The rational design of covalent organic frameworks (COFs) for solid-state electrolytes (SSEs) is hindered by the precise position of polar functional groups (C ═ O) affect Li+ transport. Herein, we synthesize four COFs materials with systematically carbonyl substitution positions to elucidate their structure-property relationships. Among them, the β-ketoenamine-based COF featuring ortho-dicarbonyl groups exhibits a significantly enhanced electronegativity, which restricts anion migration and promotes selective Li+ transport. Consequently, the rich-carbonly COF SSE achieves a high ionic conductivity of 9.83 × 10-4 S/cm, a Li+ transference number of 0.8, and an electrochemical stability window exceeding 5.1 V. Symmetric cell delivers stable Li plating/stripping for over 1200 h at 0.2 mA/cm2 with a low overpotential of ∼0.1 V, and over 460 h at 0.5 mA/cm2. When coupled with a LiFePO4 cathode, the solid-state battery retains 80% capacity after 1230 cycles at 1 C and 80.2% after 700 cycles at 5 C. Theoretical calculations reveal that the ortho-dicarbonyl coordination environment lowers the Li+ migration barrier (0.376 eV) and enhances Li+-framework affinity, accelerating charge transfer. This work establishes a clear correlation from functional group positioning to pore chemistry, ion transport kinetics, and interfacial stability, offering a molecular-level design principle for high-performance COF-based solid-state electrolytes.

Circularly polarized (CP) lasers hold great potential for advancing cutting-edge chiroptical technologies, particularly in spin information communication and high-resolution displays, due to their unique capability to produce intense, highly coherent CP light. Most existing approaches to CP lasers still face prominent limitations, including rigorous fabrication conditions, scarce available material systems, and an inherent bottleneck in simultaneously realizing strong CP emission and efficient stimulated emission. Here, we report a simple and general host-guest strategy to construct high-performance CP random lasing systems, where achiral MAPbX3 perovskite quantum dots (QDs) with different halide compositions are integrated into enantiomeric MOF via in situ encapsulation. Strong Pb-O and Eu-X coordination interactions between the chiral MOF host and achiral QD guest enable efficient chirality transfer. Meanwhile, chiral MOFs act as effective scattering centers to provide sufficient optical feedback, sustaining stable random lasing oscillation. The optimized MAPbX3@P/M-EuBTC composites exhibit stable CP random lasing with a high glum of 1.52. Benefiting from halide composition modulation, the system realizes broadband tunable lasing emission covering 523-747 nm. This work establishes a reliable platform for developing high-performance CP light sources and offers valuable insights for the rational design of advanced lasing gain materials toward next-generation CP laser devices.

The temperature rise of a solar-heating textile is controlled by both generation and dissipation of heat. However, current designs mainly focus on increasing light absorption to generate more heat, often darkening the material while leaving thermal management largely overlooked. Herein, hollowing the nanofibers in a nonwoven mat produces a counterintuitive "brighter-yet-hotter" advantage over their solid (core-shell) counterparts. The polyacrylonitrile/polypyrrole double-shelled tubular nanofibers are fabricated by selectively removing the poly(ε-caprolactone) core from core-shell nanofibers. At outer and inner diameters of about 320 and 160 nm, the hollow nanofibers enhance backscattering in the visible range, making the mat brighter. Under 1 sun irradiation, the mat of hollow nanofibers shows a temperature rise of 28°C, which is 12% greater than that of the paired solid counterpart. Thermal modeling indicates that the higher temperature rise originates from the internal channels, which disrupt heat propagation across the fibers and lower the rate of heat dissipation. Side-by-side comparisons under simulated and outdoor sunlight show that the higher-temperature region consistently appears on the mat of hollow nanofibers. This work highlights the promise of hollow nanofibers as a structural platform for optical and thermal management in solar-heating textiles.

Microsized Si/C composite anodes are promising for practical lithium-ion batteries due to their high tap density and scalability. However, their performance remains constrained by structural degradation and an unstable solid electrolyte interface (SEI), and current strategies fail to address the intrinsic coupling between interfacial chemistry and Li+ transport kinetics. Here, a structure-interface co-engineered microspherical Mo/W@Gr-Si anode is developed by integrating a flower-like graphene framework with Mo2N/W2C dual-phase heterostructures, enabling simultaneous regulation of Li+ adsorption and diffusion. Coupled density functional theory (DFT) calculations and advanced characterizations reveal a mechanism linking interfacial stabilization with Li+ transport, where the Mo2N/W2C heterophase stabilizes an inorganic-rich SEI and reduces diffusion barriers via electronic structure modulation. Consequently, the Mo/W@Gr-Si anode exhibits a low Li+ adsorption energy (-2.071 eV) and a reduced diffusion barrier (0.42 eV), delivering a high reversible capacity of 1821 mAh g- 1 at 0.1C with an initial coulombic efficiency of 88.12%, along with outstanding rate capability and cycling stability. Full cell paired with an NCM523 cathode retains 88.2% capacity after 300 cycles (0.5C), while pouch cells exhibit 84.6% retention after 200 cycles at 2C. This work offers a generalizable strategy for bridging interfacial stability and Li+ transport kinetics in high-performance silicon anodes.

Osteoarthritis (OA) is increasingly recognized as a chronic inflammatory disorder driven by immune dysregulation, with early neutrophil infiltration associated with a pro-inflammatory phenotype and disrupted mitochondrial homeostasis. However, whether restoring neutrophil mitochondrial function can reprogram their inflammatory state and ameliorate OA remains unclear. Distinct from previous piezoelectric strategies for OA that primarily focus on chondrocytes or macrophages, this study focuses on neutrophil mitochondrial immunometabolism. Here, we report piezoelectric thulium-doped zinc oxide (Tm-ZnO) nanoparticles that associate with neutrophil mitochondria to restore mitochondrial homeostasis and reprogram neutrophil polarization. The ultrasmall size and positive surface charge of Tm-ZnO facilitate mitochondrial association, while its enhanced piezoelectric properties (14-fold increase in piezoelectric coefficient) enable activation by low-intensity pulsed ultrasound (LIPUS), generating localized bioelectric cues. This stimulation reduces mitochondrial ROS, enhances oxidative phosphorylation, and is associated with suppression of HIF-1/NF-κB signaling, thereby promoting neutrophil polarization from a pro-inflammatory N1 state toward a reparative N2 phenotype. In vitro and in vivo, Tm-ZnO+LIPUS attenuates synovial inflammation, restores chondrocyte anabolic activity, limits matrix degradation, and facilitates cartilage repair. Together, these findings establish a mitochondria-associated piezoelectric strategy for bioelectric reprogramming of neutrophil immunometabolism and highlight its therapeutic potential for OA and other chronic inflammatory diseases.

Actuation performance in fiber-based artificial muscles is commonly improved by introducing sufficient twist to produce fully coiled structures. Here, we present a new strategy to achieve large-stroke actuation in twisted-only liquid crystal elastomer (TLCE) yarn muscles through a thermally triggered, reversible twist-to-coil transition. Continuous, high-strength, and scalable LCE fibers were fabricated using direct ink printing. These fibers were then integrated with carbon nanotube yarns to fabricate electrothermal hybrid TLCE muscles. Above a critical twist density, the hybrid muscles electrothermally transform into coiled or plectoneme configurations, delivering a maximum quasi-static contractile stroke of up to 86%, a fast response time of 1.8 s, and stable cyclic operation over 10 000 cycles. The stroke enhancement originates from the reversible twist-to-coil transition, which is driven by a pronounced thermal reduction in both fiber length and Young's modulus, thereby lowering the critical torque needed for coiling. This mechanism introduces a new actuation mode for fiber-based artificial muscles and shows promising potential for confined-space manipulation, robotic grippers, and adaptive smart structures.

Photoresists for nanoimprint lithography are critical materials for the fabrication of semiconductors, optical metamaterials, and flexible electronics. However, conventional photocuring-based photoresists are unstable to heat and ambient light, complicating their usage, storage, and transport. Furthermore, their irreversible photocuring nature renders defects in imprinted nanostructures permanent and complicates the cleaning of photoresist-contaminated molds. Herein, we overcome these limitations by designing azopolymer photoresists exhibiting photoinduced reversible solid-to-liquid transitions. Compared to conventional photoresists, the azopolymer photoresists exhibited superior thermo- and photostability. An azopolymer photoresist stored in our laboratory for over 10 years remained usable for nanoimprint lithography, demonstrating exceptional long-term stability. Additionally, the photoinduced reversible solid-to-liquid transitions of azopolymer photoresists enable defect correction in imprinted nanostructures. The linear chain structure of azopolymer photoresists facilitates the cleaning of photoresist-contaminated molds using solvents. The photoresists developed in this work combine long-term stability and high-resolution patterning, offering a promising approach among existing azo-based lithography strategies. This work demonstrates that azopolymers with photoinduced reversible solid-to-liquid transitions are stable photoresists with defect-correction and mold-cleaning capabilities for nanoimprint lithography.

Developing degradable poly(lactic acid) (PLA) covalent adaptable networks that simultaneously integrate mechanical robustness, creep resistance, reprocessability, and tunable multi-shape memory remains a major challenge, particularly when low-molecular-weight PLA is used as the sustainable precursor. Here, we report a poly(lactic acid) dual-dynamic network with inverse cross-link-density/activation-energy coupling constructed through a facile one-pot reaction of commercially available PLA diols, hexamethylene diisocyanate trimer, and 2,2'-diaminodiphenyl disulfide (DADS). The network architecture couples a densely cross-linked disulfide-containing dynamic network with low activation energy (Ea) and a loosely cross-linked PLA-rich dynamic network with high Ea. The dense low-Ea network provides mechanical reinforcement, low-temperature stability, and rapid thermally activated rearrangement, whereas the loose high-Ea network contributes extensibility, creep resistance, elastic energy storage, and high-temperature processability. By regulating PLA molecular weight and DADS/PLA ratio, the dual-dynamic networks show tunable glass transition, degradation rate, and rearrangement kinetics. Such unique hierarchical dual-dynamic network architecture with inverse cross-link-density/activation energy coupling endows the material with prominent stiff-toughness, reprocessability, creep resistance, and reconfigurable multi-shape memory capability. Moreover, adaptive medical fixation and photothermal-assisted therapeutic prototypes demonstrate the potential of these reconfigurable shape memory PLA networks with cytocompatibility for sustainable biomedical devices.

Semiconductor-based sensors suffer from baseline drift that compromises measurement accuracy. Ratiometric sensing offers a solution by introducing a photoresponse internal reference, yet conventional materials face an inherent trade-off between gas sensitivity and photoelectric stability. Here, we report a 2D organometallic chalcogenide, PbBD, featuring a multi-quantum well structure composed of a continuous inorganic {PbS}n layer partially covered by compact and flexible organic ligands. This unique configuration exposes active sites on the inorganic layer, allowing gas molecules to directly interact with the inorganic semiconductor layer, bypassing the indirect electron transfer pathway typically imposed by functional groups. This direct interaction facilitates electron transfer efficiency and significantly enhances the sensitivity in gas sensing applications. The PbBD nanosheet-based sensor achieves an ultrahigh response of 52900% to 10 ppm NO2 and a ratiometric value of 0.84, which is 3.67 times higher than that of AgBDT. PbBD delivers both enhanced ratiometric sensitivity and an exceptionally low detection limit of 0.245 ppt, marking the lowest value ever reported for room-temperature chemiresistive NO2 sensing. Furthermore, the ratiometric mode reduces the coefficient of variation from 21.8% to 5.5% against temperature fluctuations. This work provides a strategy for co-optimizing photoelectric and gas-sensing properties toward high-precision sensing applications.

Aesthetic and reconstructive repair requires biomaterials that restore tissue architecture while controlling contour fidelity, scar quality, mechanical compliance, and long-term morphological stability in dynamically loaded environments. However, conventional fillers, scaffolds, and wound-care materials largely act as passive supports and offer limited capacity to adaptively regulate the regenerative microenvironment. In this Review, we present piezoelectric signaling as a mechanoelectrical strategy for electro-aesthetic regulation, whereby endogenous tissue motion or externally applied mechanical energy is converted into localized bioelectrical cues. We establish a bioelectrical information framework in which mechanical inputs are encoded into spatiotemporally organized electrical signals and biologically decoded through ion-channel activation, Ca2 + signaling, cytoskeletal remodeling, immune regulation, angiogenesis, and extracellular matrix reorganization. We further examine how molecular polarity, crystalline phase, structural architecture, and interfacial coupling govern signaling across naturally derived biomolecules, synthetic polymers, inorganic materials, and hybrid piezoelectric systems. Representative applications include dermal repair and scar modulation, PLLA-based regenerative fillers and emerging injectable electroactive platforms, craniofacial reconstruction, multimodal stimulation, and sensing-enabled closed-loop bioelectronics. Key translational challenges include signal dosimetry, hydrated-state stability, degradation-dependent performance, biosafety, structural fidelity, and standardized aesthetic evaluation. Piezoelectric signaling may therefore shift aesthetic and reconstructive repair from passive structural restoration toward adaptive, bioelectrically mediated, and feedback-guided regulation.

An in situ-grown TpTt/NH2-MIL-125(Ti) covalent organic framework/metal-organic framework (COF/MOF) heterojunction was constructed for visible-light-driven degradation of imidacloprid (IMD) coupled with peroxymonosulfate (PMS) activation. The composite combines the visible-light absorption and π-conjugated charge-transport framework of TpTt-COF with the porous Ti-containing and amino-functionalized microenvironment of NH2-MIL-125(Ti). X-ray photoelectron spectroscopy (XPS) and photoelectrochemical analyses indicate interfacial charge redistribution and suppressed charge recombination. The optimized TpTt/NH2-MIL-125(Ti)/PMS/Vis system achieved 100% IMD removal within 150 min and retained activity across pH 3-9 and in the presence of common anions. Electron paramagnetic resonance spectroscopy (EPR) spectroscopy and scavenging experiments identified SO4•-, •OH, and 1O2 as the main reactive species. Liquid chromatography-mass spectrometry (LC-MS), DFT-predicted reactive sites, and ECOSAR analysis were integrated to examine the transformation pathway and the predicted ecological toxicity of the products. The distinguishing feature of this study is the integration of an in situ COF/MOF interface, photoassisted PMS activation, and pesticide-specific transformation and toxicity analysis within one catalyst system.

The carbonatation poisoning of solid oxide fuel cells (SOFC) cathode materials in CO2-containing atmospheres, which leads to a sharp decline in oxygen reduction reaction (ORR) activity and performance degradation. This seriously limits their long-term stability and practical application under medium- to low-temperature conditions. Therefore, developing cathode materials that possess both high ORR activity and excellent CO2 tolerance has become a current research focus. Although existing reviews have surveyed CO2 poisoning phenomena in SOFC cathodes, a critical knowledge gap remains regarding the systematic correlation between degradation mechanisms and rational cathode modification strategies. This paper reviews the poisoning mechanisms of SOFC cathodes in a CO2 environment, including the formation of carbonates on the cathode surface, the reduction in oxygen reduction reaction efficiency, and the deterioration of performance and stability. It also focuses on summarizing recent material design and modification strategies aimed at improving cathode performance and CO2 tolerance, and compares the effectiveness of various strategies in enhancing cathode CO2 resistance. Through a systematic review of recent related research, this paper aims to provide a clear theoretical framework and design ideas for developing CO2-tolerant cathodes with high activity and stability, in order to promote the practical application of SOFC in carbon-containing environments.

The chlorine evolution reaction (CER) is central to chlor-alkali electrolysis, yet Ru‑based anodes often suffer from competitive oxygen evolution and anodic dissolution under acidic potentials. Here, we report 2D ultrathin amorphous Sn‑doped RuOx nanosheets prepared via atomic engineering, in which Ru-O covalency and the Ru oxidation state are simultaneously modulated. Structural and spectroscopic analyses indicate that Ru centers are stabilized against over‑oxidation, suppressing the formation of volatile RuO4 or soluble RuO5 2-. Operando attenuated total reflection surface-enhanced infrared absorption spectroscopy, combined with 18O isotope labeling, reveals negligible lattice‑oxygen participation and a preference for direct Cl- adsorption, thereby suppressing oxygen evolution and promoting CER. The optimized Ru-based catalyst achieves high CER selectivity (∼97%), long-term stability (>300 h), and mass activity nearly 40 times higher than commercial benchmarks. These results highlight the significant potential of metal-oxide bond-covalency modulation as a viable strategy for durable anodic oxidation electrocatalysis.

Precise control of trap states in amorphous dielectrics requires identifying the fundamentally different physical origins of hole and electron trapping. Here, in amorphous silicon nitride (a‑SiNx), we demonstrate a dual-origin mechanism where the two trap polarities arise from decoupled structural and electronic mechanisms, enabling polarity-selective engineering of charge storage behavior. Multi-spectroscopic characterization reveals that hole traps are dictated by structural disorder, where Si-rich nanoclusters form a percolating network whose cluster-size statistics exhibit power-law scaling characteristic of disordered connectivity. In contrast, electron traps are governed by electronic-level alignment, where Hf incorporation lowers the Fermi level, activates deep in-gap states, and introduces additional shallow levels near the conduction-band edge-without perturbing the optimized nanocluster states. By linking structural topology and electronic alignment to polarity-resolved trapping, this work establishes a unified physical picture of trap polarity in disordered dielectrics and provides a practical design route for next-generation charge-trap memories and amorphous nitride/oxide electronic systems.

Disorder in multinary crystals is often the hidden degree of freedom that governs phase stability, interfacial bonding, and functional performance. Here we establish an electron-crystallographic strategy that converts atomic-resolution electron energy-loss spectroscopy (AR-EELS) acquired along multiple zone axes into quantitative, site-specific occupancies, enabling 3D decoding of cation disorder in complex solids. Applying this approach to polytypic Cu-Zn-Sn-S (CZTS) nanocrystals, we directly resolve the cation sublattices in both zincblende- and wurtzite-derived polymorphs. We find reproducible Cu/Zn mixed occupancy without detectable site preference in both phases, whereas Sn remains fully ordered in the zincblende-derived polymorph but is partially replaced by Zn (∼35%) in the wurtzite-derived counterpart, consistent with its Zn-rich/Sn-poor composition. These experimentally constrained occupancies, together with reciprocal-lattice reconstruction, support average structural models consistent with I-42m and Pmn21 symmetry. Density functional theory further compares the energetics of candidate ordered and disordered structures at fixed compositions and supports the energetic plausibility of the experimentally constrained models. This AR-EELS electron-crystallography workflow provides a potentially transferable framework for occupancy-resolved analysis of multinary materials under suitable experimental and crystallographic conditions.