ABSTRACT This work presents the design and fabrication of a conductive dual‐network hydrogel for flexible strain sensing applications. The hydrogel is constructed from two interpenetrating networks: the first formed by hydrogen‐bonded tannic acid (TA) and polyvinyl alcohol (PVA), and the second created via Ca 2+ ‐mediated ionic crosslinking of sodium alginate (SA). Structural characterization by SEM confirms the formation of an integrated dual‐network architecture, where abundant hydroxyl groups in TA synergistically interact with both the PVA network and SA chains, significantly enhancing mechanical toughness and strength. Notably, the resulting SA/PVA/TA hydrogel exhibits strong adhesion to diverse substrates—including iron, glass, plastic, and human skin (e.g., finger joints)—without the need for additional adhesives. Upon immersion in CaCl 2 solution, both tensile strength and electrical conductivity increase with crosslinking time. The hydrogel crosslinked for 30 min achieves a tensile strength of 0.234 MPa and an elongation at break of 126%. Real‐time resistance measurements during mechanical deformation demonstrate a stable and sensitive response to strain, confirming its suitability as a wearable strain sensor. This study thus introduces a simple yet effective strategy for developing adhesive, stretchable, and conductive hydrogels for next‐generation flexible electronics.
Real-time monitoring of charge storage states remains a critical challenge for advanced supercapacitors, particularly in smart and wearable energy devices. Herein, we present a self-reporting heterostructured electrode based on electrochromic metal-organic framework (MOF)-derived ZnCo-S, capable of operando optical tracking of sulfur redox dynamics through reversible color transitions. Although these transitions provide direct visual feedback on the state of charge, the ZnCo-S itself suffers from limited stability during cycling. To address this, we rationally constructed a ZnCo-S@CuFe-LDH heterostructure via potential-controlled electrodeposition, forming covalent metal-oxygen-sulfur (M-O-S) bridges at the interface that significantly enhance structural integrity. This atomic-level integration facilitates rapid electron transfer and synergistic redox coupling, yielding an exceptional specific capacitance of 2704 F g-1 at 1 A g-1-a 20 % improvement over pristine ZnCo-S-along with ultralong cycling stability (99.8 % capacitance retention over 10,000 cycles). A fabricated flexible quasi-solid-state asymmetric supercapacitor achieves a high energy density of 242.4 Wh kg-1 at a power density of 0.8 kW kg-1, while maintaining robust performance under mechanical deformation (30 degrees-180 degrees bending). This work establishes an electrochromism-guided interfacial design paradigm, transforming optical functionality from passive indication to active optimization and paving the way for intelligent energy storage systems with built-in visual monitoring and high electrochemical performance.
To enhance the interfacial charge transfer efficiency of photocatalysts, this study employed 3-aminopropyltrie-thoxysilane (APTES) to modify the surface of ZnIn2S4 (ZIS), which was then coupled with graphitic carbon nitride nanosheets (CNNS) to construct a Z-scheme heterojunction. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that the amino groups of APTES not only strengthened the interfacial adhesion between ZIS and CNNS but also served as bridging sites for electron transfer, effectively facilitating the formation of a Z-scheme charge migration pathway. The optimized composite catalyst exhibited an experimental optical band gap of 2.95 eV (narrower than pure CNNS), a continuous distribution of electronic states near the Fermi level with a theoretical band gap of 1.664 eV calculated by DFT, and significantly improved charge separation efficiency. With the assistance of peroxymonosulfate (PMS), the degradation rate of perfluorobutyric acid (PFBA) reached 97.2% within 90 min, and the apparent kinetic constant reached 35.0 & times; 10-3 min-1,which was 11.67 times higher than that of pure CNNS (3.00 & times; 10-3 min-1). Active species trapping experiments and electron paramagnetic resonance (EPR) tests confirmed that sulfate radicals (SO4-& sdot;) served as the dominant reactive species in the degradation process. Meanwhile, the Techno-economic feasibility analysis was conducted on the application of the APTES-ZnIn2S4/g-C3N4/PMS system in the wastewater degradation of industrial PFBA, demonstrating its excellent industrial application potential for PFBA. This work clarifies the regulatory role of interfacial engineering on the charge behavior in Z-scheme heterojunctions and elucidates the mechanism of synergistic PMS activation for efficient PFBA degradation, providing a new pathway for the green and efficient treatment of perfluoroalkyl substances.
The development of efficient, durable, and scalable oxygen evolution reaction (OER) electrocatalysts is pivotal for industrial green hydrogen production. Here, we report a calcination-free interfacial engineering strategy to fabricate Fe-doped CoOOH (Fe-CoOOH) nanosheets directly on nickel foam through in situ electrochemical restructuring. The resulting catalyst features vertically aligned, microcrack-enriched nanosheets with optimized electronic structure, delivering an ultralow overpotential of 283.7 mV at 100 mA cm-2 and a Tafel slope of 28.2 mV dec-1 in 1 M KOH-surpassing Ni foil. It enables stable operation for over 150 h in a practical anion exchange membrane water electrolyzer (AEMWE). In situ Raman spectroscopic, DFT and XPS analyses reveal that Fe doping promotes the formation of high-valent Co4+ species, weakens O-H bonding, enhances electrical conductivity, and shifts the OER rate-determining step from *OOH formation to a faster surface transformation pathway. This work presents a scalable, energy-efficient route to high-performance, earth-abundant OER electrocatalysts, offering a viable design principle for next-generation industrial water electrolysis.
Tangential flow filtration (TFF) is widely used for high-ratio virus enrichment in wastewater, but the inhibitory effects caused by co-concentrated chemical inhibitors in wastewater concentrates on quantitative polymerase chain reaction (qPCR) quantification remain unclear. In this study, cyanophage PP, bacteriophage phi6, and pepper mild mottle virus (pMMoV) were used to evaluate qPCR inhibition in highly concentrated wastewater produced by TFF. Concentration factors obtained by plaque assay were compared with those measured by quantitative polymerase chain reaction/reverse transcription-quantitative polymerase chain reaction (qPCR/RT-qPCR), and serial dilution regression was applied to assess inhibition. At an approximately 1250-fold volume concentration, the concentration factors measured by qPCR were on average 11.2-fold lower than those measured by plaque assay. When the dilution factor exceeded 16, cycle threshold (Ct) values showed significant linear relationships with dilution, indicating that dilution effectively reduced the inhibitory effects caused by co-concentrated chemical inhibitors in the wastewater concentrate. The concentration factors of PP, Phi6, and pMMoV were further estimated to be underestimated by 5.3-fold, 72.1-fold, and 2.6-fold, respectively, with Phi6 showing the strongest inhibition. These results demonstrate that high-ratio TFF can markedly amplify qPCR inhibition in wastewater, thereby causing virus-dependent underestimation. This study quantitatively reveals this bias in highly TFF-concentrated wastewater and provides a basis for process optimization and result correction in wastewater-based epidemiology
Quasi-two-dimensional (quasi-2D) perovskites are promising for light-emitting and lasing devices due to their strong excitonic properties and quantum-well structures; however, their performance is limited by phase inhomogeneity and defect-related nonradiative losses. Here, we incorporate 3-phosphonopropanoic acid (3-PPA) as an additive into the quasi-2D (PEA)2Csn-1PbnBr3n + 1 film to improve film quality and optical gain characteristics. The 3-PPA-treated films exhibit improved crystallization and significantly inhibit low-dimensional impurity phases. The introduction of 3-PPA extended the fluorescence lifetime to 203.63 ps and accelerated the stimulated emission process, shortening the amplified spontaneous emission (ASE) lifetime to 2.82 ps. Transient absorption and nonlinear optical measurements reveal longer gain lifetimes, enhanced two-photon absorption, and lower saturation intensity, which collectively promote more efficient population inversion. Finally, the quasi-2D perovskite film treated with 3-PPA exhibited stronger emission and a reduced ASE threshold of 2.25 mu J/cm2. This work demonstrates an effective additive engineering approach that enhances the potential of quasi-2D perovskites for efficient low-threshold photonic devices.
Accurate and interpretable estimation of lithium-ion battery state of health (SOH) is essential for ensuring the safety and reliability of energy storage systems. However, existing data-driven approaches often suffer from degraded performance under small-sample conditions and provide limited insight into how predictions are made when processing raw sensor signals. To address these challenges, this paper proposes a novel end-to-end SOH estimation framework that synergistically combines a hybrid iTransformer–BiGRU (Bidirectional Gated Recurrent Unit) architecture, diffusion-based data augmentation, and SHAP (SHapley Additive exPlanations)-guided interpretability analysis. The model takes raw voltage, current, and temperature time-series sequences as direct input, bypassing manual feature engineering. The iTransformer module captures long-range temporal correlations across cycles, while the BiGRU network models local degradation dynamics within each cycle, enabling comprehensive representation learning. To mitigate severe data scarcity—especially in batteries with few aging cycles—a denoising diffusion probabilistic model is employed to synthesize realistic multivariate time-series trajectories, effectively expanding the training set while preserving underlying degradation patterns. The Kepler Optimization Algorithm (KOA) is further integrated to automatically tune key hyperparameters of the prediction network for optimal performance. To enhance transparency, SHAP are applied post-hoc to the trained model, quantifying the relative contribution of each extracted health feature to the final SOH prediction. This provides actionable insights into which degradation-indicative features (e.g., charging time, voltage increment, temperature rise slope) are most influential for health assessment. Experimental validation on the NASA battery dataset demonstrates that the proposed method achieves a mean absolute error (MAE) of 0.0014 (i.e., 0.14% of nominal capacity) and a root mean square error (RMSE) of 0.0018, outperforming several state-of-the-art benchmarks. Ablation studies confirm the effectiveness of both diffusion-based augmentation and the iTransformer–BiGRU backbone, while post-hoc SHAP analysis reveals consistent attention to physically plausible degradation signatures. This work delivers a high-accuracy, data-efficient solution equipped with post-hoc explainability for battery health monitoring under controlled small-sample conditions, as validated on the publicly available NASA 18650 LiCoO₂ dataset.
Abstract Metal–support interactions (MSIs) in supported nanoclusters (NCs) represent a crucial factor in the design of highly efficient heterogeneous catalysts, yet the understanding of these MSIs with their catalytic activities in nature remains elusive. Here, we employ single entity collision electrochemistry to reveal an activity–stability volcano relationship in Au25 NCs for oxygen reduction reaction (ORR) at the single entity level. By in situ identification of current amplitude and duration of individual collision events, we directly correlate MSI strength with ORR activity of single Au25 NCs on five representative supports (C, CeO2, SnO2, TiO2, and Co3O4). Our combined experimental findings and theoretical calculations demonstrate that an intermediate MSI strength provided by SnO2 enables favorable charge transfer without overstabilizing intermediates, thereby affording superior ORR activity of Au25 NCs while preserving adequate anchoring. This study introduces a novel methodological framework for probing MSIs at the single entity level, advancing understanding of metal–support interplay in heterogeneous electrocatalysis.
Engineering the surface electronic structure of Pd-based catalysts is crucial for enhancing ethanol oxidation reaction (EOR) kinetics and durability in alkaline direct ethanol fuel cells. Herein, we report a high-performance PdBi alloy electrocatalyst supported on nitrogen-doped carbon monolith foam (CMF) derived from zeolitic imidazolate framework-8 (ZIF-8) pyrolysis and denoted as Pd3Bi1@CMF. The catalyst exhibits a mass activity of 1920 mA mg(-)(1)Pd-2.8-fold higher than commercial Pd/C-attributed to its high electrochemical surface area (51.2 m(2) g(-)(1)Pd) and uniform dispersion of similar to 5.7 nm nanoparticles. X-ray photoelectron spectroscopy (XPS) confirms Bi-induced downshift of Pd 3d binding energy, weakening COads adsorption, while Bi promotes OH- activation for oxidative removal of intermediates via a bifunctional mechanism. Strong metal-support interaction with N-doped CMF enhances structural stability, enabling 65.6 % activity retention after 300 CV cycles. Rotating disk electrode (RDE) analysis reveals a 5.2-electron transfer pathway, approaching the theoretical five-electron pathway for complete ethanol-to-acetate conversion. This study demonstrates that synergistic modulation of the surface electronic structure through alloying and rational support design offers a powerful strategy for developing advanced, durable, and highly active Pd-based EOR electrocatalysts.
Direct ethanol fuel cells (DEFCs) face significant challenges, including high costs, low electrocatalytic activity, poor long-term stability, and susceptibility to poisoning. To address these issues, we developed Pd@P-rGO catalysts through a two-step process involving high-temperature annealing of phosphorus-doped graphene oxide (P-rGO) followed by Pd reduction using sodium borohydride. The optimized Pd@P3-rGO catalyst demonstrated exceptional performance in alkaline conditions, achieving a mass activity of 2.54 f 0.04 A/mgPd, which is 2.9 times higher than that of commercial Pd/C (0.86 f 0.03 A/mgPd), also significantly outperformed Pd@F3-rGO (0.81 f 0.02 A/mgPd) and Pd@N3-rGO (0.78 f 0.03 A/mgPd). This enhancement is attributed to the increased specific surface area and improved electrical conductivity of the P-rGO support, as well as the electronic structure modulation induced by phosphorus doping. Meanwhile, the rotating disk electrode (RDE) and CO-stripping results proves that Pd@P3-rGO possesses a faster kinetic process of ethanol oxidation and enhanced anti-CO poisoning ability. These findings highlight the potential of phosphorus-doped graphene-supported Pd catalysts as a sustainable and efficient alternative to conventional platinum-based catalysts.
Alloying nanoclusters (NCs) with monoatom doping represents an effective strategy to enhance catalytic performances due to the synergistic interactions between the dopant and host atoms. However, in-depth understanding the position effects of monoatom doping within alloying NCs, particularly at the atomic level, remains elusive. Here, we employed single entity collision electrochemistry method to investigate the electrocatalytic behaviors of individual monoatom-doped bimetallic M1Ag24 (M = Ag, Au, Pt, and Cu) NCs toward oxygen reduction reaction (ORR). By relying on high-resolution and high-throughput electrochemical measurements, we successfully discriminated the effects of monoatom variation in M1Ag24 NCs on ORR activity at the single atom resolution and identified different M1Ag24 NCs across characteristic populations. Our experimental findings and theoretical calculations reveal the electrocatalytic reaction dynamics associated with intracluster migration of Au monoatom during the dynamic alloying process of Au1Ag24 NCs. This work demonstrates a novel approach for in situ identifying the position effects of foreign doping atoms on the electrocatalytic activity of alloy NCs at the single atom level.
Viscoelastic heterogeneity of matrices plays a pivotal role in cancer cell spreading, migration, and metastasis. However, the creation of viscoelastic platforms with spatial-temporal regulation is hindered by cytotoxicity and short regulation durations. Our research presents a dual mechanism for stress relaxation regulation- both intrinsic and responsive- by incorporating Schiff base bonds and a visible light-responsive thiuram disulfide (TDS) moiety into the hydrogel. Modifying base bonds facilitates a broad spectrum of intrinsic stress relaxation times. At the same time, incorporating the visible light-responsive TDS moiety endows the hydrogel with responsive viscoelastic properties. These properties are characterized by minimal cytotoxicity, spatial-temporal controllability, dose dependency, and reversibility. Utilizing this platform, we demonstrate that ovarian cancer cells exhibit contrasting behaviors in contraction and spreading when subjected to dynamic stress relaxation changes over various time periods. Additionally, we observed a “memory effect” in the cell’s response to alterations in stress relaxation time. We can spatially direct cell migration through viscoelastic heterogeneity, achieved via photopatterning substrates and laser spots. This innovative approach provides a means to regulate the viscoelasticity of hydrogels across a wide range of timescales, thereby opening avenues for more advanced studies into how cells interpret and respond to spatiotemporal viscoelastic signals. The viscoelastic properties of a matrix influence the behaviour of cancer cells, but platforms with the required spatial and temporal control over properties is challenging. Here, the authors report a hydrogel combining Schiff base and thiuram disulfide groups for light responsive behaviour and varying stress relaxation.
Efficient, safe, and reliable energy output from high-energy-density lithium metal batteries (LMBs) at all climates is crucial for portable electronic devices operating in complex environments. The performance of corresponding cathodes and lithium (Li) metal anodes, however, faces significant challenges under such demanding conditions. Herein, a nonflammable electrolyte for high-voltage Li||LCO cells has been designed, including partially-fluorinated ethyl 4,4,4-trifluorobutyrate (ETFB) as the key solvent, guided by theoretical calculations. With this ETFB-based electrolyte, Li||LCO cells exhibit enhanced reversible capacities and superior capacity retention at an elevated charge voltage of 4.5 V and a wide operating temperature range spanning from -60 degrees C to 70 degrees C. The cells achieve 67.1% discharge capacity at -60 degrees C, relative to room temperature capacity, and 85.9% 100th-cycle retention at 70 degrees C. The outstanding properties are attributed to the LiF-rich interphases formed in the ETFB-based electrolyte with a finetuned solvation structure, in which the coordination environment in the vicinity of Li+ cations and the distance between anion and solvents are subtly adjusted by introducing ETFB. This solvation structure has been mutually elucidated through joint spectra characterizations and atomistic simulations. This work presents a new strategy for the design of electrolytes to achieve all-climate reliable and safe application of LMBs. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Metal-organic frameworks (MOFs) are promising energy storage materials due to their high specific surface area and tunable structures. However, their practical application is limited by poor conductivity and structural stability. This study proposes a dual-strategy modification combining sulfidation and MnO2 coating to address these issues. A bimetallic Cu-Co-MOF was grown on nickel foam via hydrothermal synthesis, followed by sulfidation to form Cu-Co-S, enhancing conductivity through electron structure optimization. Subsequent rapid electrodeposition of MnO2 created a heterojunction structure, improving structural stability and forming an interfacial electric field to boost electron mobility and ion adsorption. The Cu-Co-S@MnO2 electrode achieved a specific capacitance of 1483.3 F g-1 at 1 A g-1 and retained 93% capacitance after 10 000 cycles. A flexible asymmetric supercapacitor using this electrode retained 88.1% capacitance after 5000 cycles. Additionally, the device achieves an energy density of up to 185.25 Wh kg-1 at high power density of 0.75 kW kg-1. These results highlight the potential of this strategy for developing high-performance, durable energy storage devices for flexible electronics.
Vascular smooth muscle cell (VSMC) phenotypic transition contributes to restenosis, impacting the long-term efficacy of percutaneous coronary intervention in diabetic patients. While DOT1L is known to regulate atherosclerosis, its role in diabetic VSMC phenotypic modulation remains unclear. Using insulin-stimulated rat thoracic aorta VSMCs and a diabetic rat carotid artery balloon injury model, we investigated VSMC proliferation, migration, and collagen synthesis. Histological and molecular analyses were performed to assess vascular remodeling and protein expression. Our findings revealed that 100 nmol/L insulin stimulation for 24 h or 28 days post-injury significantly increased DOT1L and H3K79me1 expression, correlating with VSMC phenotypic changes. DOT1L overexpression upregulated synthetic phenotype proteins in VSMCs and carotid arteries, with a 4.07-fold increase in H3K79me1 at the FGFR4 promoter region, activating the PI3K/AKT/Jag1/Notch1 pathway. These results demonstrate that DOT1L promotes intimal hyperplasia in diabetic vascular injury by mediating VSMC phenotypic switching through H3K79me1-mediated FGFR4 activation and subsequent PI3K/AKT/Jag1/Notch1 signaling.
Mechanical forces play a critical role in regulating cancer cell behavior, particularly during metastasis. Here we present a three-dimensional hydrogel platform embedded with near-infrared-responsive macromolecular actuators that enable precise mechanical stimulation of specific integrin subtypes in cancer cells. By leveraging this system, we investigate how different force parameters-magnitude, frequency, and duration-affect the migration and invasion of ovarian cancer cell spheroids, focusing on the integrins αvβ3 and αvβ6. We find that mechanical stimulation enhances collective invasion at early stages and triggers a mesenchymal-to-amoeboid transition during later migration, especially when high-frequency, large-amplitude forces disrupt αvβ3-ligand interactions. In contrast, cells engaging αvβ6-through higher-affinity binding-show limited transition under similar conditions. Molecular simulations support these findings by revealing the underlying mechanics of integrin-specific responses. This 3D hydrogel platform provides a powerful tool for studying mechanotransduction in cancer cells and offers potential insights for developing targeted cancer therapies.