Fixed-Point Atomic Regulation Engineered Low-Thickness Wideband Microwave Absorption.

Atomic doping is widely employed to fine-tune crystal structures, energy band structures, and the corresponding electrical properties. However, due to the difficulty in precisely regulating doping sites and concentrations, establishing a relationship between electricity properties and doping becomes a huge challenge. In this work, a modulation strategy on A-site cation dopant into spinel-phase metal sulfide Co9S8 lattice via Fe and Ni elements is developed to improve the microwave absorption (MA) properties. At the atomic scale, accurately controlling doped sites can introduce local lattice distortions and strain concentration. Tunned electron energy redistribution of the doped Co9S8 strengthens electron interactions, ultimately enhancing the high-frequency dielectric polarization (ɛ' from 10.5 to 12.5 at 12 GHz). For the Fe-doped Co9S8, the effective absorption bandwidth (EAB) at 1.7 mm increases by 5%, and the minimum reflection loss (RLmin) improves by 26% (EAB = 5.8 GHz, RLmin = -46 dB). The methodology of atomic-scale fixed-point doping presents a promising avenue for customizing the dielectric properties of nanomaterials, imparting invaluable insights for the design of cutting-edge high-performance microwave absorption materials.

In Situ Constructed Spinel Layer Stabilized Upcycled LiCoO2 for High Performance Lithium-Ion Batteries.

With ever-increasing requirements for cathodes in the lithium-ion batteries market, an efficiency and eco-friendly upcycling regeneration strategy is imperative to meet the demand for high-performance cathode materials. Herein, a facile, direct and upcycling regeneration strategy is proposed to restore the failed LiCoO2 and enhance the stability at 4.6 V. Double effects combination of relithiation and outside surface reconstruction are simultaneously achieved via a facile solid-phase sintering method. The evolution process of the Li-supplement and grain-recrystallization is systematically investigated, and the high performance of the upcycled materials at high voltage is comprehensively demonstrated. Thanks to the favorable spinel LiCoxMn2-xO4 surface coating, the upcycled sample displays outstanding electrochemical performance, superior to the pristine cathode materials. Notably, the 1% surface-coated LiCoO2 achieves a high discharge-specific capacity of 207.9 mA h g-1 at 0.1 C and delivers excellent cyclability with 77.0% capacity retention after 300 cycles. Significantly, this in situ created spinel coating layer can be potentially utilized for recycling spent LiCoO2, thus providing a viable, promising recycling strategy insights into the upcycling of degraded cathodes.

Distinct skyrmion phases at room temperature in two-dimensional ferromagnet Fe3GaTe2.

Distinct skyrmion phases at room temperature hosted by one material offer additional degree of freedom for the design of topology-based compact and energetically-efficient spintronic devices. The field has been extended to low-dimensional magnets with the discovery of magnetism in two-dimensional van der Waals magnets. However, creating multiple skyrmion phases in 2D magnets, especially above room temperature, remains a major challenge. Here, we report the experimental observation of mixed-type skyrmions, exhibiting both Bloch and hybrid characteristics, in a room-temperature ferromagnet Fe3GaTe2. Analysis of the magnetic intensities under varied imaging conditions coupled with complementary simulations reveal that spontaneous Bloch skyrmions exist as the magnetic ground state with the coexistence of hybrid stripes domain, on account of the interplay between the dipolar interaction and the Dzyaloshinskii-Moriya interaction. Moreover, hybrid skyrmions are created and their coexisting phases with Bloch skyrmions exhibit considerably high thermostability, enduring up to 328 K. The findings open perspectives for 2D spintronic devices incorporating distinct skyrmion phases at room temperature.

Construction of Selective Ion Transport Polymer at Anode-Electrolyte Interface for Stable Aqueous Zinc-Ion Batteries.

Rampant dendrite formation and serious adverse parasitic reactions induced by migration of dissolved V/Mn cathode ions on Zn anode have hampered the high performance of aqueous zinc-ion batteries (AZIBs). Inspired by the coordination chemistry between functional groups of polymer and electrolyte ions, a freestanding layer consisting of dopamine-functionalized polypyrrole (DA-PPy) nanowires served as a selective ion transport layer at the anode-electrolyte interface to address these two issues, which could simultaneously avoid polarization caused by the introduction of an additional interface. On the one hand, the DA-PPy layer displays excellent zinc ion and charge transfer ability, as well as provides chemical homochanneling for zinc ions at the interface, which endow the DA-PPy layer with properties as a chemical guider and physical barrier for dendrite inhibition. On the other hand, the DA-PPy layer can trap excess transition metal ions fleeing from the cathodes, thus serving as a chemical barrier, preventing the formation of Vx+/Mnx+-passivation on the surface of the zinc anode. Consequently, the AZIBs based on V2O5 and MnO2 cathodes involving the DA-PPy functional layer show a great improvement in the capacity retention.

Cocatalyst Modified Polymeric Carbon Nitride Photoanode for Enhanced Photoelectrochemical Properties.

As a new organic photocatalyst, polymeric carbon nitride (CN) has shown good application potential in the field of photoelectrochemistry due to its unique physical and chemical properties, but its application has been seriously hindered due to its inherent characteristics such as the difficulty in charge separation. In this study, FeOOH modified CN photoanode (CN-Fe) was constructed to investigate the effect of the cocatalyst on the charge injection capacity of organic semiconductor photoelectrodes. The experimental results demonstrate significant improvement in the charge injection efficiency of the photoanode due to the introduction of FeOOH cocatalyst, leading to enhanced photoelectrochemical performance with approximately 2.4 times increase in photocurrent density. By thoroughly investigating the mechanism behind the loading of FeOOH on the polymeric carbon nitride photoanode, we gained profound insights into the behavior of charge carriers and reaction kinetics during the photoelectrocatalytic process.

Utilizing procalcitonin, C-reactive protein, and serum amyloid A in combination for diagnosing sepsis due to urinary tract infection.

OBJECTIVE: In this study, we aimed to evaluate the combined diagnostic value of procalcitonin (PCT), C-reactive protein (CRP), and serum amyloid A (SAA) in sepsis caused by urinary tract infection. METHOD: A total of 80 patients with urosepsis who were hospitalized were included in the study group, and 80 patients with urinary tract infection without sepsis were included in the control group. We collected the PCT, SAA, and CRP levels of patients following admission. Subsequently, we conducted a comparative analysis to assess the specificity, accuracy, and sensitivity of combined diagnostic approaches in contrast to individual diagnostic methods for blood PCT, SAA, and CRP. RESULTS: The levels of PCT, SAA, and CRP in the study group were significantly higher than those in the control group, and the differences were statistically significant (P < 0.01). Multi-factor logistic regression analysis revealed that the levels of PCT (P = 0.003) and SAA (P = 0.014) were associated with urosepsis. The sensitivity of PCT was 87.133% and the specificity was 93.066%, which were higher than that of SAA and CRP. The specificity of the combined detection of the three was 95.670%, which was higher than that of PCT, SAA, and CRP alone. Correlation analysis revealed that PCT had a significant positive correlation with CRP and SAA (P < 0.01), and a weak correlation with white blood cell count (WBC) and fibrinogen (FIB) (P = 0.03 for WBC, P = 0.04 for FIB). CONCLUSION: PCT, SAA, and CRP indicators in patients with urosepsis are significantly elevated, and all three are valuable in the diagnosis of urosepsis. PCT alone has good diagnostic efficiency for urosepsis, and a certain correlation with other inflammatory factors. The diagnostic efficacy of the three indicators in combination is better than that of any one of the three, and is worthy of widespread clinical application.

Controllable Synthesis of Highly Symmetrical Streamlined Structure for Wideband Microwave Absorption.

Highly symmetrical and streamlined nanostructures possessing unique electron scattering, electron-phonon coupling, and electron confinement characteristics have attracted a lot of attention. However, the controllable synthesis of such a nanostructure with regulated shapes and sizes remains a huge challenge. In this work, a peanut-like MnO@C structure, assembled by two core-shell nanosphere is developed via a facile hydrogen ion concentration regulation strategy. Off-axis electron holography technique, charge reconstruction, and COMSOL Multiphysics simulation jointly reveal the unique electronic distribution and confirm its higher dielectric sensitive ability, which can be used as microwave absorption to deal with currently electromagnetic pollution. The results reveal that the peanut-like core-shell MnO@C exhibits great wideband properties with effective absorption bandwidth of 6.6 GHz, covering 10.8-17.2 GHz band. Inspired by this structure-induced sensitively dielectric behavior, promoting the development of symmetrical and streamlined nanostructure would be attractive for many other promising applications in the future, such as piezoelectric material and supercapacitor and electromagnetic shielding.

Hierarchical Fe-Co@TiO2 with Incoherent Heterointerfaces and Gradient Magnetic Domains for Electromagnetic Wave Absorption.

Induced polarization response and integrated magnetic resonance show prosperous advantages in boosting electromagnetic wave absorption but still face huge challenges in revealing the intrinsic mechanism. In this work, we propose a self-confined strategy to construct hierarchical Fe-Co@TiO2 microrods with numerous incoherent heterointerfaces and gradient magnetic domains. The results demonstrate that the use of polyvinylpyrrolidone (PVP) coating is crucial for the subsequent deposition of Co-zeolitic imidazolate frameworks (ZIF-67), the distance of ordered arranged metal ions manipulates the size of magnetic domains, and the pyrolysis of PVP layers restricts the eutectic process of Fe-Co alloys to some extent. As a result, these introduced lattice defects, oxygen vacancies, and incoherent heterointerfaces inevitably generate a strong polarization response, and the regulated gradient magnetic domains realize integrated magnetic resonance, including macroscopic magnetic coupling, long-range magnetic diffraction, and nanoscale magnetic bridge connection, and both of the intrinsic mechanisms in dissipating electromagnetic energy are quantitatively clarified by Lorentz off-axis electron holography. Owing to the cooperative merits, the Fe-Co@TiO2 absorbents exhibit enhanced absorption intensity and strong absorption bandwidth. This study inspires us to develop a generalized strategy for manipulating the size of magnetic domains, and the integrated magnetic resonance theory provides a versatile methodology in clarifying magnetic loss mechanism.

High-performance aqueous rechargeable NiCo//Zn battery with molybdate anion intercalated CoNi-LDH@CP bilayered cathode.

Seeking cathode materials with high areal capacity and excellent cycling tolerance is a key step to develop aqueous rechargeable zinc-based alkaline batteries with high energy density, power density and excellent stability. Here, the bilayered cathode composite (MCN-LDH@CP) of molybdate intercalated cobalt-nickel layered hydroxide nanosheets (MCN-LDH) grown on cobalt phosphate octahydrate microsheet (CP) was prepared by a two-step hydrothermal process. Molybdate intercalation significantly reduces the thickness of cobalt-nickel layered hydroxide, greatly increases its specific surface area, regulates its pore distribution, increases the crystal plane spacing, promotes the diffusion rate of hydroxide in it, and increases its specific capacity. Meanwhile, the bilayered MCN-LDH@CP electrode significantly improved the areal energy density (2.89 mWh/cm2) and peak power density (111.22 mW/cm2) and cycle stability (97.8 % after 7000 cycles) of the CoNi//Zn battery. The excellent stability is mainly due to the fact that the MCN-LDH overlay inhibits the loss of P element of CP and improves the structural stability of the sample. The quasi-solid-state MCN-LDH@CP//Zn battery can still charge a mobile phone even when hammered and pierced, showing excellent safety and reliability. This work opens a new avenue to develop CoNi//Zn batteries with high energy density, power density and excellent tolerance.

Skin-adhesive lignin-grafted-polyacrylamide/hydroxypropyl cellulose hydrogel sensor for real-time cervical spine bending monitoring in human-machine Interface.

Developing a straightforward method to produce conductive hydrogels with excellent mechanical properties, self-adhesion, and biocompatibility remains a significant challenge. While current approaches aim to enhance mechanical performance, they often require additional steps or external forces for fixation, leading to increased production time and limited practicality. A novel lignin-grafted polyacrylamide/hydroxypropyl cellulose hydrogel (L-g-PAM/HPC hydrogel) with a semi-interpenetrating polymer network structure had been developed in this research that boasted exceptional adhesion to the skin (∼68 kPa) and stretchability properties (∼1637 %) compared to PAM-based hydrogels. By incorporating conductive additives such as silver nanowires and carbon nanocages to construct a bridge-like structure within the hydrogel matrix, the resulting AgC@L-g-PAM/HPC hydrogel exhibited impressive electrical conductivity, surpassing that of other PAM-based hydrogels relying on MXene, with a maximum value of 0.76 S/m. Furthermore, the AgC@L-g-PAM/HPC hydrogel retained its efficient electrical signal transmission capability even under mechanical stress. These make it an ideal flexible strain sensor capable of detecting various human motions. In this study, a smart real-time monitoring system was successfully developed for tracking cervical spine bending, serving as an extension for monitoring human activities.

Mechanisms of magnetic sensing and regulating extracellular electron transfer of electroactive bacteria under magnetic fields.

Electroactive bacteria can display notable plasticity in their response to magnetic field (MF), which prompted bioelectrochemical system as promising candidates for magnetic sensor applications. In this study, we explored the sensing and stimulatory effect of MF on current generation by Geobacter sulfurreducens, and elucidated the related molecular mechanism at the transcriptomic level. MF treatment significantly enhanced electricity generation and overall energy efficiency of G. sulfurreducens by 50 % and 22 %, respectively. The response of current to MFs was instantaneous and reversible. Cyclic voltammetry analysis of the anode biofilm revealed that the redox couples changed from -0.31 to -0.39 V (vs. Ag/AgCl), suggesting that MFs could alter electron transfer related components. Differential gene expression analysis further verified this hypothesis, genes associated with electron transfer were upregulated in G. sulfurreducens under MF treatment relative to the control group, specifically, genes encoding periplasmic c-type cytochromes (ppcA and ppcD), outer membrane cytochrome (omcF, omcZ, omcB), pili (pilA-C, pilM, and pilV2), and ribosome. The enhanced bacterial extracellular electron transfer process was also linked to the overexpression of the NADH dehydrogenase I subunit, the ABC transporter, transcriptional regulation, and ATP synthase. Overall, our findings shed light on the molecular mechanism underlying the effects of magnetic field stimuli on EAB and provide a theoretical basis for its further application in magnetic sensors and other biological system.

Electrochemical Aging Protocol Governed Capacity Losses and Structure Degradations in Layered LiNi0.8 Co0.1 Mn0.1 O2 Oxides.

The comparatively poor endurance of Ni-rich cathode materials restricts their application in high-energy lithium-ion batteries. A thorough understanding of the degradation characteristics of such materials under complex electrochemical aging protocols is required to further improve their reliability. In this work, the irreversible capacity losses of LiNi0.8 Mn0.1 Co0.1 O2 under different electrochemical aging protocols are quantitatively evaluated via a well-designed experiment. In addition, it is discovered that the origin of irreversible capacity losses is highly related to electrochemical cycling parameters and can be divided into two types. Type I is heterogeneous degradation caused by low C-rate or high upper cut-off voltage cycling and features abundant capacity loss during H2-H3 phase transition. Such capacity loss is attributed to the irreversible surface phase transition that limits the accessible state of charge during the H2-H3 phase transition stage via the pinning effect. Type II is fast charging/discharging induced homogeneous capacity loss that occurs consistently throughout the whole phase transition time. This degradation pathway shows a distinctive surface crystal structure, which is dominated by a bending layered structure rather than a typical rock-salt phase structure. This work offers detailed insight into the failure mechanism of Ni-rich cathodes and provides guidance on designing long-cycle life, high-reliability electrode materials.

Developing Superior Hydrophobic 3D Hierarchical Electrocatalysts Embedding Abundant Catalytic Species for High Power Density Zn-Air Battery.

It is essential but still challenging to design and construct inexpensive, highly active bifunctional oxygen electrocatalysts for the development of high power density zinc-air batteries (ZABs). Herein, a CoFe-S@3D-S-NCNT electrocatalyst with a 3D hierarchical structure of carbon nanotubes growing on leaf-like carbon microplates is designed and prepared through chemical vapour deposition pyrolysis of CoFe-MOF and subsequent hydrothermal sulfurization. Its 3D hierarchical structure shows excellent hydrophobicity, which facilitates the diffusion of oxygen and thus accelerates the oxygen reduction reaction (ORR) kinetic process. Alloying and sulfurization strategies obviously enrich the catalytic species in the catalyst, including cobalt or cobalt ferroalloy sulfides, their heterojunction, core-shell structure, and S, N-doped carbon, which simultaneously improve the ORR/OER catalytic activity with a small potential gap (ΔE = 0.71 V). Benefiting from these characteristics, the corresponding liquid ZABs show high peak power density (223 mW cm-2 ), superior specific capacity (815 mA h gZn -1 ), and excellent stability at 5 mA cm-2 for ≈900 h. The quasi-solid-state ZABs also exhibit a very high peak power density of 490 mW cm-2 and an excellent voltage round-trip efficiency of more than 64%. This work highlights that simultaneous composition optimization and microstructure design of catalysts can effectively improve the performance of ZABs.

Responsive Ag@NiCo2O4 Nanowires Anchored on N-Doped Carbon Cloth as Array Electrodes for Nonenzymatic Glucose Sensing.

The development of responsive materials in a predictable manner is high on the list of the material industry's trends. In this work, responsive Ag@NiCo2O4 nanowires were, firstly, anchored on N-doped carbon cloth (NC) and, then, employed as array electrodes for a nonenzymatic glucose-sensing application. The results showed that the highly conductive NiCo2O4 nanowires supported Ag nanoparticles and exhibited high conductivity and electrocatalytic properties. The fully exposed crystalline planes of Ag nanoparticles provided more active surface sites. As a result, the assembled Ag@NiCo2O4-NC electrodes for the glucose-sensing evaluation delivered a selectivity of 2803 µA mM-1 cm-2 and a detection limit of 1.065 µM, which outperformed the literature-reported Ag- and NiCo2O4-based glucose-sensing catalysts.

Tailoring the Hollow Structure within CoSn(OH)6 Nanocubes for Advanced Supercapacitors.

The enhanced application performance of hollow-structured materials is attributed to their large surface area with more active sites. In this work, the hollow CoSn(OH)6 nanocubes with increased surface area and mesopores were derived from dense CoSn(OH)6 nanocube precursors by alkaline etching. As a result, the hollow CoSn(OH)6 nanocubes-based cathode electrode exhibited a higher area-specific capacitance of 85.56 µF cm-2 at 0.5 mA cm-2 and a mass-specific capacitance of 5.35 mF g-1 at 0.5 mA cm-2, which was more extensive than that of the dense precursor. Meanwhile, the current density was increased 4-fold with good rate capability for hollow CoSn(OH)6 nanocubes.

Controllable Topological Magnetic Transformations in the Thickness-Tunable van der Waals Ferromagnet Fe5GeTe2.

Recent observations of topological meron textures in two-dimensional (2D) van der Waals (vdW) magnetic materials have attracted considerable research interest for both fundamental physics and spintronic applications. However, manipulating the meron textures and realizing the topological transformations, which allow for exploring emergent electromagnetic behaviors, remain largely unexplored in 2D magnets. In this work, utilizing real-space imaging and micromagnetic simulations, we reveal temperature- and thickness-dependent topological magnetic transformations among domain walls, meron textures, and stripe domain in Fe5GeTe2 (FGT) lamellae. The key mechanism of the magnetic transformations can be attributed to the temperature-induced change of exchange stiffness constant within layers and uniaxial magnetic anisotropy, while the magnetic dipole interaction as governed by sample thickness is crucial to affect the critical transformation temperature and stripe period. Our findings provide reliable insights into the origin and manipulation of topological spin textures in 2D vdW ferromagnets.

Magnetic-Field-Assisted Diffusion Motion of Magnetic Skyrmions.

Studies of the diffusion dynamics of magnetic skyrmions have generated widespread interest in both fundamental physics and spintronics applications. Here we report the magnetic-field-assisted diffusion motion of skyrmions in a microstructured chiral FeGe magnet. We demonstrate the enhancement of diffusion motion of magnetic skyrmions that is manipulated and driven by an oscillatory magnetic field. Further, the directed diffusion of skyrmions is observed when an in-plane field was introduced to break the symmetry of the system. Finally, we demonstrate the application of a magnetic field can induce an arrangements transition of skyrmions assemble in microstructure, that is, from a stiff hexagonal lattice to a weak interactional isotropic state. By using a step-ascended magnetic field we finished the observation of a particle-like diffusive motion for magnetic skyrmions that transport from high-concentration regions to low-concentration regions and the diffusion flux is proportional to the concentration gradient followed Fick's law.

Achieving Sustainable and Stable Potassium-Ion Batteries by Leaf-Bioinspired Nanofluidic Flow.

In nature, living systems have evolved integrated structures, matching optimized nanofluidics to adapt to external conditions. In rechargeable batteries, high-capacity electrodes are often plagued by the crucial and universal bottleneck of dissolution and shuttle of active substance into electrolyte, posing obstacles of inevitable capacity degradation. Introducing the concept of intelligent nanofluidics to electrodes, a leaf-bioinspired electrode configuration with hierarchical architecture to tackle this problem is proposed. This integrated structure with fine-tuned surface pores and unobstructed interior porous media, can spatially control the anisotropic nanofluidic flux, in an efficient and self-protectable way: tailoring the outflow across the electrode's surface and free transport in interior, to ensure speedy and stable energy conversion. As proofs of concept, applications of sustainable electrodes rejuvenated from fallen leaf and spent commercial batteries, are designed with leaf-bioinspired architecture. Both KCoS2 and KS battery systems show advanced steady cycling with effectively mitigated shuttle issues in this smart architecture (0.15% and 0.21% capacity decay per cycle), even at high areal mass loading, when compared with open porous structure (0.60% and 0.39%). This work may pave a new way from a biomimetic view to integrated electrode engineering with regulated surface shielding to conquer the universal dissolution-shuttle problems facing high-capacity materials.

Effect of a Cocatalyst on a Photoanode in Water Splitting: A Study of Scanning Electrochemical Microscopy.

With a proper band gap of ∼2.4 eV for solar light absorption and suitable valence band edge position for oxygen evolution, scheelite-monoclinic bismuth vanadate (BiVO4) has become one of the most attractive photocatalysts for efficient visible-light-driven photoelectrochemical (PEC) water splitting. Several studies have indicated that surface modification of BiVO4 with a cocatalyst such as NiFe layered double hydroxide (LDH) can significantly increase the PEC water splitting performance of the catalyst. Herein, we experimentally investigated the charge transfer dynamics and charge carrier recombination processes by scanning electrochemical microscopy (SECM) with the feedback mode on the surface of BiVO4 and BiVO4/NiFe-LDH as model samples. The ratio of rate constants for photogenerated hole (kh+0) to electron (ke-0) via the photocatalyst of BiVO4/NiFe-LDH reacting with the redox couple is found to be five times larger than that of BiVO4 under illumination. In this case, the ratio of the rate constants kh+0/ke-0 stands for the interfacial charge recombination process. This implies the cocatalyst NiFe-LDH suppresses the electron back transfer greatly and finally reduces the surface recombination. Control experiments with cocatalysts CoPi and RuOx onto BiVO4 further verify this conclusion. Therefore, the SECM characterization allows us to make an overall analysis on the function of cocatalysts in the PEC water splitting system.

Synthesis of Ni3Bi2S2 Coupled with N-Doped Carbon Sheets as Electrocatalyst for Triiodide and Oxygen Reduction.

Herein, we report a novel composite structure consisting of Ni3Bi2S2 particles coupled with N-doped carbon (NC) sheets. Different from the generally used high vacuum or microwave-assisted technologies, metal-rich Ni3Bi2S2 can be successfully synthesized via a simple pyrolysis procedure, with NC employed as a reducing agent. In addition, the phase purity, size, and dispersity of the Ni3Bi2S2 particles, which were encapsulated by the NC shell, were modulated by the content of NC. The X-ray photoelectron spectroscopy (XPS) analysis demonstrated the metallic state of the Ni and Bi elements, which ensured good Ni3Bi2S2 electrical conductivity. As a result, the resultant Ni3Bi2S2/NC (0.55 II) catalyzed triiodide reduction with a lower charge transfer resistance than commercial Pt/C (1.4 II). Moreover, Ni3Bi2S2/NC catalyzed the oxygen reduction reaction with a positive ORR half-wave potential (0.81 V vs. RHE) and a low Tafel slope (47 mV dec-1). Our study thus provides the novel exploration of the electrochemical performance of Ni3Bi2S2 and indicates its promising application in electrocatalytic reactions.