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The oxidation of tetraselenatetracene (TSeT) by tetracyanoquinodimethane in the presence of dysprosium(III) tris(hexafluoroacetylacetonate), DyIII(hfac)3, produces black crystals of {TSeT1.5}â+[DyIII(hfac)4]- (1) salt, which combines conducting and magnetic sublattices. It contains one-dimensional stacks composed of partially oxidized TSeT molecules (formal averaged charge is +2/3). Dimers and monomers can be outlined within these stacks with charge and spin density redistribution. The spin triplet state of the dimers is populated above 128 K with an estimated singlet-triplet energy gap of 542 K, whereas spins localized on the monomers show paramagnetic behavior. A semiconducting behavior is observed for 1 with the activation energy of 91 meV (measured by the four-probe technique for an oriented single crystal). The DyIII ions coordinate four hfac- anions in [DyIII(hfac)4]-, providing D2d symmetry. Slow magnetic relaxation is observed for DyIII under an applied static magnetic field of 1000 Oe, and 1 is a single-ion magnet (SIM) with spin reversal barrier Ueff = 40.2 K and magnetic hysteresis at 2 K. Contributions from DyIII and TSeTâ+ paramagnetic species are seen in EPR. The DyIII ion rarely manifests EPR signals, but such signal is observed in 1. It appears due to narrowing below 30 K and has g4 = 6.1871 and g5 = 2.1778 at 5.4 K.
Assuntos
Disprósio , Semicondutores , Disprósio/química , Ânions/química , Dimerização , Modelos Moleculares , Fenômenos Magnéticos , MagnetismoRESUMO
For materials with coexisting phases, the transition from a random to an ordered distribution of materials often generates new mechanisms. Although the magnetic confinement effect has improved the electromagnetic (EM) performance, the transition from random to ordered magnetic confinement positions remains a synthetic challenge, and the underlying mechanisms are still unclear. Herein, precise control of magnetic nanoparticles is achieved through a spatial confinement growth strategy, preparing five different modalities of magnetic confined carbon fiber materials, effectively inhibiting magnetic agglomeration. Systematic studies have shown that the magnetic confinement network can refine CoNi NPs size and enhance strong magnetic coupling interactions. Compared to CoNi@HCNFs on the hollow carbon fibers (HCNFs) outer surface, HCNFs@CoNi constructed on the inner surface induce stronger spatial charge polarization relaxation at the interface and exhibit stronger magnetic coupling interactions at the inner surface due to the high-density magnetic coupling units at the micro/nanoscale, thereby respectively enhancing dielectric and magnetic losses. Remarkably, they achieve a minimum reflection loss (RLmin) of -64.54 dB and an absorption bandwidth of 5.60 GHz at a thickness of 1.77 mm. This work reveals the microscale mechanism of magnetic confinement-induced different polarization relaxation and magnetic response, providing a new strategy for designing magnetic materials.
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Compact reliable structure and strong electromechanical coupling are hot pursuits in piezoelectric vibration energy harvester (PVEH) design. PVEH with a static arc stopper makes piezoelectric stress uniformly distributed and widens the frequency band by collision but wastes space. This Article proposes a hinged PVEH with two arc mass stoppers (AS-H-PVEH). Two arc stoppers as movable masses increase the vibration energy and the effective electromechanical coupling coefficient to achieve strong electromechanical coupling. AS-H-PVEH generates a 4.1 mW power output at 11.6-12.0 Hz and 0.2 g. AS-H-PVEH sustains 4 g acceleration vibration for 10 min without attenuation. To offset the resonance frequency increase caused by arc contact, we discuss the magnetic coupling, and axial force effects are discussed. The design of the arc stopper radius, nonlinear electromechanical coupling model, and system parameter identification method are presented. The displacement varied mechanical quality factor and effective electromechanical coupling coefficient are considered in the modified model for the first time. The model obtained good agreement under experiments. The power generation and driven wireless sensor performance of AS-H-PVEH was verified. This research has important theoretical and application value for the performance optimization of PVEH with an arc stopper.
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Soft magnetic spinel ferrites are indispensable parts in devices such as transformers and inductors. Mechanical surface processing is a necessary step to realize certain shapes and surface roughness in producing the ferrite but also has a negative effect on the magnetic properties of the ferrite. In the past few years, a new surface layer was always believed to form during the mechanical surface processing, but the change of atomic structure on the surface and its effect on the magnetic structure remain unclear. Herein, an interface structure consisting of a rock-salt sublayer, distorted NiFe2O4 sublayer, and pristine NiFe2O4 was found to form on mechanically polished single-crystal NiFe2O4 ferrite. Such an interface structure is produced by phase transformation and lattice distortion induced by the mechanical processing. The magnetic domain observation and electrical property measurement also indicate that the magnetic and electrical anisotropy are both enhanced by the interface structure. This work provides deep insight into the surface structure evolution of spinel ferrite by mechanical processing.
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The emergence of an intrinsic quantum anomalous Hall (QAH) insulator with long-range magnetic order triggers unprecedented prosperity for combining topology and magnetism in low dimensions. Here, based on stacked two-dimensional LiFeTe, we confirm that magnetic coupling and topological electronic states can be simultaneously manipulated by just changing the layer numbers. Monolayer LiFeTe shows intralayer ferrimagnetic coupling, behaving as a QAH insulator with Chern number C = 2. Beyond the monolayer, the odd and even layers of LiFeTe correspond to uncompensated and compensated interlayer antiferromagnets, resulting in unexpected QAH and quantum spin Hall (QSH) states, respectively. Moreover, the spin Chern number is proportional to the stacking layer numbers in even-layer LiFeTe, proving that the spin Hall conductivity can be continuously enhanced by increasing layer numbers. Therefore, the odd-even-layer-dependent QAH and QSH effects found in LiFeTe topological insulators offer new insight into regulating quantum states in two-dimensional topological materials.
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Anionic ancillary ligands play a critical role in the construction of rare earth (RE) metal complexes due to the large influence on the stability of the molecule and engendering emergent electronic properties that are of interest in a plethora of applications. Supporting ligands comprising oxygen donor atoms are highly pursued in RE chemistry owing to the high oxophilicity innate to these ions. The scarcely employed bis(acyl)phosphide (BAP) ligands feature oxygen coordination sites and contain a phosphide backbone rendering it attractive for RE-coordination chemistry. Here, we integrate bis(mesitoyl)phosphide (mesBAP) as an ancillary ligand into REIII chemistry to generate the first dinuclear trivalent RE complexes containing BAP ligands; [{mesBAP}2RE(THF)(µ-Cl)]2 (RE=Y, (1), Gd (2), and Dy (3); THF=tetrahydrofuran). Each RE center is ligated to two monoanionic mesBAP ligands, one THF molecule and one chloride ion. All three molecules were characterized through single-crystal X-ray diffraction, 31P NMR, IR and UV-Vis spectroscopy. 31P, 1H and 13C NMR on the diamagnetic yttrium congener 1 confirm asymmetric ligand coordination. DFT calculations conducted on 2 provided insight into the electronic structure. The magnetic properties of 2 and 3 were investigated via SQUID magnetometry. The GdIII ions exhibit weak antiferromagnetic coupling, corroborated by DFT results.
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Binary superparticles formed by self-assembling two different types of nanoparticles may utilize the synergistic interactions and create advanced multifunctional materials. Bi-magnetic superparticles with a core-shell structure have unique properties due to their specific spatial configurations. Herein, we built Mn3O4@Ni core-shell binary superparticles via an emulsion self-assembly technique. The superparticles are generated with a spherical morphology, and have a typical average size of about 240 nm. By altering the ratio of the two magnetic nanoparticles, the thickness of Ni shells can be adjusted. Oleic acid ligands are crucial for the formation of core-shell structure. Magnetic analysis suggests that core-shell superparticles display dual-phase magnetic interactions, contrasting with the single-phase magnetic behaviors of commonly core-shell magnetic nanoparticles. The calculation on the effective magnetic anisotropy constants indicates that the presence of Ni shell layers reduces the dipole interactions among the Mn3O4 core particles. Due to the presence of Ni nanoparticle shells, the blocking temperature of Mn3O4 is reduced, while the Curie temperature of Mn3O4 is independent on Ni content. Tunable magnetic properties can be achieved by modulating the Ni nanoparticle shell thickness. This study offers insights for the development of core-shell superparticles with varied magnetic characteristics.
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Ocean energy harvesting based on a triboelectric nanogenerator (TENG) has great application potential, while the encapsulation of triboelectric devices in water poses a critical issue. Herein, a triboelectric-electromagnetic hybrid nanogenerator (TE-HNG) consisting of TENGs and electromagnetic generators (EMGs) is proposed to harvest water flow energy. A magnetic coupling transmission component is applied to replace traditional bearing structures, which can realize the fully enclosed packaging of the TENG devices and achieve long-lasting energy harvesting from water flow. Under the intense water impact, magnetic coupling reduces the possibility of internal gear damage due to excessive torque, indicating superior stability and robustness compared to conventional TENG. At the waterwheel rotates speed of 75 rpm, the TE-HNG can generate an output peak power of 114.83 mW, corresponding to a peak power density of 37.105 W m-3. After 5 h of continuous operation, the electrical output attenuation of TENG is less than 3%, demonstrating excellent device durability. Moreover, a self-powered temperature sensing system and a self-powered cathodic protection system based on the TE-HNG are developed and illustrated. This work provides a prospective strategy for improving the output stability of TENGs, which benefits the practical applications of the TENGs in large-scale blue energy harvesting.
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Extremely low-frequency (ELF) electromagnetic (EM) waves adeptly propagate in harsh cross-medium environments, overcoming rapid decay that hinders high-frequency counterparts. Traditional antennas, however, encounter challenges concerning size, efficiency, and power. Here, drawing inspiration from nature, we present a groundbreaking piezo-actuated, bionic flapping-wing magnetic-dipole resonator (BFW-MDR), operating in the electro-mechano-magnetic coupling mechanism, designed for efficient ELF EM wave transmission. The unique rigid-flexible hybrid flapping-wing structure magnifies rotation angles of anti-phase magnetic dipoles by tenfold, leading to constructive superposition of emitted magnetic fields. Consequently, the BFW-MDR exhibits a remarkable quality factor of 288 and an enhanced magnetic field emission of 514 fT at 100 meters with only 6.9 mW power consumption, surpassing traditional coil antennas by three orders of magnitude. The communication rate is doubled by the ASK+PSK modulation method. Its robust performance in cross-medium communication, even amidst various interferences, underscores its potential as a highly efficient antenna for underwater and underground applications.
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Photosynthetic water splitting, when synergized with hydrogen production catalyzed by hydrogenases, emerges as a promising avenue for clean and renewable energy. However, theoretical calculations have faced challenges in elucidating the low-lying spin states of iron-sulfur clusters, which are integral components of hydrogenases. To address this challenge, we employ the Extended Broken-Symmetry method for the computation of the cubane-[Fe3S4] cluster within the [FeNi] hydrogenase enzyme. This approach rectifies the error caused by spin contamination, allowing us to obtain the magnetic exchange coupling constant and the energy level of the low-lying state. We find that the Extended Broken-Symmetry method provides more accurate results for differences in bond length and the magnetic coupling constant. This accuracy assists in reconstructing the low-spin ground state force and determining the geometric structure of the ground state. By utilizing the Extended Broken-Symmetry method, we further highlight the significance of the geometric arrangement of metal centers in the cluster's properties and gain deeper insights into the magnetic properties of transition metal iron-sulfur clusters at the reaction centers of hydrogenases. This research illuminates the untapped potential of hydrogenases and their promising role in the future of photosynthesis and sustainable energy production.
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Harvesting wind energy from the environment and integrating it with the internet of things and artificial intelligence to enable intelligent ocean environment monitoring are effective approach. There are some challenges that limit the performance of wind energy harvesters, such as the larger start-up torque and the narrow operational wind speed range. To address these issues, this paper proposes a wind energy harvesting system with a self-regulation strategy based on piezoelectric and electromagnetic effects to achieve state monitoring for unmanned surface vehicles (USVs). The proposed energy harvesting system comprises eight rotation units with centrifugal adaptation and four piezoelectric units with a magnetic coupling mechanism, which can further reduce the start-up torque and expand the wind speed range. The dynamic model of the energy harvester with the centrifugal effect is explored, and the corresponding structural parameters are analyzed. The simulation and experimental results show that it can obtain a maximum average power of 23.25 mW at a wind speed of 8 m/s. Furthermore, three different magnet configurations are investigated, and the optimal configuration can effectively decrease the resistance torque by 91.25% compared with the traditional mode. A prototype is manufactured, and the test result shows that it can charge a 2200 µF supercapacitor to 6.2 V within 120 s, which indicates that it has a great potential to achieve the self-powered low-power sensors. Finally, a deep learning algorithm is applied to detect the stability of the operation, and the average accuracy reached 95.33%, which validates the feasibility of the state monitoring of USVs.
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We reversibly control ferromagnetic-antiferromagnetic ordering in an insulating ground state by annealing tensile-strained LaCoO3 films in hydrogen. This ionic-magnetic coupling occurs due to the hydrogen-driven topotactic transition between perovskite LaCoO3 and brownmillerite La2Co2O5 at a lower temperature (125-200 °C) and within a shorter time (3-10 min) than the oxygen-driven effect (500 °C, tens of hours). The X-ray and optical spectroscopic analyses reveal that the transition results from hydrogen-driven filling of correlated electrons in the Co 3d-orbitals, which successively releases oxygen by destabilizing the CoO6 octahedra into CoO4 tetrahedra. The transition is accelerated by surface exchange, diffusion of hydrogen in and oxygen out through atomically ordered oxygen vacancy "nanocomb" stripes in the tensile-strained LaCoO3 films. Our ionic-magnetic coupling with fast operation, good reproducibility, and long-term stability is a proof-of-principle demonstration of high-performance ultralow power magnetic switching devices for sensors, energy, and artificial intelligence applications, which are keys for attaining carbon neutrality.
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The magnetomechanical actuation of micropillars is developed for the contactless manipulation of miniaturized actuators and microtextured surfaces. Anisotropic geometry of micropillars can significantly enhance the magnetic actuation compared with their isotropic counterparts by directional stress distributions. However, this strategy is not viable for triangular micropillars owing to insufficient anisotropy. In this study, a significant improvement in the magnetic actuation of triangular micropillars using composite magnetic particles is reported. A minute and optimal amount of hard magnetic gamma-ferrite nanorods are hybridized with soft magnetic iron microspheres to generate synergistic effects of magnetic coupling and percolation phenomenon on the magnetic actuation of polymer composites. The addition of 1 wt% face-centered cubic-phased gamma-ferrite nanorods suppresses the magnetic coupling interference of body-centered cubic-phased iron microspheres. Furthermore, the nanorods reduce the percolation threshold by participating in the percolation of the microspheres. A systematic compositional study on the magnetization and magnetorheological properties reveals that the coupling effect dominates the percolation effect at a low magnetic field, whereas the percolation effect governs the magnetic actuation at a high magnetic field. This hybrid approach can help in designing material constituents for effective magnetic actuators and robotic systems that can sensitively respond to an external magnetic field.
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Hierarchical architecture engineering is desirable in integrating the physical-chemical behaviors and macroscopic properties of materials, which present great potential for developing multifunctional microwave absorption materials. However, the intrinsic mechanisms and correlation conditions among cellular units have not been revealed, which are insufficient to maximize the fusion of superior microwave absorption (MA) and derived multifunctionality. Herein, based on three models (disordered structure, porous structure, lamellar structure) of structural units, a range of MXene-aerogels with variable constructions are fabricated by a top-down ice template method. The aerogel with lamellar structure with a density of only 0.015 g cm-3 exhibits the best MA performance (minimum reflection loss: -53.87 dB, effective absorption bandwidth:6.84 GHz) at a 6 wt.% filling ratio, which is preferred over alternative aerogels with variable configurations. This work elucidates the relationship between the hierarchical architecture and the superior MA performance. Further, the MXene/CoNi Composite aerogel with lamellar structure exhibits >90% compression stretch after 1000 cycles, excellent compressive properties, and elasticity, as well as high hydrophobicity and thermal insulation properties, broadening the versatility of MXene-based aerogel applications. In short, through precise microstructure design, this work provides a conceptually novel strategy to realize the integration of electromagnetic stealth, thermal insulation, and load-bearing capability simultaneously.
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Extremely/super low frequency (ELF/SLF) electromagnetic wave can effectively propagate in the harsh cross-medium environment where a high-frequency electromagnetic wave cannot pass due to the fast decay. For efficiently transmitting a strong ELF/SLF radiation signal, the traditional electromagnetic antenna requires a super-large loop (>10 km). To address this issue, in this work, a piezoelectric ceramic/ferromagnetic heterogeneous structured, cantilever beam-type electric-mechano-magnetic coupled resonator at only centimeter scale for ELF/SLF cross-medium magnetic communication is reported. Through designing hard-soft hybrid step-stiffness elastic beam, the resonator exhibits a much higher quality factor Q (≈240) for ELF/SLF magnetic field transmitting, which is one to five orders of magnitude higher than those of previously reported mechanical antennas and loop coil antennas. Moreover, the resonator exhibits a 5000 times higher magnetic field emitting efficiency compared to a conventional loop coil antenna in ELF/SLF band. It also demonstrates a 200% increase in magnetic field emitting capacity compared to existing piezoelectric-driven antennas. In addition, an ASK+PSK modulation method is proposed for suppressing relaxation time of the resonator, and a reduction in the relaxation time by 80% is observed. Furthermore, an air-seawater cross-medium magnetic field communication is successful demonstrated, indicating its potential as portable, high-efficient antenna for underwater and underground communications.
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Metal-organic gel (MOG) derived composites are promising multi-functional materials due to their alterable composition, identifiable chemical homogeneity, tunable shape, and porous structure. Herein, stable metal-organic hydrogels are prepared by regulating the complexation effect, solution polarity and curing speed. Meanwhile, collagen peptide is used to facilitate the fabrication of a porous aerogel with excellent physical properties as well as the homogeneous dispersion of magnetic particles during calcination. Subsequently, two kinds of heterometallic magnetic coupling systems are obtained through the application of Kirkendall effect. FeCo/nitrogen-doped carbon (NC) aerogel demonstrates an ultra-strong microwave absorption of - 85 dB at an ultra-low loading of 5%. After reducing the time taken by atom shifting, a FeCo/Fe3O4/NC aerogel containing virus-shaped particles is obtained, which achieves an ultra-broad absorption of 7.44 GHz at an ultra-thin thickness of 1.59 mm due to the coupling effect offered by dual-soft-magnetic particles. Furthermore, both aerogels show excellent thermal insulation property, and their outstanding radar stealth performances in J-20 aircraft are confirmed by computer simulation technology. The formation mechanism of MOG is also discussed along with the thermal insulation and electromagnetic wave absorption mechanism of the aerogels, which will enable the development and application of novel and lightweight stealth coatings.
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The rational design of absorber size is a promising strategy for obtaining excellent electromagnetic wave (EMW) absorption performance. However, achieving controllable tuning of the material size through simple methods is challenging and the associated EMW attenuation mechanisms are still unclear. In this study, the sizes of metal-organic frameworks (MOFs) are successfully tailored by changing the growth time and the molar ratio of iron (Fe)/organic ligands. The lateral and vertical lengths of MOFs vary in the range of 200 nm to 2 µm and 100 nm to 1 µm, respectively. Both experiments and simulations confirm that the decrease of MOF size favors the formation of more conductive networks, which is beneficial for improving the conductivity loss. Meanwhile, the micromagnetic simulation reveals that the magnetic coupling can be effectively enhanced by the decrease of MOF size, which is conducive to the improvement of magnetic loss, especially in low-frequency range. The reflection loss of Fe-based MOFs with optimized size reaches -46.4 dB at 6.2 GHz with an effective absorption bandwidth of 3.1 GHz. This work illustrates the important role of size effect in EMW dissipation and provides an effective strategy for enhancing the low-frequency EMW absorption performance.
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The energy of rotating machinery exists widely in the environment. It is of great significance to collect and utilize the energy of rotating machinery for sustainable development. In this paper, a novel piezoelectric and electromagnetic energy harvester, which is capable of generating electrical energy under rotary excitation, is proposed based on array magnetic coupling. The working principle of this kind of energy harvester is analyzed. And the energy output modeling of the harvester is developed and output results are simulated. Based on the experimental test platform built in the laboratory, the output characteristics of the piezoelectric and electromagnetic energy harvester are tested. Results show that the maximum output power of the proposed energy harvester reaches 182 mW when the excitation speed is 120 rpm. Furthermore, both the piezoelectric module and the electromagnetic module can reach the maximum output power at the excitation speed of 120 rpm.
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In order to solve the problem of the quantification of detection signals in the magnetic flux leakage (MFL) of defective in-service oil and gas pipelines, a non-uniform magnetic charge model was established based on magnetic effects. The distribution patterns of magnetic charges under different stresses were analyzed. The influences of the elastic load and plastic deformation on the characteristic values of MFL signals were quantitatively assessed. The experimental results showed that the magnetic charge density was large at the edges of the defect and small at the center, and approximately decreased linearly with increasing stress. The eigenvalues of the axial and radial components of the MFL signals were compared, and it was found that the eigenvalues of the radial component exhibited a larger decline rate and were more sensitive to stress. With the increase in the plastic deformation, the characteristic values of the MFL signals initially decreased and then increased, and there was an inflection point. The location of the inflection point was associated with the magnetostriction coefficient. Compared with the uniform magnetic charge model, the accuracy of the axial and radial components of the MFL signals in the elastic stage of the improved magnetic charge model rose by 17% and 16%, respectively. The accuracy of the axial and radial components of the MFL signals were elevated by 9.15% and 9%, respectively, in the plastic stage.
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Piezoelectric vibration energy harvester (PVEH) is a promising device for sustainable power supply of wireless sensor nodes (WSNs). PVEH is resonant and generates power under constant frequency vibration excitation of mechanical equipment. However, it cannot output high power through off-resonance if it has frequency offset in manufacturing, assembly and use. To address this issue, this paper designs and optimizes a PVEH to harvest power specifically from grid transformer vibration at 100 Hz with high power density of 5.28 µWmm-3g-2. Some resonant frequency modulation methods of PVEH are discussed by theoretical analysis and experiment, such as load impedance, additional mass, glue filling, axial and transverse magnetic force frequency modulation. Finally, efficient energy harvesting of 6.1 V output in 0.0226 g acceleration is tested in grid transformer reactor field application. This research has practical value for the design and optimization process of tunable PVEH for a specific vibration source.