-xTe2 nanowhiskers act as an electron expressway by shortening the path of carrier transportation in the axial direction from a counter electrode to electrolytic ions to enhance the reaction kinetics in DSSCs. This work demonstrates that the nanowhisker-structured 1T'- & Td-Mo0.66W0.32Te2.02/CC with high carrier mobility and robust surface states can serve as a highly efficient counter electrode in DSSCs to replace the conventional Pt counter electrode for electrocatalytic applications.

Influence of gamma-ray irradiation and post-annealing studies on pentacene films: the anisotropic effects on structural and electronic properties.

In this work, γ-ray irradiation effects on pentacene thin films are investigated in terms of the change in the crystallinity, and electronic structure as well as chemical states of the film. The pentacene films are γ-irradiated up to 3 kGy and then characterized using synchrotron X-ray diffraction, near edge X-ray absorption fine structure (NEXAFS) and X-ray photoelectron spectroscopy. We found that γ-ray irradiation creates defects, resulting in a decrease of X-ray diffraction intensity both in the plane normal and in-plane directions. From angle dependent NEXAFS; the transition of C 1s to π* orbital for irradiated samples increases; suggesting that the unoccupied π* states enhance due to defects or radical formation in pentacene thin films. Additionally, the in-plane resistivity shows a decreasing trend of resistance after irradiation. This trend of increase in conductivity is also consistent with C 1s to π transition, which manifests the increase in carrier concentration. Hall effect measurements further confirmed the increase in carrier concentration as a function of dose; however, the mobility of the sample decreases as the dose rate increases due to the defects created. By post-irradiation annealing, the thin film phase diffraction intensity can be recovered. Altogether, the anisotropic studies on pentacene films disclosed that the irradiation leads to defect formation along in-plane and plane normal directions. Overall, these results suggest that pentacene is one of the robust organic electronic materials; whose structure remains mostly intact even after irradiation up to a dose of 3 kGy.