Physics
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Electrically Responsive Membrane The cover highlights the electrically responsive MXene/Co–C3N4 membrane designed for efficient dye separation. Under an electric field, the membrane exhibits enhanced permeability, high selectivity, and antifouling properties. This synergistic design, combining conductive pathways and interfacial engineering, provides a molecular-level approach for advanced wastewater treatment applications. More details can be found in the Research Article by Liguo Shen and co-workers (DOI: 10.1002/adfm.75584).
ABSTRACT For the development of proton exchange membranes (PEMs), particularly for high‐temperature anhydrous proton transport, a phosphonate polymerizable amphiphile (PPA) is newly synthesized. To fabricate an anhydrous proton conductive (APC) polymer‐stabilized film, PPA is combined with a liquid crystal (LC) crosslinker in a 6:4 weight ratio, forming an LC reactive mesogen (LCRM) mixture. This mixture self‐assembles under uniaxial orientation in the smectic mesophase, and subsequent photopolymerization generates continuous and aligned proton transport pathways within the hierarchical two‐dimensional (2D) nanostructure film. The resulting polymer film exhibits high proton conductivity at elevated temperatures, with anisotropic transport properties dictated by molecular orientation. Furthermore, the proton conductivity can be finely tuned by manipulating the molecular self‐assembly at the nanoscale and the molecular orientation at the macroscale. A comprehensive understanding of the interplay between molecular packing structure, macroscopic molecular orientation, and proton transport behavior in APCs demonstrates the critical role of precise functional group positioning in establishing efficient proton conduction pathways. The hydrophobic nature, high thermal stability, and exceptional chemical durability of these proton‐conductive films further emphasize their potential as next‐generation materials for high‐temperature PEM applications.
ABSTRACT The sulfur reduction reaction (SRR) involves complex multi‐phase transitions, posing conflicting demands that single‐component catalysts cannot meet. Zr‐based MOFs (e.g., UiO‐66) offer high stability but suffer from orbital mismatch between hard Lewis acidic nodes and soft polysulfides, limiting host–guest interactions and hindering liquid‐to‐solid conversion kinetics. Herein, we bridge this gap through Lewis acidity tailoring. A Co‐doped UiO‐66‐NO 2 modified separator is constructed to establish a synergistic hard–soft acid interface. By incorporating soft Co active sites into the robust hard Zr‐MOF framework, we harmonize the host–guest interaction based on the Hard‐Soft Acid‐Base (HSAB) principle. DFT calculations and kinetic analyses reveal a specific dual‐mechanism where the Co sites utilize optimized d‐p orbital hybridization to strongly anchor soft polysulfides, while concurrently acting as targeted catalytic centers to severely reduce the nucleation barrier of the sluggish Li 2 S 4 → Li 2 S 2 /Li 2 S transformation. Consequently, the cell achieves a high reversible capacity of 902.1 mAh g −1 at 0.5 C and an ultralow decay rate of 0.0238% over 500 cycles. This work not only demonstrates a high‐performance Li–S battery separator but also establishes a molecular‐level HSAB‐guided strategy for designing advanced catalyst materials in multi‐phase conversion electrochemistry.
ABSTRACT Femtosecond laser‐driven synthesis provides a versatile method for producing nanoparticles with high purity and compositional tunability, suitable for applications in catalysis and nanomanufacturing. However, conventional kinetic models typically treat reactions as continuous, overlooking the pulsed nature of laser excitation, thereby constraining their applicability in directing experimental synthesis. In this study, we established a femtosecond laser‐induced strategy for nanostructures by dividing the processing timeline into pulse‐on and pulse‐off phases to elucidate nanoparticle formation dynamics. Nanoparticle generation encompasses two principal processes: Ultrafast reduction and nucleation ( k 1 ) primarily during pulse‐on phases, and growth ( k 2 ) across both phases. Mass spectrometry further revealed the evolution of solution species in a representative metal precursor system. Employing this framework, we adjusted laser repetition rate to modulate pulse‐on proportion. Higher repetition rates increased k 1 , boosting nucleation and yielding smaller nanoparticles. Lower rates favored k 2 , producing larger particles. This methodology was extended to synthesize diverse monometallic, bimetallic, and high‐entropy nanoparticles across various elements and substrates, as demonstrated by their applicability in representative electrocatalytic reactions, including CO 2 reduction and hydrogen evolution. This work offers a mechanistic basis connecting laser parameters, pulsed dynamics, and nanoparticle properties, promoting rational ultrafast laser nanomaterial design for a wide range of metal and alloy systems.
ABSTRACT Arterial diseases alter blood vessel function through complex mechanisms, requiring microphysiological systems that mimic human arteries. We established an artery‐on‐chip (ARTOC) using vascular derivatives of human induced pluripotent stem cells (iPSCs) cultured with pulsatile flow on an electrospun fibrin hydrogel. ARTOCs possessed mature, multilayered smooth muscle expressing robust extracellular matrix and contractile proteins, exhibiting stimuli‐induced contractility and achieving material properties comparable to those of native arteries. Using real‐time monitoring of circumferential strain and luminal pressure to inform computational fluid dynamics modeling, we successfully tuned biomechanical cues to promote the function of both endothelial and smooth muscle cells simultaneously in the ARTOC. Multiplexed protein and transcriptomic expression analysis of ARTOCs revealed a dynamic response to pulsatile flow over time. For disease modeling, we used iPSCs from a polycythemia patient, finding aberrant cytoskeletal protein expression and increased vessel wall stiffness in diseased ARTOCs compared to controls. We then characterized a novel isogenic disease model using iPSCs CRISPR‐edited with the LMNA Hutchinson‐Guilford Progeria Syndrome mutation. LMNA HGPS ARTOCs showed excessive extracellular matrix accumulation, medial layer loss, premature senescence, and reduced tissue elasticity. The tunable material‐based ARTOC platform accurately models healthy and diseased arteries, representing a significant step toward translational research.
ABSTRACT Owing to its economic and environmental benefits, direct regeneration has been regarded as a promising approach. However, for degraded high‐nickel layered cathodes during cycling, the rock‐salt phase could be formed on the surface, serving as Li‐ions diffusion barrier, which would inhibit the in‐depth relithiation and structural recovery. Herein, the Li 2 MoO 4 ‐induced surface reconstruction strategy is proposed to successfully regenerate spent NCM. Significantly, the surface properties are further reconstructed, along with the doping of Mo‐atoms into the lattice framework with improved stability. Assisted by ex/in situ exploring, it could be confirmed that Li 2 MoO 4 could promote charge redistribution and strengthen TM─O─Mo coupling, which contributes to the lowering of Li + migration barrier and the recovery of layered phase. As a result, the as‐regenerated NCM delivers a high discharge capacity of 179.1 mAh g − 1 at 1.0 C and retains 87.71% capacity after 200 cycles, better than that of traditional solid‐state regenerated NCM (58.11%). Moreover, the reconstructed surface is beneficial for suppressing structural strain and interfacial side reactions, leading to improved kinetic behavior and stability. This work is expected to shed light on the transformation behaviors for overcoming surface structural barriers, meanwhile offering significant strategies for direct regeneration of high‐nickel cathodes.
ABSTRACT Controlling nucleation behavior represents a critical yet underexplored avenue for improving non‐fused acceptor–based organic solar cells (OSCs), where sluggish nucleation and uncontrolled phase separation often limit optimal morphology formation. Here, we propose an effective strategy to modulate nucleation dynamics through side‐chain fluorination. Two non‐fused acceptors, 3TT‐0F and 3TT‐9F, were designed to probe how side‐chain fluorination modulates thermodynamics and intermolecular organization. Differential scanning calorimetry reveals that 3TT‐9F exhibits a larger Gibbs free energy difference between liquid and crystalline phases, indicating a reduced nucleation barrier. Complementary density functional theory and molecular dynamics simulations demonstrate that side‐chain fluorination enhances molecular dipole moment and strengthens intermolecular interactions, fostering tighter packing and improved donor–acceptor interaction. Consequently, 3TT‐9F forms smaller domain sizes and purer phase domains with enhanced molecular ordering in blend films, which is confirmed by grazing‐incidence wide‐angle x‐ray scattering and Resonant soft x‐ray scattering analysis. These synergistic effects facilitate more balanced charge transport and suppressed recombination. Devices incorporating 3TT‐9F achieve outstanding efficiencies of 17.2% in binary and 20.0% in ternary devices. This work establishes fluorination as an effective strategy to regulate nucleation behavior and morphological evolution in high‐performance non‐fused acceptor systems.
ABSTRACT Introducing controlled porosity into crystalline materials endows them with properties not exhibited by their solid counterparts. However, producing microparticles that combine submicron macroporosity and uniform particle shapes remains a significant challenge. Here, we present a general strategy that yields unique single‐crystal microparticles with closed‐cell macropores (300–500 nm), a size ideal for generating structural colour. Using a bioinspired approach, we occlude three distinct additives, polystyrene microspheres, polymer vesicles, and amino acids, within 10–20 µm calcite (CaCO 3 ) single crystals. Remarkably, after thermal annealing, all systems are transformed into particles with well‐defined shapes and macroporosity, while retaining their single‐crystal character. This is particularly surprising for the amino acids, which are originally distributed as individual molecules throughout the crystal lattice. Mechanistic studies using solid state NMR and in situ TEM directly track pore formation and reveal that co‐occluded water associated with the amino acids is crucial in creating the pores. This simple method—where the occlusion of amino acids is scalable and compatible with industrial calcite synthesis—delivers a new class of macroporous microparticles suited to coatings, fillers and photonic applications, where their bright white appearance and intense broadband light reflection makes them an environmentally‐benign alternative to titanium dioxide for whitening applications.
Abstract Steep-slope transistors are essential for next-generation ultra-low-power electronic systems operating at reduced supply voltages. However, conventional silicon tunnel field-effect transistors (TFETs) suffer from limited ON-state current due to weak tunneling probability at the source-channel junction. In this work, aSi₀.₅Ge₀.₅ source graded-channel ferroelectric TFET (SiGe-GC-Fe-TFET) is proposed and systematically investigated using calibrated TCAD simulations. The device integrates SiGe source bandgap engineering, graded channel electrostatic modulation, and a ferroelectric Si:HfO₂ gate stack to simultaneously enhance tunneling efficiency and gate controllability. The optimized structure demonstrates a high ON-current of 3.95 × 10⁻⁴ A, an I ON /I OFF current ratio of ~1.2 × 10¹⁰, and a steep point subthreshold swing of 23.8 mV/dec at V DD = 0.5 V, confirming superior switching performance. The proposed device further exhibits improved analog/RF behaviour with a cutoff frequency of ~15 GHz, gain-bandwidth product of ~33 GHz, and reduced Miller capacitance, enabling enhanced high-frequency response. Linearity analysis shows improved distortion immunity with VIP3 ≈ 3 V and IMD3 ≈ -2 dBm, while noise analysis reveals significantly suppressed current and voltage noise spectral densities. Finally, inverter circuit implementation confirms enhanced static noise margin and reduced dynamic overshoot. These results demonstrate that the integrated effect of SiGe heterostructure engineering, graded channel design, and ferroelectric negative capacitance provides an effective pathway toward high-performance, energy-efficient TFETs for future low-power mixed-signal and RF applications.
Abstract Oxygen vacancies play a crucial role in determining the electronic structure, thermoelectric, and optical properties of β-Ga₂O₃ , while their influence is highly dependent on the crystallographic site due to the monoclinic structure with three inequivalent oxygen positions. In this work, we systematically investigate the site-dependent effects of oxygen vacancies in two-dimensional(2D) β-Ga₂O₃ using First-principles with the HSE06 hybrid functional coupled with Boltzmann transport theory. Our calculations reveal that oxygen vacancies act as deep donor levels in 2D β-Ga₂O₃ . The thermoelectric properties exhibit pronounced site dependence: the V O3 vacancy yields the largest Seebeck coefficient ( 1912μV/K at 300 K) and the highest n-type electrical conductivity (2.5×10 18 /(Ω•m•s) at 300 K), leading to an outstanding power factor of 7.48×10 10 W/(m•K² for pristine and oxygen-deficient •s). Meanwhile, the optical properties are most strongly modulated by the V O2 vacancy, which induces the largest red shift of the absorption edge (down to 2.83 eV) and gives rise to two distinct absorption peaks. These results demonstrate that oxygen vacancies play a key role in determining the thermoelectric and optical properties of 2D β-Ga₂O₃ due to the site-dependent modulation of electronic structure, thereby providing valuable guidance for defect engineering in optoelectronic and thermoelectric devices.
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