The rational design of photocatalysts for stable and efficient seawater splitting remains a formidable challenge. Leveraging ionic components of seawater can regulate the electrostatic microenvironment efficiently for boosting photocatalytic activity. Taking graphitic carbon nitride (CN) as the model, three electron mediators (EMs) with different electrostatic characteristics were incorporated. Among them, the charged-EM functionalized CN-1% BPD exhibits the best H2-evolution performance, which increases from 493 to 4637.78 mu mol g- 1 h- 1 after altering freshwater to seawater. A unique electrostatic sieving phenomenon was recorded, where major seawater anions all contribute positively to seawater-splitting performance. Characterization and theoretical calculations reveal that the positively charged-EM skeleton optimizes the electron distribution of the photocatalyst, while the predominant anions in seawater further increase the dipole moment, thereby facilitating directional photogenerated carrier migration. Moreover, the derived CNBPD@EEA membrane also exhibits satisfactory H2-evolution activity, whether in freshwater (25.53 mmol m- 2) or seawater (27.46 mmol m- 2).
Intracerebral hemorrhage (ICH) is a lethal stroke subtype with limited treatment options, largely due to secondary injury driven by oxidative stress and neuroinflammation. Here, we developed a ruthenium (Ru)-manganese (Mn) composite nanozyme by integrating Ru nanozyme into Mn-doped zeolitic imidazolate framework (Mn-ZIF) to enable cascade catalytic activity for efficient ROS clearance. In vitro, Ru@Mn-ZIF nanozyme reduced LPS-induced microglia activation and H2O2-induced neuronal oxidative damage, showing stronger protective effects than Mn-ZIF nanozyme. In vivo, both intranasal and intravenous administration of Ru@Mn-ZIF nanozyme significantly decreased hematoma volume, preserved blood-brain barrier integrity, suppressed inflammatory responses, and improved neurological recovery in collagenase- and autologous blood-induced ICH models. Biosafety evaluation revealed no pathological or biochemical abnormalities after treatment. These findings highlight Ru@Mn-ZIF nanozyme as a promising therapeutic strategy for mitigating secondary brain injury and improving outcomes after ICH.
Two-dimensional materials have garnered significant attention in recent years due to their remarkable electronhole transfer capability. However, the advancement of convenient and rapid synthesis techniques remains crucial for further research in this field. In this study, lamellar anatase/rutile-TiO2 phase heterojunctions with a favorable phase interface was synthesized through a fast annealing route using glucose as the template and titanium tetrachloride. The sample synthesized at 600 degrees C with a holding time of 20 min exhibited the most significant levels of H2 evolution activity (53.22 mmol g- 1 h-1) with a low loading of 0.05 wt% Pt co-catalyst, which is significantly higher than the commercial P25 sample. The characterization reveals that the anatase/ rutile-TiO2 phase heterojunction in the two-dimensional sheet exhibits excellent phase interface contact and possesses a large specific surface area with an appropriate pore size. These characteristics are advantageous for facilitating the separation and migration of carriers, thereby enhancing the efficiency of the H2 production reaction through hydrolysis. This study presents a novel approach towards the advancement of highly effective two-dimensional photocatalysts.
As a novel type of battery for energy devices, Li-CO2 batteries have a slow kinetic reaction during carbon dioxide reduction and evolution, which leads to problems such as high battery polarization potential, poor cycling performance, and a short lifetime. Therefore, it is important to explore electrocatalysts with high activity and stability. In this study, a novel high-loaded single-atom catalyst was prepared by uniformly anchoring single-atom Ni/Co on N-doped carbon (NiNC/CoNC). Compared with previous reports, the doping amount of Ni is as high as 10 wt%. The Li-CO2 battery assembled using NiNC achieves a high discharge capacity of 51,125 mAh g-1 at 100 mA g-1 current density and displays a low overpotential of 1.63 V after 268 stable cycles (more than 2600 h) at 200 mA g-1 current density. The X-ray absorption fine structure analysis of NiNC reveals the presence of Ni and NiN4 sites. Combined with density functional theory calculations, it is found that NiNC adsorbs CO2 reactive species more strongly. Moreover, the electronic synergism of the NiN4 sites can weaken the decomposition barrier of the discharge product Li2CO3 and accelerate the reaction kinetic process, thereby enhancing the electrocatalytic activities of CO2 electroreduction and CO2 reduction reaction.
CaBi2Nb2O9 (CBN) piezoceramics have been extensively studied due to their high Curie temperature, which enables them to maintain functionality at elevated temperatures. However, achieving both high piezoelectric performance and resistivity at temperatures exceeding 500 °C remains a critical challenge. Through Li/Ce co-doping and grain engineering, we have synthesized Ca0.88(Li0.5Ce0.5)0.12Bi2Nb2O9 ceramic, which exhibits optimal performance with a piezoelectric coefficient d33 of 17.0 pC/N, a very high Curie temperature of 921 °C, and a high-temperature resistivity of 1.2 × 106 Ω cm at 550 °C. Microstructural analysis reveals that grain refinement plays a pivotal role in optimizing the properties of the CBN piezoceramics.
Solid polymer electrolytes are promising for lithium metal batteries, yet achieving both high ionic conductivity and interfacial stability remains a major challenge. Here, we report a molecular rotor strategy that addresses this trade-off by incorporating 3-(1-Pyridinio)-1-propanesulfonate zwitterions (PP-Z) into a polyvinylidene difluoride electrolyte. This design establishes a dipole-rotation-assisted ion transport mechanism distinct from conventional polymer relaxation-dependent conduction. Molecular dynamics simulations and experiments reveal that the anchored cationic group of PP-Z serves as a pivot, while the mobile anionic end creates a dynamic coulombic field. This configuration facilitates rapid Li+ migration through coordinated intrachain transport and interchain hopping, significantly enhancing ionic conductivity (5.1 × 10-4 S cm-1 at 25°C and 1.5 × 10-4 S cm-1 at 0°C) and the Li+ transference number (0.52). The anionic terminals further participate in Li+ solvation and promote formation of a LiF-rich solid electrolyte interphase, enabling stable cycling for 1200 h in Li||Li cells at 0.3 mA cm-2 and > 500 cycles in Li||LiFePO4 cells at 1C (25°C). Even at 0°C, the Li||LiNi0.8Co0.1Mn0.1O2 (1.8 mAh cm-2) pouch cell retains 85.1% capacity over 50 cycles while delivering 78.3% of its room-temperature capacity initially.
Conventional planar copper (Cu) current collectors severely limit the rate capability and cycle life of lithium-ion batteries. To overcome this, we report a three-dimensional (3D) porous Cu-Sn alloy architecture fabricated via scalable, cyanide-free electrodeposition and chemical dealloying methods. Its core innovation lies in the synergistic benefits of the porous structure and Cu-Sn alloying: the interconnected pores facilitate rapid Li. transport and buffer graphite's volume expansion, while the intrinsic lithiophilicity of Sn ensures a stable, low-impedance interface. Consequently, an anode using the optimized porous collector delivers a remarkable specific capacity of 120.3 mAh g.(1) at 5C, representing a nearly five-fold enhancement in high-rate capacity retention over conventional Cu foil. The collector also confers exceptional cycling stability, enabling a 57.2 % capacity increase over 200 cycles, in stark contrast to the decay observed with standard foil. Electrochemical analysis confirms that the porous design drastically reduces electrode impedance while maintaining structural integrity. This work validates that engineering the current collector architecture is a powerful and effective strategy for developing high-performance, fast-charging batteries.
With the development of high-frequency integration of electronic devices, electromagnetic wave-absorbing materials should possess excellent absorbing properties, as well as good thermal conductivity and flame retardancy, to meet the requirements of practical applications. A novel poplar catkin-like short rod-shaped boron nitride/carbon (BNC) heterostructured filler was fabricated via a facile strategy using hexagonal boron nitride (h-BN) and aramid nanofibers (ANFs), and incorporated into epoxy resin (EP) matrix to develop multifunctional composites with integrated microwave absorption, thermal conductivity and flame retardancy. The BNC-2/EP composite with optimal carbon content exhibited the best microwave absorption performance at 50 wt% filler loading, achieving a minimum reflection loss (RLmin) of −53.4 dB and a maximum effective absorption bandwidth (EABmax) of 6.0 GHz at a thickness of 2.0 mm. The superior performance is attributed to the synergistic effects of conduction loss, interfacial polarization, dipole/defect polarization, and multiple reflections/scattering induced by the unique short rod-shaped architecture. Meanwhile, compared with neat EP, the thermal conductivity of BNC-2/EP was enhanced by 737%, while the peak heat release rate (PHRR) and total heat release (THR) were reduced by 40.06% and 38.96%, respectively. This work provides a referable and facile structural design strategy for tuning the electromagnetic wave absorption performance of carbon-based composite materials.
The supercapacitors with conductive cement as electrodes exhibit a great charm of massive energy storage. Improvement in the charge capacity and transferring efficiency is required for its infrastructure applications. This paper investigates the capacitance and coulombic efficiency of carbon cement supercapacitors as functions of cement hydration, large-volume preparation, and carbon black types, with the aim of carbon cement electrode optimization. The correlation between capacitance and coulombic efficiency is weak, and they are sensitive to the exposed surface area of carbon black in cement-based electrodes and electrode resistance, respectively. These two performances are highly microstructure-dependent and can be weakened by the wrapping of carbon black particles by cement hydrates. An increase in electrode area can significantly improve both the capacitance and coulombic efficiency, while electrode thickness increment can only rise the capatitance. It opens up a way for independent design of charge capacity and transferring losses of carbon cement supercapacitor.
The development of an efficient photocatalyst to remove pollutants from wastewater is pivotal to solving the problem of environmental pollution. This study reports a Z-scheme heterojunction between oxygen-doped carbon nitride (OCN) and MgIn2S4 (MIS), which can exhibit excellent photocatalytic ability on both reduction of U (VI) and oxidation of methyl orange (MO) without sacrificial agents. The internal structure of OCN/MIS can be effectively adjusted by changing the amount of MIS, leading to an enhancement of the separation rate of carriers and the inhibition of the photocorrosion for MgIn2S4. The reaction rate constants of U(VI) reduction and MO degradation by the optimized MIS2.5/OCN were 56 and 8 times higher than those of OCN and 3 times and twice higher than those of MIS, respectively. This study provides a novel approach for constructing graphitic carbon nitride-based Z-scheme heterojunction photocatalysts to deal with environmental pollution problem without sacrificial agents.
The main challenge for electrocatalytic CO2 reduction reaction (CO2RR) remains the limited CO2 mass transport, especially under high current density. Designing an electrocatalyst that can enrich CO2 concentration is an effective strategy to improve CO2RR. Herein, we designed an efficient Ag-based electrocatalyst modified by ApmimBr ionic liquid (Ag-ApmimBr/KB) via a simple hydrothermal and in situ electroreduction approach, aiming to simultaneously tailor its structural and regulate the reaction microenvironment. The optimal Ag1.0-ApmimBr1.5/KB electrocatalyst exhibits excellent catalytic activity, selectivity, and stability in flow cell, achieving a CO Faradaic efficiency (FECO) of 95.1 % at-0.9 V (vs. RHE) and maintaining > 90 % FECO from-0.7 V to-1.0 V (vs. RHE). Furthermore, it retains over 80 % FECO after 10 h of continuous operation at-0.8 V (vs. RHE). Experimental results reveal that the high electrocatalytic performance of the Ag-ApmimBr/KB electrocatalyst is attributed to the introduction of ApmimBr, since it can modulate the electronic structure of Ag active sites and construct a CO2-enriched local reaction microenvironment. This work provides an innovative strategy using ionic liquids to rationally design efficient electrocatalysts for CO2RR.
Photoreduction of CO2 into high value-added products offers a promising approach to mitigating the global energy crisis. Coordination polymers (CPs) show promising potential in CO2 photoreduction due to their tunable structures. However, CP-based catalysts for CO2 photoreduction are limited by their poor recyclability and weak light absorption. Here, we have designed a new Zn-based CP {Zn-CP: [Zn(Bipn)Br2]n}, via the self-assembly of Zn ions and Bipn [N,N'-bis(3-imidazol-1-ylpropyl)naphthalenediimide]. Zn-CP shows high reactivity toward CO2 photoreduction with H2O, mainly due to the strong wide light absorption and high photoelectric conversion ability of the large conjugated naphthalenediimide rings of Bipn. Most importantly, the evolution rate of CH3OH (4.00 μmol g-1 h-1) is maintained after 10 photocatalytic cycles, while that of CO (45.28 μmol g-1 h-1) is maintained after 7 photocatalytic cycles and then significantly increased by ∼1.33 times for the next three photocatalytic cycles, demonstrating excellent catalytic stability of Zn-CP. The excellent recyclability of Zn-CP is much better than that of the most reported CP-based photocatalysts. The catalytic mechanism of Zn-CP toward CO2 photoreduction has been proposed based on experimental data combining with the DFT-calculated results. This work offers a promising strategy for developing efficient and ultrastable CP-based photocatalysts for solar-driven CO2 reduction.
Herein, a WO3@TCN photocatalyst was successfully synthesized using a self-assembly method, which demonstrated effectiveness in degrading organic dyestuffs and photocatalytic evolution of H2. The synergistic effect between WO3 and TCN, along with the porous structure of TCN, facilitated the formation of a heterojunction that promoted the absorption of visible light, accelerated the interfacial charge transfer, and inhibited the recombination of photogenerated electron–hole pairs. This led to excellent photocatalytic performance of 3%WO3@TCN in degrading TC and catalyzing H2 evolution from water splitting under visible-light irradiation. After modulation, the optimal 3%WO3@TCN exhibited a maximal degradation rate constant that was twofold higher than that of TCN alone and showed continuous H2 generation in the photocatalytic hydrogen evolution. Mechanistic studies revealed that •O2− constituted the major active species for the photocatalytic degradation of tetracycline. Experimental and DFT results verified the electronic transmission direction of WO3@TCN heterojunction. Overall, this study facilitates the structural design of green TCN-based heterojunction photocatalysts and expands the application of TCN in the diverse photocatalytic processes. Additionally, this study offers valuable insights into strategically employing acid regulation modulation to enhance the performance of carbon nitride-based photocatalysts by altering the topography of WO3@TCN composite material dramatically.
We present a ligand-to-metal charge transfer (LMCT)-enabled catalytic platform utilizing cerium(IV) benzoate complexes to address the long-standing challenge of directly coupling free alcohols with electron-rich alkenes, overcoming inherent polarity mismatches. This approach effectively circumvents the typical selectivity in single-electron transfer processes, enabling the selective generation of electrophilic alkoxy radicals from free alcohols in the presence of redox-labile electron-rich alkenes. The Ce-benzoate-based photocatalytic protocol promotes regioselective hydroetherification via both intramolecular cyclization and intermolecular addition pathways, showcasing broad functional group tolerance, operational simplicity, and versatility across a diverse array of alkenes, including silyl enol ethers and enamides/enecarbamates. Detailed mechanistic studies elucidate the structure of the active Ce(IV) benzoate catalyst, highlighting its unique selectivity for alkoxy radical generation, thereby establishing a practical and atom-economical framework for hydroetherification.
Methicillin‐resistant Staphylococcus aureus (MRSA) bloodstream infections pose significant health risks, potentially leading to severe conditions such as bacteremia. Developing effective treatments to eliminate resistant bacteria from the bloodstream, simultaneously mitigate infection‐related complications, and reduce mortality remains challenging. Herein, microspheres are synthesized with bacterial elimination and inflammation prevention by crosslinked sulfonium poly(amino acids). As‐synthesized microsphere, PM 1 0.6B MS, exhibits an ultrafast adsorption efficiency of 0.41 × 10 8 CFU mg −1 min −1 for MRSA, which positions the highest index among the reported resin and inorganic adsorptions. This bacterial‐specific and efficient capture of PM 1 0.6B MS is attributed to its strong interactions with teichoic acids in MRSA (Ka: 1.8 × 10 5 M −1 ) rather than acting with phospholipids of mammalian cells. Unlike the present resin‐based adsorbent, for example, heparin‐modified polyethylene in the only commercial Seraph ® 100, PM 1 0.6B MS kills adsorbed bacteria within 1 h and can be reused by simple treatment. Meanwhile, PM 1 0.6B MS also shows good hemocompatibility and longer thrombin activation time to reduce the risk of thrombosis and hemolysis. In vivo experiments further confirm the abilities of PM 1 0.6B MS to prevent inflammation by removing bacteria. This adsorbent is a promising candidate for early treating life‐threatening bloodstream infections, potentially preventing bacteremia and subsequent organ damage.
Dislocations in third-generation semiconductor gallium nitride (GaN) have always been a subject of intense study. Here, we investigate the core structures and electronic properties of prismatic edge dislocations in wurtzite GaN using a combination of the discrete Peierls theory and first-principles calculations. We identify four primary analytical core configurations, some of which exhibit reconstruction. Stable glide dislocations are found to be dangling-bond-free, whereas shuffle dislocations typically possess dangling bonds yet exhibit limited electronic activity. Different shuffle-type cores show similar electronic properties, consistent with their structural similarities. The intermediate states during glide dislocation motion may significantly influence GaN's electronic behavior. This work validates the accuracy of our combined theoretical and computational approach for atomic-scale dislocation characterization and establishes a foundation for dislocation engineering in high-performance GaN devices.
Over the past years, metasurfaces have demonstrated remarkable and diverse capabilities in advanced control over light properties. Embedding metasurfaces into the Fabry–Pérot (meta-F–P) cavity reduces the required cavity length and provides new degrees of freedom for tuning. Most meta-F–P cavities exhibit excellent color filtering effects within the visible spectrum. However, achieving single mode-F–P resonance across the entire near-infrared range remains challenging due to the phase condition limitations of the metasurfaces. Here, we explore the integration of silver metasurfaces into an F–P cavity with a cavity length of only 150 nm. The very short cavity length allows for the existence of gap surface plasmons between the silver metasurfaces and both the top and bottom silver mirrors of the F–P cavity. This setup achieves narrowband filtering in an ultra-wide spectral range from 626.6 to 2548.3 nm while consistently maintaining single-mode resonance. Furthermore, we analyze the filtering effects of embedding anisotropic structures into the F–P cavity under x- and y-polarized incident light, revealing polarization-dependent filtering capabilities. Embedding the metasurface within the F–P cavity also allows for stable responses to different angles of incident light. This study underscores the potential of meta-F–P cavities in advancing optical filter technology for diverse applications in spectroscopy, telecommunications, and sensing.