Metal-doped carbonized polymer dots (CPDs) have shown remarkable potential for serving as nanozymes to mimic the catalytic performance of natural enzymes. However, systematic strategies for constructing metaldoped CPDs nanozymes with different skeletons and revealing the role of surface functional groups that influence peroxidase-like (POD-like) catalytic activity remain limited. Herein, CPDs-Fe with three kinds of skeletons (IE-Fe, TE-Fe, and TM-Fe) were prepared to explore POD-like catalytic activity. The intrinsic POD-like activities of the three CPDs-Fe were examined by catalytic oxidation of 3, 3 ', 5, 5 '-tetramethylbenzidine (TMB) with hydrogen peroxide (H2O2). The results showed that the performances of the three CPDs-Fe were superior to those of natural horseradish peroxidase (HRP) and other mimetic peroxidases. Notably, the POD-like activity of TE-Fe was better than that of IE-Fe and TM-Fe. TE-Fe was further applied to the photocatalytic degradation of malachite green (MG) and neutral red (NR), and the removal rates of both dyes had reached over 90 %. This study provides a new strategy for constructing metal-doped CPDs nanozymes with enhanced POD-like activity and highlights their potential for environmental remediation.
Polyetheretherketone (PEEK) has been regarded as a prospective alternative orthopedic implant, because of its elastic modulus approximately equal to human cortical bone. However, the poor antibacterial and angiogenic properties of bioinert PEEK have become a limitation to its clinical application. Therefore, a biomimetic metal organic framework acid-controlled release nanocarrier consisting of Zeolitic Imidazolate Framework-8 (ZIF-8) nanoparticles loaded with gentamicin and modified with silk fibroin nanospheres for PEEK implants is prepared. In this study, acidity-responsive PEEK implant can efficiently capture bacteria and eradicate bacterial biofilms, achieving antibacterial rates up to 99.9% against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). Furthermore, acidity-responsive PEEK implant is expected to promote angiogenesis by assisting proliferation and migration of endothelial cells, thereby accelerating peri-implant tissue regeneration. By constructing subcutaneous infection models, it is further indicated that acidity-responsive implant can resist bacterial proliferation and facilitate peri-implant angiogenesis. In summary, this study provided an effective approach for the improvement of orthopedic implants that realized antibacterial and angiogenic effects, offering a potential solution for preventing infection and promoting angiogenesis during the early phase after implantation.
Hydrogels have attracted considerable attention for electromagnetic interference (EMI) shielding applications. However, their practical use is often limited by insufficient mechanical robustness and poor self-healing performance. Herein, a simple and effective strategy is reported to fabricate a self-healing EMI shielding hydrogel composed of 2-phenyl-1H-indole-3-carbaldehyde (PICA)-grafted polyvinyl alcohol (PVA) (denoted as PVA-PICA) and Ti3C2Tx MXene nanosheets, crosslinked with borax and Fe3+. The as-prepared hydrogel exhibits excellent mechanical properties and rapid self-healing capability, which are attributed to the steric hindrance effect of bulky 2-phenylindole side groups and the formation of multiple dynamic bonds. Benefiting from the synergistic interactions among ions, MXene nanosheets, water molecules and the porous network structure, the as-prepared hydrogel achieves a maximum EMI shielding effectiveness (SE) of 57.6 dB in the X-band at the frequency of 8.2 GHz. Notably, the EMI SE can be reversibly switched between on and off states through repeated wetting-drying cycles. This work provides a promising strategy for the development of self-healing EMI shielding hydrogels for next-generation flexible and wearable electronics.
Magnetic microwave absorption materials are widely applied in electromagnetic compatibility, national defense stealth, environmental protection, and other fields, serving as key materials to address the challenges posed by modern electromagnetic environments. However, the self-aggregation phenomenon of magnetic nanoparticles significantly limits further enhancement of their performance in electromagnetic wave absorption. To address this issue, this study proposes a preparation strategy for the controllable dispersion of magnetic nano-units. A core-shell carbon nanofibers (CNFs)-Fe3O4@MXene composite material was successfully fabricated using electrospinning technology, enabling the micro-scale controllable dispersion of magnetic nano-units, manifested as long-range isolation, short-range dispersion, and close packing. By simply adjusting the loading number of magnetic nano-units, different levels of magnetic loss can be regulated, thereby optimizing the microwave absorption performance of the composite material. Under conditions of 4 wt.% Fe3O4 filler and a 1.5 mm film thickness, the CNF-Fe3O4@MXene composite material achieved a high reflection loss (RL) of -70.87 dB and a wide effective absorption bandwidth (EAB) of 6.56 GHz. Additionally, radar cross-section (RCS) simulations confirmed the stealth performance of the composite material in real-world environments. Electromagnetic simulations further revealed the microscopic loss mechanisms responsible for the superior microwave absorption properties of CNF-Fe3O4@MXene. This study provides novel insights and strategies for the design and optimization of magnetic microwave absorption materials.
Superamphiphobic coatings have emerged as a solution to the traditional challenges of surface adhesion, contamination, corrosion, and liquid repellency. These coatings endow substrates with resistance to various types of fluids, such as water and oil, and represent a key technology for developing a new generation of “maintenance-free” self-cleaning surfaces. In this study, a series of multifunctional composite coatings (PPS/POS@Al2O3/ADP) featuring a rough microstructure and low-surface-energy functional groups were fabricated via the synergistic effect of polysiloxane-coated alumina nanoparticles (POS@Al2O3), polyphenylene sulfide (PPS), and an aluminum dihydrogen phosphate binder (ADP). The coating exhibits excellent superamphiphobicity toward liquids of different surface tensions and maintains stable superamphiphobicity on a broad range of substrates, including metals and ceramics. Specifically, this coating significantly delays the icing process and prolongs the complete freezing time of contaminated water droplets on the coated surface. This study provides an effective strategy for developing high-performance coatings that integrate superamphiphobicity, robust mechanical durability, and delayed icing properties. Such coatings show promising applications in anti-corrosion, self-cleaning, and anti-icing fields.
Engineering strategies to enhance plasmonic effects in photocatalysis usually focus on nanostructure design. However, the systematic relationship between surface plasmon resonance (SPR) characteristics and catalytic activity, particularly with respect to ordered structures, remains underexplored. This study focuses on three types of Au(Ag)-TiO2-based heterogeneous periodic structures-films, nanoholes, and nanocones-spanning from 2D to 3D systems, aiming at systematically elucidating how the plasmon resonance mode and intensity affect photocatalytic degradation. The results show that Ag-TiO2 nanocones exhibit the strongest photocatalytic performance for MB molecules, whereas Au-TiO2 nanocones are more effective for CV molecules. Our understanding of plasmonic resonance has been further deepened by discussing it in the context of two key mechanisms: plasmonic resonance energy transfer (PRET) and hot-electron transfer (HET). As the plasmonic resonance intensity diminishes with morphological adjustments, photocatalytic performance decreases accordingly. Enhancement differences between metals and molecules originate from tuning the degree of overlap between the designed plasmonic resonance band and the absorption band of dye molecules. Femtosecond transient absorption spectroscopy (fs-TA) reveals that, within materials of different morphologies but the same metal, strong plasmonic effects extend the hot electron lifetime through electron-phonon (e-p) scattering, effectively suppressing charge carrier recombination and minimizing non-reactive energy loss through phonon-phonon (p-p) scattering. This efficiently facilitates carrier generation, accelerates energy transfer, and enhances the yield of reactive oxygen species. Therefore, this study provides theoretical guidance for the design of ordered structural models influenced by hot carrier dynamics, enabling the development of efficient photocatalytic systems.
Stable organic radicals with unique luminescence have demonstrated great importance in photoelectromagnetic materials and have found broad applicability in the field of organic light-emitting diode (OLEDs). Aiming to further extend their application into chiral optoelectronic devices, by employing topologically chiral [2]catenane as the key chiral skeleton, this work presents the first successful construction of circularly polarized OLEDs (CP-OLEDs) based on donor-acceptor (D-A•) type neutral tris(2,4,6-trichlorophenyl)methyl (TTM) radicals. Remarkably, the topologically chiral skeleton, in combination with its controllable dynamic features, enables the system to exhibit a luminescence dissymmetry factor (|gPL|) value as high as 7.1 × 10-3, as well as reversible circularly polarized luminescence (CPL) on/off switching in film state. Importantly, the resulting CP-OLEDs exhibit deep red emission, a maximum external quantum efficiency (EQEmax) of 3.92%, and a |gEL| value of 7.2 × 10-3. These findings demonstrate the successful development of not only luminescent radicals with unique switchable CPL performances, but also the first CP-OLEDs with promising device performance based on topologically chiral radical emitter, providing a distinctive design principle and a versatile platform for the creation of next-generation smart CP-OLEDs.
Petroleum-contaminated wastewater and industrial effluents are increasingly threatening ecosystem. Aerogels possess immense potential for oil-water separation with their porous structure and high porosity. However, the inherent brittleness of conventional aerogels severely limits their practical utility under demanding conditions. Nanofiber aerogels (NFA) present a compelling alternative by integrating mechanical flexibility with a resilient 3D porous network. Inspired by the reversible water uptake and loss in plant cells, a superhydrophobic poly ether ether ketone (PEEK) nanofiber aerogel (Si@PEEK NFA) with a three-dimensional (3D) hierarchical cellular structure was constructed through directional freeze-drying and cross-linking. The biomimetic 3D hierarchical cellular structure exhibited exceptional compressive strength, achieved 1.1 MPa compressive stress (8 = 80%) and 80% retention after 100 cycles (8 = 50%). Notably, the Si@PEEK NFA retained stable and durable mechanical properties even in high-temperature solvent. Through hydrolysis-polymerization of methyltrichlorosilane (MTCS), lotus leaf-like nipple structure was constructed on PEEK NFA surface, which conferred excellent organic solvent absorption capacity and recyclability (94% retention after 20 cycles). Simultaneously, Si@PEEK NFA exhibited outstanding emulsion separation capabilities at both ambient and high-temperature, achieved nonane emulsion flux of 6970 L m- 2 h-1 (room temperature) and 8200 L m-2 h-1 (90 degrees C), with separation efficiency both exceeding 99%. This work provides an effective strategy for the fabrication of mechanically robust nanofiber aerogels for emulsion separation under harsh condition.
Selective photocatalytic oxidation of methane to value-added C1 oxygenates under mild conditions is attractive but remains limited by poor control over branching selectivity, because methanol and formaldehyde share closely related energetics and pathways. Here we demonstrate programmable selectivity in methane photooxidation by steering the dominant type of photogenerated charge carriers at metal/boron nitride (BN) interfaces. Carrier enrichment at the active sites dictates the hydrogen-transfer steps that govern the fate of a common hydroxymethyl intermediate, enabling selective switching between methanol and formaldehyde. We propose that electron-enriched AuNPs/BN facilitates hydroxymethyl intermediate hydrogenation to methanol, whereas hole-accumulating PdSA/BN promotes hydroxymethyl intermediate dehydrogenation to formaldehyde. Under atmospheric pressure, PdSA/BN gives formaldehyde with ~90% selectivity and generation rate of 1653.75 μmol·g−1·h−1, while AuNPs/BN achieves ~92% selective methanol production at 1070.17 μmol·g−1·h−1. Here, we show that establishing carrier-polarity programming at heterogeneous interfaces as a general strategy to control branching selectivity in photocatalytic C-H oxidation. Charge-carrier enrichment at active sites enable type-dependent product selectivity in methane photooxidation: electron-enriched AuNPs/BN favors methanol selectivity ( ~ 92%), while hole-enriched PdSA/BN favors formaldehyde selectivity ( ~ 90%).
Piezoelectric materials are pivotal to sensors, actuators, and energy harvesting technologies. However, their advancement is impeded by the brittleness and biotoxicity of inorganic piezoelectric ceramics, the low piezoelectric response of piezoelectric polymers, incompatible heterogeneous interfaces in piezoelectric composites and the bio-inertness of piezoelectric single crystal surfaces. Polydopamine (PDA), a mussel-inspired biopolymer, offers a universal strategy to address these interfacial challenges. This review systematically elucidates how PDA, as an interfacial modifier, enhances piezoelectric system performance. It explores PDA's key mechanisms involving modulating the arrangement of piezoelectric polymer chains via interfacial interactions, strengthening the interfacial coupling between inorganic piezoelectric fillers and piezoelectric polymer matrices in heterogeneous composites, and constructing functionalized platforms using its surface rich in active functional groups. Furthermore, this review summarizes application examples of PDA modified piezoelectric materials in frontier fields. Furthermore, it discusses the challenges and limitations encountered during actual usage. This review aims to provide valuable insights for the further optimization and design of PDA in the interface engineering of piezoelectric materials.
Pyrolytic carbon black (CBp) and graphene oxide (GO) are commonly used to reinforce polymer matrices; however, their tendency to agglomerate limits composite performance. Conventional dual filler systems are frequently costly and challenging to scale. We exploited synergistic CBp-GO interactions to suppress agglomeration and establish a stable filler network, thereby improving the mechanical and electrical properties of natural rubber (NR) composites. Composites were prepared by blending CBp (40 phr) with GO at 0-8 phr. Filler dispersion was characterized by scanning electron microscopy and a carbon black dispersibility tester. Mechanical, vulcanization, and electrical properties were measured. At an optimal CBp/GO ratio of 40:4, a continuous filler network formed, reducing volume resistivity by eight orders of magnitude relative to CBp-only composites and by three orders relative to composites containing 2 phr GO. The 300% modulus increased by 18.3%, and the electrical percolation threshold decreased by 22%. Excess GO (>4 phr) induced agglomeration and reduced tensile strength by 16.4%. A key innovation is the use of CBp in constructing a low-cost multi-filler system that suppresses GO agglomeration without chemical modification. This approach provides a sustainable route to producing highperformance rubber composites and promotes the recycling of waste rubber.
By adopting a hydrothermal-sulfidation stepwise optimization strategy, nickel-vanadium sulfide (NiV-S) composite electrodes with hierarchical interwoven porous structures and bimetallic synergistic effects were successfully constructed in situ on nickel foam substrates. The synergistic regulation of material properties by Ni/V molar ratio, hydrothermal time, and sulfidation degree was systematically investigated, and optimal performance was achieved at Ni/V = 1:0.3, hydrothermal time of 12 h, and S/Ni = 0.8, showing a superior specific capacitance of 3732.9 F g(-1) at 1 A g(-1), along with outstanding rate performance and cycling stability (70.1% capacity retention after 5000 cycles). The assembled asymmetric supercapacitor achieved an energy density of 105.4 Wh kg(-1) at a power density of 800 W kg(-1), maintaining 67.1 Wh kg(-1) even at a high power density of 15,997.4 W kg(-1). Compositional and structural characterizations revealed that moderate sulfidation resulted in the formation of a NiV2S4/Ni9S8 multiphase composite. Concurrently, an ultra-thin nanosheet-interwoven threedimensional multi-level pore network was formed, significantly increasing specific surface area and active site exposure. X-ray photoelectron spectroscopic analysis confirmed the presence of Ni2+/Ni3+ and V4+/V5+ multivalent systems within the material, with sulfur introduction significantly enhancing electrical conductivity. This study elucidates how sulfurization enhances electrode performance through regulation of microstructure, electrical properties, and valence composition, providing an effective strategy for designing high-performance supercapacitor electrode materials.
Over the past decade, metasurfaces have undergone substantial advancements, facilitating the development of compact and integrated electromagnetic devices. Recently, bound state in the continuum (BIC) has garnered considerable interest due to its exceptionally high quality factors and pronounced electromagnetic field confinement. In this study, we propose a dual-band terahertz modulator by integrating aluminum rectangular aperture array with the phase-change material Ge2Sb2Te5 (GST), employing both numerical simulations and experimental validation. The hybrid metasurface supports a BIC mode and a single resonant peak in the terahertz transmission spectrum. Importantly, the disruption of structural symmetry through geometric parameter modification converts the BIC into a quasi-BIC (QBIC), causing the original single peak to split into two distinct peaks. Moreover, the phase transition of GST from its amorphous to crystalline state induces a substantial modulation of the transmission amplitudes of these two resonant peaks, attributable to the enhanced conductivity of GST. Experimentally, maximum modulation efficiencies of 90.6 % and 91.6 % were achieved at frequencies of 0.5 THz and 0.79 THz, respectively. This hybrid phase-change metasurface demonstrates significant potential for applications in terahertz modulators, filters, and related devices.
Efficient and selective ultra-low-temperature (<150 °C) NH3-SCR for NOx abatement in non-power industry is highly significant yet remains challenging due to sluggish reaction kinetics and inferior N2 selectivity. Herein, a photothermal catalytic strategy was developed by tailoring a Cu-doped SmMn2O5 (Cu-SMOM4R) catalyst, leveraging its high-efficiency photothermal conversion capability. Acid etching selectively removed surface Sm atoms, thus increasing the Mn4+/Mn3+ ratio to enhance surface acidity and redox capacity. Cu doping created coordination-unsaturated structures at Mn3+ sites, which enabled the selective activation of NO to nitrite (NO2−) species, thereby driving a highly efficient and selective photothermal SCR reaction. The optimized catalyst achieved 98.1% NOx conversion and 98.6% N2 selectivity at 90 °C under 1.2 W/cm2 irradiation, with excellent 144-h stability. Comprehensive characterizations confirm that the Mn4+-O-Cu2+ dual-functional active sites in Cu-SMOM4R not only provide more L-acid sites for NH3 adsorption but also modulate NO activation states to accelerate the reaction efficiency through both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. This study establishes photothermal catalysis as an energy-efficient platform for industrial NOx control under challenging ultra-low-temperature conditions.
Lightweight, environmentally resistant electromagnetic shielding materials are critical for aerospace and military applications. Constructing multi-layer conductive network structure offers an effective pathway to achieve high-performance electromagnetic interference (EMI) shielding. In this work, we developed a lightweight fiber-reinforced composite paper that delivered ultra-high EMI shielding performance (SE) even under harsh conditions. A three-dimensional conductive network was formed by the controlled incorporation of Cu@PEEK fibers and carbon fibers (CFs) into a carbon nanotubes (CNTs)/PEEK fiber matrix. Experimental results revealed remarkable synergistic effects among the multi-scale fibers, endowing the composite paper with an exceptional EMI shielding effectiveness of 54.4 dB at an ultra-thin thickness of 0.3 mm (12 GHz). Furthermore, the stability of the EMI shielding performance was evaluated under extreme temperatures and near-infrared high-power laser irradiation. The composite paper retains over 80% of its shielding effectiveness, demonstrating the potential for application in complex environments. This work provides valuable insights for designing high-stability EMI shielding materials suited for extreme operational environments.
The S-scheme heterojunction has excellent light utilization efficiency, charge separation efficiency and redox capability, and shows high application potential in the field of photocatalytic antibacterial. This study successfully synthesized the TPTh/TP-PCN S-scheme heterojunction composed of carboxyl-functionalized thiophene-based conjugated polymer (TPTh) and fragmented carbon nitride (TP-PCN), significantly improving the photocatalytic antibacterial performance. Among them, the composite material TPTh-7/TP-PCN can achieve 100% elimination of 107cfu/mL methicillin-resistant Staphylococcus aureus (MRSA) within 60 s under visible light irradiation, reaching the cutting-edge level of global photocatalytic antibacterial efficiency. This outstanding antibacterial effect is not only attributed to the S-scheme heterojunction structure between TPTh and TP-PCN, but also benefits from the it-it stacking interaction, which enhances carrier efficiency and strengthens the capture effect of surface functional groups on bacteria. Further in vitro and in vivo experiments also confirmed that TPTh-7/TP-PCN can promote angiogenesis and wound healing, while inhibiting inflammatory responses. In conclusion, the TPTh-7/TP-PCN type ultra-high-efficiency organic-inorganic S-scheme heterojunction photo-catalyst has great development potential, providing strong support for the design and preparation of such materials, and also offering assistance in preventing wound infections and promoting wound healing.
Persulft-based advanced oxidation processes (PS-AOPs) are an efficient strategy to degrade refractory pollutants. Fabricating a highly efficient catalyst is the most pivotal factor in PS activation. This study designs a novel CoP3-anchored layered Bi2O2S through an interface engineering strategy, where the unique electronic structure and surface properties of Bi2O2S lead to dramatically reduced cobalt ion leaching compared with that of CoP3. It exhibited outstanding catalytic activity and achieved nearly complete removal (>99%) of 50 mg L-1 2,4-Dichlorophenol (2,4-DCP) within 30 min. Radical quenching experiments, EPR technique, electrochemical tests, and HPLC validated the coexistence of radical (center dot OH, SO4 center dot-) and non-radical (O-1(2), electron transfer, high-valent metal species) pathways in the Light/Bi2O2S/CoP3/PMS system for 2,4-DCP degradation. Importantly, Bi2O2S/CoP3 induced a pronounced photothermal effect that enhanced 2,4-DCP degradation efficiency. Furthermore, the attack sites of 2,4-DCP were precisely identified based on the Fukui index. Based on density functional theory calculation and high-performance liquid chromatography-mass spectrometry, the detailed degradation pathways were proposed. The toxicity of 2,4-DCP and its intermediate products were predicted by using the toxicity assessment software tool. Moreover, excellent reusability, real-water treatment efficacy (verified by 3D-EEM), high-efficiency removal of multiple pollutants, and wide pH adaptability (3-11) confirm practical potential for sewage treatment. This study provides insight into designing a highly efficient and green catalyst for simultaneous pollutant treatment.
Supercapacitors are a new type of energy storage device with broad application prospects in fields such as new energy vehicles and portable electronics, thanks to their high power density and long cycle life. Three components make up supercapacitors: electrodes, electrolyte, and separator material. These elements determine the performance characteristics of the material. Due to its designable chemical structure, excellent mechanical flexibility, good electrolyte compatibility, and controllable porous structure, polyurethane emerges as an ideal candidate material for core components in supercapacitors. This review explores the performance characteristics and potential advantages of polyurethane and its derivatives in supercapacitors. It summarizes strategies for regulating the mechanical and conductive properties of polyurethane and its derivatives, and discusses the latest research on applications of polyurethane in supercapacitor electrodes, electrolytes and separators. Moving beyond the single-component perspective, this review provides a comprehensive examination of the multifunctional role of polyurethane in supercapacitor electrodes, electrolytes, separators, and integrated devices. devices. It also analyses the intrinsic relationship between structure, performance, and application. Finally, it summarizes the challenges and future development directions for the development of polyurethane-based supercapacitors, providing new insights for developing next-generation supercapacitor electrodes with high energy density, a long cycle life, environmental adaptability, and intelligent functionality.
Photoelectrochemical (PEC) water splitting represents a promising technology for converting solar energy into chemical fuels, offering a sustainable pathway to address the growing global energy demand and environmental challenges associated with fossil fuels. However, the widespread industrialization of PEC systems is hindered by inherent limitations of semiconductors, such as rapid charge recombination and sluggish surface reaction kinetics. In response, surface and interface engineering has emerged as a highly effective strategy to boost PEC performance by modifying photoelectrodes with functional materials. Among these, metal-organic frameworks (MOFs) have garnered significant attention due to their tunable band gaps, high density of active sites, exceptional catalytic activity, and porous structures that facilitate mass transport. In this review, we present comprehensively summarizes recent advances in the synthesis strategies for growing MOFs on photoelectrodes and elucidates their multifaceted roles in surface/interface engineering, including serving as passivation layers, cocatalysts, and heterojunction components. Finally, we provides a critical perspective on the current challenges and future opportunities in harnessing MOFs for high-performance PEC water splitting.
Ruren Xu (徐如人)合作论文数College of Chemistry, Jllin University20