PILPMS triple-network hydrogel containing MXene/IL dual conductive networks shows superior mechanics, high conductivity and efficient NIR photothermal effect, suitable for motion monitoring, TENGs, wearable heating and self-powered sensing.
High-performance polydicyclopentadiene(PDCPD) elastomeric materials were prepared by copolymeri-zing dicyclopentadiene(DCPD) with tricyclopentadiene(TCPD) and introducing a low-molecular-weight polybuta-diene(PB) with good compatibility for blending modification. The copolymerization of DCPD and TCPD allowed for the tuning of material rigidity; the introduction of PB decreased the crosslinking density, reduced the proportion of rigid cyclic structures, and provided a plasticizing effect, collectively transforming PDCPD from a rigid thermoset into a flexible elastomer. When the PB content(mass ratio to DCPD/TCPD mixture) reached 35%, the modified PDCPD exhibited a tensile strength of 12 MPa and an elongation at break of 296%, demonstrating a thermoset elasto & hybull; meric behavior. Scanning electron microscopy of the tensile fracture surface, dynamic mechanical analysis, and ther & hybull; mogravimetric analysis indicated that PB existed in the system as a physically blended phase. Although excessive PB addition slightly deteriorated the water resistance, the maximum water absorption of the material remained below 0.9% after immersion in deionized water at 60 degrees C for 48 h. This study provided an effective approach to transforming PDCPD into an elastomer through blending modification with low-molecular-weight polymers.
Self-assembled monolayers (SAMs) serve as critical hole-transporting components at the buried interfaces of high-performance inverted perovskite solar cells (PSCs). Herein, comprehensive classical molecular dynamics (MD) simulations were performed to elucidate the intricate non-covalent interactions governing the co-assembly of symmetric and asymmetric SAM configurations. Our molecular insights reveal that the asymmetric SAMs possess a pronounced dipole moment that promotes robust interfacial hydrogen bonding while simultaneously mitigating homo molecular π-π packing. Crucially, blending symmetric and asymmetric SAMs further decouples the π-π interactions, thereby synergistically boosting anchoring stability and maximizing surface coverage. Overall, these findings demonstrate that precise manipulation of weak non-covalent interactions within SAM networks represents a potent and generalizable paradigm for optimizing interfacial properties in advanced optoelectronics.
Flexible aqueous zinc-ion batteries (FAZIBs) are hindered by the intrinsic instability of water in conventional hydrogel electrolytes, resulting in narrow electrochemical windows and poor performance across extreme temperatures. A hierarchical water-regulation strategy is introduced to concurrently suppress free water at the salt level and immobilize residual water within a polymer network. A one-pot dual-network hydrogel electrolyte (PX-Zn) is developed by integrating a low-cost, TFSI-free ZnCl2-based water-in-salt system with a poly(2hydroxyethyl acrylate)/xanthan gum framework. The concentrated ZnCl2 disrupts the bulk hydrogen-bonding network of water, while abundant -OH and -COOH groups in the polymer matrix lock residual water through dynamic hydrogen and ionic interactions. This dual confinement expands the electrochemical stability window to 3.15 V, suppresses freezing and evaporation, and enables stable operation from -20 to 80 degrees C. Cl--mediated coordination promotes dissociation of Zn2+-Cl-complexes and inhibits anion migration, leading to a high Zn2+ transference number (0.53) and dendrite-free zinc deposition. The PX-Zn electrolyte exhibits high ionic conductivity (42.6 mS cm-1 at 20 degrees C, 18.2 mS cm-1 at -20 degrees C), transparency, toughness, and strong adhesion. Flexible Zn//PX-Zn//polyaniline batteries deliver capacities of 137 mAh g-1 at 25 degrees C and 93 mAh g-1 at -20 degrees C (2.5 A g-1), and demonstrate exceptional cycling stability-over 4000 cycles at -20, 0, and 25 degrees C and 1000 cycles at 40 degrees C-with nearly 100% Coulombic efficiency. This TFSI-free, scalable design overcomes the traditional trade-off among ionic conductivity, mechanical robustness, and thermal resilience, offering a practical pathway toward durable, wide-temperature FAZIBs for wearable electronics.
The electrochemical performance of Ti3C2Tx MXene arises from chemical and electrostatic interactions between its surface terminations and interlayer molecules. Moving beyond the conventional paradigm of relying on the intercalation of external guest species to modulate this network, this study addresses a more fundamental question: can the interaction environment be intrinsically engineered from within the MXene lattice? Here, carbon (C) vacancies are introduced as a precise strategy to polarize the surface electronic structure, specifically enhancing the electronegativity of oxygen terminations. This polarization strengthens the hydrogen bonding (H-bonding) interactions with confined water, leading to the formation of a thermally stable, "active and fixed" interlayer architecture. This optimized structure results in a significant increase in intrinsic capacitance, with the Ti3C1.7 electrode achieving 348 F g-1 at 5 mV s-1, a 47% enhancement over the near-stoichiometric Ti3C2.0. Subsequent anodic oxidation alleviated ion diffusion limitations at high rates, synergistically improving rate capability. The co-engineered electrode achieved a high capacitance of 382 F g-1 while retaining 45% capacitance at an ultra-high scan rate of 5000 mV s-1. This work establishes the rational design of interfacial H-bonding networks as a core principle for advanced MXene electrodes, offering a pathway to high energy and power densities.
Aqueous zinc-ion batteries (AZIBs) have been the focus of significant research interest in the field of energy storage at an extensive scale; however, their practical application remains constrained by the slow diffusion rate of Zn2+ and limited utilization of active sites in cathode materials. Herein, an iodine-doping strategy is developed to modulate the crystal and electronic structure of iodine-doped Na2V6O16·3H2O (INVO) via a one-step hydrothermal route. The incorporation of iodine has been shown to induce abundant oxygen vacancies and to enlarge the interlayer distance, which synergistically accelerates charge transfer and increases Zn2+ diffusion kinetics. The optimized electrode demonstrates significant advantages in terms of structure and electronics, which contribute to its exceptional performance. It exhibits a considerable capacity of 582.2 mAh g-1 at 0.1 A g-1, a notable rate capability of 470.6 mAh g-1 at 1 A g-1, and high cycling stability with 90.3
Chiral vanadium oxide nanoparticles (V2O3 NPs) with different chiroptical signals were successfully prepared by employing tartaric acid, malic acid, and penicillamine as chirality-inducing agents. These chiral nanoparticles show sensitivity to pH values as they could express various optical transition modes such as charge transfer, d-d transitions, and surface plasmon resonance due to their rich electronic states, leading to tunable chiral optical activities in the UV-visible range. The different colors of V2O3 NPs with varied ligands at different pH values indicate the configuration variation of the chiral ligands as revealed by UV-visible absorption spectroscopy and circular dichroism (CD) characterizations. In addition, the as-synthesized chiral V2O3 NPs exhibit suitable properties for use as biomolecular probes and exhibit a limit of detection (LOD) of 3.185 mu M for H2O2 sensing, indicating that chiral V2O3 NPs could provide a highly sensitive and real-time sensing scheme, which may provide a useful strategy for the development of chiral materials in the areas of chiroptics and biosensors.
Biodiesel, a renewable bio-based transport fuel consisting of alkyl esters of long-chain fatty acids, is gaining attention as an alternative to non-renewable petroleum diesel. We prepared adjustable interlayer spacing ureacrosslinked 3D graphene oxide/MXene-SO3/cyclodextrin (MGUC) film to achieve efficient and sustainable biodiesel production. Ti3C2TX (MXene) grafted sulfonic acid groups as acid-catalytic sites of the film with graphene oxide (GO) via urea cross-linking and doping cyclodextrin (CD) to construct multistage pore structures (internal pore structures generated by urea cross-linking as well as CD host-guest structures) synergistically catalyzed biodiesel production. Meanwhile, the heterogeneous carbon-based materials based on GO and MXene-S have excellent photothermal efficiency, which can achieve 95.6 % biodiesel conversion at 4 h and maintain 75.32 % activity after 8 cycles. We verified the reason for the high catalytic activity of the MGUC films, which rationalized the fast mass transfer mechanism of CD by Density functional theory (DFT)and verified the transport mechanism of the heterojunction for efficient photothermal. Therefore, this CD carbon-based solid acid film catalytic platform provides a new direction for the green and efficient preparation of bioenergy.
The performance of sulfur-based cathodes is restricted by the poor conductivity of sulfur and the shuttle effect of lithium polysulfides (LiPSs). Herein, an effective N-doped carbon/Ti3C2T x (NC/Ti3C2T x ) free-standing architecture was designed as a sulfur host for achieving high sulfur loadings, considerable electronic conductivity and good LiPS trapping ability to suppress the shuttle effect. Consequently, an excellent electrochemical performance was achieved for the NC-S/Ti3C2T x freestanding structure with a 38% increase in capacity compared with the counterpart electrode of slurry-coated NC-S/Ti3C2T x . Moreover, the NC-S/Ti3C2T x freestanding structure exhibits a high capacity of 1156 mA h g-1 at 0.1C and a high capacity retention of 79.5% after 100 cycles. Moreover, this architecture enabled high sulfur loadings, and thus, a high areal capacity of 3.41 mA h cm-2 was obtained.
Bioelectric fields play a critical role in skin wound repair by guiding cell proliferation, migration, and differentiation, and thereby accelerating wound healing. However, the biochemical microenvironment in diabetic wounds can diminish the endogenous electric fields (EEFs) and severely delay the healing process. Therefore, constructing bionic skin capable of restoring the EEF is an effective strategy for diabetic wound repair. In this study, a thermoelectric hydrogel-based bionic skin is developed using an artemisinin (ART)-loaded silver selenide methacrylate hydrogel (Ag2Se@GelMA/ART). Using the thermoelectric effect, the bionic skin can generate a bioelectric field driven by a skin-to-air temperature gradient, thereby offering a novel approach for restoring EEFs. In vitro studies show that Ag2Se@GelMA/ART bionic skin significantly promoted the proliferation, migration, and angiogenesis of human umbilical vein endothelial cells. In vivo, the bionic skin accelerated diabetic wound healing and enhanced neovascularization and collagen deposition. Subsequent observation suggested that the bionic thermoelectric skin generating the external electric field inhibits the expression of prolyl hydroxylase domain-containing protein 2 (PHD2), and upregulates the hypoxia inducible factor (HIF)-1 alpha and vascular endothelial growth factor (VEGF)-A, which can benefit the process of angiogenesis. Thermoelectric bionic skin represents a novel therapeutic strategy for diabetic wound care, offering new avenues for tissue engineering.
The current treatment of diabetic foot ulcers remains a great challenge due to the persistent chronic inflammatory trauma microenvironment caused by oxidative stress, elevated levels of inflammatory factors, impaired angiogenesis, and bacterial infection. However, current therapeutic strategies primarily focus on wound closure rather than addressing the underlying pathophysiology of diabetic wounds. Therefore, there is an urgent need for advanced wound dressings that not only promote wound closure but also modulate the wound microenvironment to accelerate tissue regeneration. Here, we report a multifunctional hydrogel dressing that can be conveniently fabricated through copolymerization of a complex formed by a polydopamine-polyethyleneimine hybrid coating (PDA-PEI) and GelMA. This hydrogel exhibits excellent mechanical strength, tissue adhesion, and self-healing capacity. It demonstrates antibacterial activity, alleviates oxidative stress and inflammation, promotes angiogenesis, regulates macrophage polarization, and enhances full-thickness skin regeneration in MRSA-infected diabetic mice. The article highlights the potential of this hydrogel as a promising therapeutic strategy for improving the clinical management of diabetic foot ulcers.
Colloidal quantum dots (QDs), notably lead sulfide (PbS) QDs, represent a promising platform for short-wave infrared (SWIR) photodetection, offering a cost-effective and scalable alternative to conventional indium gallium arsenide (InGaAs) systems. This study investigates the pivotal role of PbS QD size in optimizing the hole transport layer (HTL) for SWIR photodetectors, addressing the interplay among film morphology, electronic structure, and device performance. Through the precise synthesis of monodisperse PbS QDs (3.33-4.14 nm) and solid-state ligand exchange with 1,2-ethanedithiol (EDT), we reveal that smaller QDs, while benefiting from strong quantum confinement and superior electron blocking, suffer from pronounced volumetric shrinkage and microcracking due to high ligand-to-QD ratios. Conversely, larger QDs enhance film integrity but introduce surface-facet-dependent defects and increase dark current density. Combining transmission electron microscopy, absorption spectroscopy, photoluminescence quenching, and space-charge-limited current analysis, we elucidate the size-dependent trade-offs governing HTL functionality. Devices with intermediate-sized QDs (e.g., 4.04 nm) achieve peak external quantum efficiency (55.74%), responsivity (0.54 A/W), and specific detectivity (5.50 × 1012 Jones), while smaller QDs (3.33 nm) excel in trap state suppression and faster response speed (1.0 μs rise and 1.3 μs fall). These findings establish a materials-by-design framework for tailoring QD size to balance mechanical stability and optoelectronic performance, advancing solution-processed SWIR imaging technologies.
Enzyme immobilization has emerged as a promising strategy to facilitate the industrialization of biomolecules. However, immobilized systems are now still facing great challenges such as maintaining enzyme activity, large‐scale manufacturing recovery and leaching or conformational changes of enzymes. Therefore, advanced enzyme immobilization techniques (efficient, stable and tunable catalysis) are currently an important challenge in this field. Here, enzyme@cyclodextrin covalent organic framework films are synthesized by template method and further constructed three‐dimensional (3D) hydrogen bond‐enhanced efficient MXene/enzyme membrane reactor. This strategy provides a spacious microenvironment for the release of enzyme molecules, a simpler process, an easier‐to‐etch template, a more biocompatible carrier. Furthermore, a versatile platform for interfacial photothermal and fast mass‐transfer by constructing films with MXene. The obtained biocatalysts have excellent reusability, high activity and stability, which can be used as efficient biocatalysts for important industrial reactions. The enzyme membrane reactor is constructed by the ‘smart capsule ’ with enzyme@cyclodextrin‐COF structure. The strategy can solve the challenging problems of the original previous enzyme immobilization system. Overall, a new idea is provided for the green, efficient, stable and sustainable general enzyme catalytic platform.
Due to the ease of chemisorption of self-assembled molecules on metal oxides, the dipole generation significantly minimizes interface recombination and improves hole extraction at the buried interface in inverted perovskite solar cells. By applying the same technique to the surface of perovskite films to enhance electron extraction and transportation properties, benzamidines are assembled on the surface of perovskite films via a unique host-guest strategy in this study. The ammonium cation, as a guest, interlocks itself in the crown ether's cavity at the crown ether-treated perovskite films. Experimental characterizations and theoretical analyses show that this tightly bound interlocking self-assembles the benzamidine and creates dipole at the perovskite surface, facilitating electron extraction and preventing hole recombination. Consequently, it reduces the perovskite's work function, thus establishing minimal photovoltage and filling factor losses with an efficiency of 25.19%. As analyzed via different theoretical calculations, the strength of this host-guest interlocking even stayed effective in the aqueous solution. Furthermore, the modified devices showed long-term stability under high humidity conditions due to host-guest films' high hydrophobicity.
Although electrochemical technologies offer vast industrial prospects, broader adoption-particularly in consumer applications-remains constrained by high costs and limited component lifespans. Here, we present a gravity-assisted, membrane-free electrochemical oxygen (O2) removal (EOR) reactor coupling oxygen reduction (ORR) and oxygen evolution (OER) reactions. Leveraging fluid mechanics insights, buoyant O2 bubbles ascend rapidly, achieving 95% product self-separation and eliminating the need for membranes or external circulation. To withstand high hydrostatic pressures and ensure a 10-year operational lifespan, we developed an integrative gas diffusion electrode (GDE) with ~85.5% conductivity and 80.2% gas permeability relative to conventional carbon paper, yet 2.2-fold higher mechanical strength and 30-fold greater stability. In a household refrigerator, our two-cell system boosts fresh-keeping capacity by 3.4-fold. Comprehensive economic analysis reveals a 22.6-fold increase in O2 removal per unit cost compared with ion-exchange membrane-based reactors, underscoring this design's cost-effective, long-lived potential for diverse real-world applications.
Continuous Glucose Monitoring (CGM) device was a kind of based on flexible electrode interstitial fluid (ISF) implantation that used electrochemical methods to track blood glucose fluctuations, which made continuous real-time glucose monitoring and personalized blood glucose management increasingly possible. However, when the electrode of CGM in the body fluid environment for a long time, the occurrence of bio-fouling will lead to CGM signal deviation, service life reduction, accuracy decline and other problems. Therefore, in this paper, we constructed a new strategy that provided a well-defined, anti-biofilm coating based and integrated smartphone-controlled wearable microneedle system CGM (acCGM) that can significantly improve accuracy during use and potentially extend service life. In vivo ISF blood glucose monitoring experiment, compared with the commercial blood glucose meter, the acCGM system can accurately monitor the blood glucose level of healthy rats for 21 days. Comparing the two kinds of CGM, it can be found that the MARD of coated CGM within 21 days was 9.69%, and that of uncoated CGM was 16.75%, indicating that the coating had a more obvious anti-biofouling effect. Notably, at 14-21 days after implantation, the MARD of the CGM with the anti-biofouling coating remained at 11.67%, indicating that the acCGM also had the potential to work longer. In addition, the acCGM system with anti-biofouling coating also offered low cost, biosafety, high accuracy and no need for manual calibration.
Precise annealing is vital for achieving high performance in solution-processed PbS quantum-dot (QD) devices, yet conventional methods such as one-variable-at-a-time, full factorial design, and standard machine-learning schemes require large data sets and separate validation steps. Here we report an integrated "search-and-verification" framework that couples ant-colony optimization with hill climbing (ACO-HC) and feeds real-time experimental results back into the algorithm for precise annealing parameter prediction. Starting from a coarse large-spacing factorial design, the ACO-HC method narrows the search space iteratively to 1 degrees C and 1 min resolution without exhaustive screening. Applied to layer-by-layer PbS QD photoconductors, ACO-HC identifies an annealing condition of 109 degrees C for 32 min that boosts responsivity by 265% relative to the unannealed baseline and outperforms the best large-spacing factorial point (110 degrees C, 30 min). Compared with the dense small-spacing full factorial design method, ACO-HC cuts experimental time and material consumption by up to 99%. This universal, scalable strategy provides an efficient route for multiparameter process optimization and holds strong potential to accelerate the development of next-generation solution-processed semiconductor technologies.
Tuning the catalytic pathways of atomically dispersed single-atom catalysts (SAC) has emerged as an effective strategy to optimize their overall catalytic activity. Herein, we present Ru 1 @m-tube, a hollow carbon nitride-supported Ru SAC, coated with eutectic galinstan (GaInSn), as a model catalyst, we demonstrate a performance inversion in vanillin conversion. Vanillin, as a biomass-derived compound with industrial relevance, presents challenges in catalytic hydrogenation, making it an ideal model reaction to test and compare the catalyst's selectivity and efficiency. The as-obtained Ru 1 @m-tube(GaInSn) achieved nearly 100% vanillin conversion within 5 h and exhibited an impressive 93.8% selectivity for vanillyl alcohol. Electron spillover from gallium-based eutectic alloys to highly diluted ruthenium sites enhances the desorption of vanillyl alcohol, resulting in an exceptional performance shift between hydrogenation and hydrodeoxygenation. Our findings not only offer a novel approach for modulating SAC performance via liquid–metal interfaces but also expand the understanding of promoter screening for various challenging reactions.
Diabetic neuropathy reduces patients' ability to sense pressure and respond to stimuli, leading to repetitive injuries and impaired wound healing, often resulting in ulcers. Bacterial infection and the accumulation of reactive oxygen species (ROS) due to hyperglycemia further complicate wound management. To address these challenges, this study developed a multifunctional PDA-PLA@Fe3+@MXene/Ag nanocomposite hydrogel dressing with epidermal sensing, antibacterial, and antioxidant properties. This hydrogel was synthesized by incorporating antimicrobial Ag nanoparticles (Ag NPs) and two-dimensional conductive MXene into a polydopamine (PDA) and polylipoic acid (PLA) hydrogel matrix. The PLA component reacts with ROS to mitigate oxidative stress, creating partial defects that facilitate the release of antibacterial Ag NPs. Consequently, the hydrogel promotes diabetic wound healing by enhancing angiogenesis, collagen deposition, and anti-inflammatory factor expression through its antibacterial and antioxidant properties. Additionally, the hydrogel functions as a sensor capable of monitoring cutaneous pressure, human locomotion, and thermal responses of animals, thus supporting long-term surveillance and therapeutic management of diabetic foot ulcers (DFU). In conclusion, the PDA-PLA@Fe3+@MXene/Ag nanocomposite hydrogel dressing offers a comprehensive approach to diabetic wound management by addressing oxidative stress, bacterial infection, and mechanical sensing.
Lixin Dai (戴立信)合作论文数State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences5