ABSTRACT Natural tendon provides an ideal multilength‐scale network structure design for loading‐bearing soft materials. Despite many recent advances, it remains challenging to fully imitate their multiscale architectures to effectively leverage their collaborative force sharing capacity. Herein, we propose to fuse the chemical microphase separation and mechanical twisting–weaving approaches to devise robust multiscale tendon–mimetic hydrogel structures. First, cosolvent‐induced microphase separation is employed to uniformly disperse the rigid metal‐coordinated poly(acrylamide‐co‐sodium 6‐(3‐(2‐(methacryloyloxy)ethyl)ureido)pyridinecarboxylate) (PA6M) phases into the soft hydrophilic polyurethanes (PU) network. This architecture enables significant energy dissipation through the plastic deformation of hard/soft phases and reversible dissociation of abundant metal coordination and hydrogen‐bonding interactions, yielding enhanced fracture energy (13.7 kJ/m2) and high toughness (28.7 MJ/m3). Second, the mechanical twisting–weaving is developed to transform these tough hydrogels into hydrogel fibers that can be further weaved into 2D/3D hydrogel structures. Such weaving hydrogel structures are found to optimize the distribution of forces to avoid excessive stress concentration for significantly increasing the overall load‐bearing stability, ultimately achieving an effect where the total load‐bearing capacity of the whole woven structure exceeds the sum of the capacities of several individual hydrogel fibers under the tested weaving configuration.
ABSTRACT Discovering non‐noble metal catalysts that can circumvent traditional activity‐stability trade‐off is critical for the development of proton exchange membrane fuel cells (PEMFCs). Incorporating two distinct MNx single‐atom sites into carbon catalysts is emerging as an effective strategy to simultaneously boost activity and stability for oxygen reduction reaction (ORR). Herein, we construct cobalt‐manganese dual‐metal single‐atom catalysts (Co,Mn‐SACs‐CNF) with abundant MnNx sites and CoNx sites anchored on N‐doped carbon frameworks. Detailed characterization studies confirm the co‐existence of isolated Co and Mn atoms in the catalysts. Density functional theory calculations establish that Co single atoms act as the active center during ORR for oxygen adsorption and reduction, whilst Mn single atoms serve as electron donors to regulate the electronic structure of Co sites, thus optimizing the d‐band position of Co sites and favorably tuning the binding energy of oxygen intermediates. Benefitting from the synergistic interaction between nearby Co and Mn atoms, the synthesized Co,Mn‐SACs‐CNF exhibits outstanding stability after 10,000 cycles in 0.5 M H2SO4, whilst delivering comparable ORR activity to the state‐of‐the‐art Pt/C. The stability enhancement is further demonstrated in PEMFC tests, with the device showing a modest (19.6%) loss in initial peak power density after a 30,000‐cycle accelerated stress test.
ABSTRACT Sodium‐ion batteries (SIBs) are promising for low‐temperature applications compared with commercial lithium‐ion batteries, because of the weaker solvation and higher conductivity of Na+ in electrolytes. However, the large size of Na+ leads to slow ionic transport and sluggish reaction kinetics in the electrodes, which is more severe after the lattice shrinks under low temperatures. Herein, a conjugated coordination polymer (CCP) is reported as a cathode for low‐temperature SIBs, by using naphthazarin (DHNQ) as the ligands and Ni2+ as the metal centers. Benefiting from the π‐d conjugation, the Ni‐DHNQ exhibits a high electrical conductivity of 69.7 mS/m and maintains both structural integrity and efficient electron and ion transport even at −40°C. These characteristics collectively enhance the reaction kinetics and cycling stability. The Ni‐DHNQ cathode enables ultrafast charging to 52% state‐of‐charge (SOC) in 90 s and exhibits an ultralow capacity decay rate of 0.0028% per cycle over 5000 cycles. When paired with an organic anode, the pouch full‐cell could reach 87% of its SOC even at −40°C, far higher than the commercial lithium‐ion batteries (12%) and reported alkali‐metal‐ion batteries. This work demonstrates the promise of CCPs for high‐performance sustainable energy storage under extreme conditions.
ABSTRACT Implantable brain‐computer interfaces are undergoing a paradigm shift from rigid silicon architectures to soft, structurally adaptive systems capable of seamless, long‐term integration with neural tissue. Driven by breakthroughs in materials science and micro/nanofabrication, these next‐generation systems achieve unprecedented mechanical compliance, robust interfacial adhesion, and high‐fidelity neural recording. This review comprehensively summarizes the material and structural innovations propelling this evolution. We systematically categorize recent developments by electrode dimensionality: 1D fibers for minimally invasive deep‐brain targeting, 2D flexible arrays for expansive cortical mapping, and 3D microarchitectures for volumetric recording and stimulation. Crucially, we examine the synergy between structural engineering and advanced functional materials such as conductive polymers, carbon nanomaterials, and bio‐derived hydrogels to optimize neural interface and suppressing neuroinflammatory cascades. We further explore how emerging dynamic systems including stimuli‐responsive, self‐healing, and bioresorbable materials impart adaptive functionalities to sustain chronic operation. We also discuss multimodal integration of electrical, optical, and acoustic modalities, as well as ongoing efforts toward miniaturization, standardization, and clinical translation. Finally, we outline future directions toward intelligent, bioresorbable, and AI‐integrated neural interfaces that promise to achieve seamless, bidirectional communication with the human brain.
ABSTRACT Engineering inorganic matrices with optimized photon absorption and interfacial energy transfer is pivotal for advancing laser desorption/ionization mass spectrometry (LDI‐MS) toward high‐fidelity metabolomic analysis. Here, we developed a metal‐organic framework (MOF)‐derived porous iron oxide (pFO) nanomatrix for LDI‐MS‐based metabolomics. The pFO exhibits strong UV absorption at 355 nm, a high specific surface area (59.7 m2/g), and a uniform mesoporous structure, which collectively afford low background noise, enhanced analyte signal intensity, and high analytical reproducibility (coefficient of variation < 9.2%). Using this platform, metabolic fingerprints were rapidly acquired from 269 tobacco leaf samples. Integrated with Random Forest, the approach achieved accurate discrimination of leaf stalk position (AUC = 0.962) and reliable differentiation between southwestern and southeastern production regions (AUC > 0.944). Furthermore, eight representative m/z features were identified to construct a reduced classification panel, which maintained robust predictive performance in the test set (AUC > 0.913). This study establishes MOF‐derived pFO as a high‐performance inorganic matrix for LDI‐MS metabolomics and establishes a rapid and reproducible analytical strategy for digital classification and quality traceability of agricultural products.
ABSTRACT Thermal transfer printing (TTP) offers scalable patterning for electronic textiles, but poor mechanical compatibility and weak adhesion at the conductor–fabric interface often cause failure during deformation and washing. Here we report a TTP strategy that produces mechanically robust and wash‑durable textile electrodes using a dual‑crosslinked conductive composite (DCCC). The composite integrates PEDOT:PSS with sorbitol as a dopant/plasticizer, thermoplastic polyurethane (TPU) as a viscoelastic binder, and (3‐glycidoxypropyl) trimethoxysilane (GOPS) as a coupling crosslinker. GOPS covalently stabilizes the PEDOT:PSS network and chemically links it to TPU, while TPU chains interdiffuse with a hot‑melt adhesive (HMA) during transfer. Simultaneously, molten HMA penetrates textile pores to form mechanical interlocking, enabling strong bonding on diverse fabrics. The resulting electrodes exhibit high adhesion, with peel strength above 900 N/m and lap‐shear strength above 7.85 MPa. During machine washing, the sheet resistance initially decreases because of washing‐induced surface conditioning and then stabilizes, allowing the electrodes to retain electrical performance after 50 standard washing cycles. They also remain stable after 240 days of water immersion and 100 h at 85°C/85% RH, and tolerate repeated bending and abrasion. We demonstrate practical use in motion‑robust wearable ECG monitoring and low‐voltage Joule‑heating textiles for automatic thermal regulation. This work provides a general interface design for reliable, mass‑producible electronic textiles.
ABSTRACT Machine vision systems in real‐world applications require devices capable of adapting to multiple operational modes, including high‐sensitivity photodetection, neuromorphic synaptic behavior, and optical memory. However, integrating these distinct optoelectronic functionalities into a single device presents a challenge due to their conflicting requirements for photoresponse time and retention. Here, a gate‐programmable multifunctional transistor based on a MoS2/MAPbBr3 van der Waals (vdW) heterostructure is fabricated. By using the gate field to tune the interfacial electric field and trapping/release kinetics associated with shallow‐ and deep‐level states, the device can be programmed to operate as a photodetector, synaptic transistor, and gate‐bias‐assisted multilevel optical memory. Under a positive gate voltage (VG), a pronounced photogating effect enables photodetection with responsivity (R) of ∼2397 A/W. At VG = –20 V, the device switches to synaptic mode. At a more negative gate bias, the device enters a gate‐bias‐assisted optical‐memory mode under sustained gate bias. To illustrate the utility of this programmable multifunctionality, frequency‐encoded image recognition is demonstrated with 96.4% accuracy. In addition, a device‐enabled reservoir‐computing (RC) scheme with software‐assisted readout improves classification accuracy by ~20% through deep delay‐based processing. This work demonstrates a multimodal transistor architecture that integrates multiple optoelectronic functions in a single device and suggests a compact hardware route toward adaptive in‐sensor optical information processing.
ABSTRACT Chronic fatigue triggers multi‐system symptoms and cognitive impairments, increasing the risk of cardiovascular and metabolic diseases. Although the electrocardiogram (ECG) offers real‐time, noninvasive detection of physiological abnormalities associated with chronic fatigue, traditional electrodes are susceptible to interference from sweat and motion artifacts, and may cause skin irritation, reducing the accuracy of assessments. Here, we introduce a flexible and long‐term sweat‐resistant ECG acquisition system. By integrating bio‐inspired polydopamine (PDA) hydrogel electrodes with flexible microcircuitry, the system enables unobtrusive, continuous acquisition of heart rate variability (HRV) features for robust fatigue assessment. The developed hydrogel electrode achieves long‐term stability (> 30 days), retaining 90% conductivity after 500 mechanical cycles, and demonstrates over 40% improvement in signal‐to‐noise ratio (SNR) under humid conditions. Its excellent mechanical properties, self‐adhesion, and light transmittance make it suitable for human‐machine interaction, including real‐time monitoring of dynamic motion signals, characteristic pulse waveforms, and handwriting trajectory recognition. Furthermore, by integrating flexible microcircuits and robust deep learning algorithms, fatigue assessment can achieve a recognition accuracy of 88.7% and provide early warnings. Through the synergistic integration of bio‐adhesion, environmental adaptability, and signal fidelity, the flexible biomimetic ECG acquisition sensor provides strong support for personal health risk assessment, early warning, and precise intervention, thereby promoting the intelligent and personalized development of health management.
ABSTRACT Effective monitoring of food spoilage is crucial for global food security, as nearly one‐third of the food produced worldwide each year is wasted and 29% of the population faces nutritional risk. However, existing gas sensing technologies suffer from high material costs, limited sensitivity, and inefficient data transmission. Here, we report a low‐cost electrochemical H 2 S sensor based on a metal‐organic framework‐derived ZrO 2 @C‐900 composite. This active material costs only US$0.09 g −1 , has high sensitivity, and retains 97% of its initial performance after 120 days of continuous operation. This device integrates Bluetooth transmission functionality to monitor H 2 S release in real time as a biomarker of food spoilage. This sensor operates stably under high humidity and low temperature conditions, making it suitable for use in intelligent cold chain systems.
ABSTRACT Low tumor immunogenicity and limited immune‐cell infiltration remain major barriers to effective breast cancer immunotherapy. Although sonodynamic therapy (SDT) offers a noninvasive strategy for deep‐tissue tumor treatment, its efficacy is often restricted by insufficient reactive oxygen species (ROS) generation and the immunosuppressive tumor microenvironment. Here, we report a sonosensitizer‐functionalized polymetallic nanozyme, Pd@PtBi 2 ‐Ce6@HA (PPBCH), as a multifunctional theranostic platform for photoacoustic imaging‐guided sonodynamic cancer immunotherapy. Upon ultrasound (US) activation, PPBCH exhibits catalase‐, peroxidase‐, and glutathione oxidase‐like activities, thereby enabling O 2 generation, ROS amplification, and intracellular glutathione depletion. This coordinated redox disruption induces mitochondrial dysfunction, lipid peroxidation, and GPX4 downregulation, leading to severe oxidative damage, ferroptotic stress, and subsequent immunogenic cell death. PPBCH also elicits canonical hallmarks of immunogenic cell death, including calreticulin exposure, HMGB1 release, and extracellular ATP secretion, thereby promoting dendritic cell maturation and antitumor immune activation. In parallel, the polymetallic framework enables photoacoustic imaging for monitoring tumor accumulation and guiding treatment timing in vivo. More importantly, PPBCH‐mediated SDT remodels the immunosuppressive tumor microenvironment, enhances CD8 + T‐cell infiltration, promotes M1‐like macrophage polarization, and markedly improves the therapeutic efficacy of anti‐PD‐L1 immunotherapy. This work establishes a polymetallic nanozyme strategy that integrates catalytic sonodynamic amplification, imaging‐guided intervention, and immunomodulation for precise cancer immunotherapy.
ABSTRACT Solar‐driven interfacial evaporation has evolved into a sustainable technology with the potential to alleviate the shortage of freshwater resources. Despite remarkable progress in developing photothermal materials, substrates and hybrid configurations, these approaches aimed at improving the evaporation performance appear to have hit a plateau. This limitation can be attributed to the neglect of thermal convection, a critical factor that significantly impacts evaporator performance. Herein, a wood‐based evaporator featuring a dual convection structure was developed by creating a central cavity in a wood block and integrating MXene photothermal materials. It is worth highlighting that the evaporator delivers an exceptional evaporation rate of 2.16 kg/(m2·h) and a photothermal conversion efficiency of 118% without necessitating the use of special materials or intricate architectures. Simulations revealed that the purposely designed dual‐convection structure effectively regulates the heat distribution and reduces the humidity above the evaporation surface, which proved to greatly enhance both the evaporation rate and the overall photothermal conversion efficiency. Furthermore, the device demonstrates good resistance to saline conditions and long‐term operational stability, even under extreme pH conditions. This work provides novel insights into the design of high‐efficiency, structurally simplified solar interfacial evaporators and broadens the potential applications of wood‐based materials in solar‐driven evaporation systems.
Effective monitoring of food spoilage is crucial for global food security, as nearly one-third of the food produced worldwide each year is wasted and 29% of the population faces nutritional risk. However, existing gas sensing technologies suffer from high material costs, limited sensitivity, and inefficient data transmission. Here, we report a low-cost electrochemical H2S sensor based on a metal-organic framework-derived ZrO2@C-900 composite. This active material costs only US$0.09 g-1, has high sensitivity, and retains 97% of its initial performance after 120 days of continuous operation. This device integrates Bluetooth transmission functionality to monitor H2S release in real time as a biomarker of food spoilage. This sensor operates stably under high humidity and low temperature conditions, making it suitable for use in intelligent cold chain systems.
ABSTRACT Mesoporous zinc‐based nanomaterials exhibit considerable potential across a spectrum of applications, yet their controlled synthesis remains challenging due to the rapid hydrolysis and condensation kinetics of Zn2+ ions. Herein, we report a facile surfactant‐directed synthesis strategy for the controllable synthesis of monodisperse mesoporous Zn(OH)2 nanospheres and they can be readily converted into semiconducting mesoporous ZnO (denoted mZnO) nanospheres via calcination. In this synthesis, by employing sodium salicylate (NaSal) as a multifunctional modulator, we regulate micelle organization and zinc precursor diffusion, overcoming the inherent kinetic limitations of Zn2+. The resulting crystalline mZnO can serve as an ideal host for loading ultrasmall Pt nanoclusters to produce Pt/mZnO composite nanospheres with abundant metal–metal oxide interfaces. Using Pt/mZnO nanospheres as the sensitive materials, gas sensors were fabricated on micro‐electromechanical systems (MEMS) devices, which display an exceptional performance in the detection of low‐concentration acetone vapor. The gas sensor exhibited high response (4.9 toward 1 ppm acetone), low detection limit (170 ppb), excellent selectivity, and good long‐term stability. In situ spectroscopy characterization results reveal that, during the gas‐sensing process, the reaction pathway involves catalytic oxidation of acetone over Pt/mZnO nanospheres via intermediate carboxylates. This work offers a generalized approach for designing functional mesoporous metal oxides with enhanced interfacial activity for advanced sensing and catalytic applications.
ABSTRACT The electrocatalytic nitrate reduction reaction (NO3RR) provides a sustainable route for nitrogen pollution remediation and ammonia production under ambient conditions. However, the process involves sluggish multi‐electron/proton transfer and suffers from competing hydrogen evolution (HER) which severely limits efficiency and selectivity. Herein, we construct a Pdx‐CeO2/C composite catalyst, in which strong interactions between Pd and CeO2 induce interfacial electronic redistribution, thereby effectively modulating the Pd electronic structure. This interfacial coupling enhances water dissociation, accelerates the generation of reactive *H, and promotes its spillover from Pd to CeO2. In‐situ attenuated total reflection surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) confirms that hydrogen spillovers facilitate stepwise hydrogenation of intermediates while suppressing HER. Density functional theory calculations further reveal that Pd‐Ce interactions inhibit HER and enable N─O side‐on adsorption, shifting the potential‐determining step and lowering the reaction barrier, thus boosting electrocatalytic activity. As a result, the optimized 5 wt.% Pd‐CeO2/C delivers a Faradaic efficiency of 98.0% for ammonia at −0.4 V (vs. RHE), and achieves an ammonia yield rate of 4.17 mmol/(mgPd∙h) at −0.6 V. This work offers new insights into the application of interfacial engineering for efficient electrocatalytic ammonia synthesis.
ABSTRACT Despite advances in computational catalysis, the complexity of theoretical calculations and specialised expertise requirements limit the broader adoption of catalyst design tools. This work introduces CatPath‐GPT, a mixture‐of‐experts framework that democratizes computational catalyst design by integrating three AI specialists: product prediction (77.2% accuracy), computational planning, and automated code generation through a unified BERT‐based router. Experimental validation through two case studies demonstrates practical impact: systematic screening of CuxZn1−x catalysts identifies optimal compositions for selective CO2RR (Cu75Zn25 for ethanol), while high‐throughput metal oxide screening reproduces Nørskov's classical scaling relationships and identifies high‐activity materials. Benchmarking against GPT‐4 and Mistral‐7B demonstrates superior performance across catalyst‐related tasks, particularly in modeling complex surface reactions. The open‐source framework enables researchers without computational expertise to perform advanced catalyst design, potentially transforming how catalytic materials are discovered and optimized.
ABSTRACT The slow kinetics and high overpotentials of the oxygen evolution reaction (OER) remains a major challenge for electrocatalytic energy conversion. Spin manipulation has emerged as a promising strategy for enhancing OER performance by modulating the adsorption of intermediates, thereby reducing the reaction energy barrier and accelerating OER kinetics. Herein, we demonstrate that chiral nanostructured Pd films (CNPFs) can enhance OER performance. CNPFs were electrodeposited on a nickel foam substrate using methionine as a symmetry‐breaking agent. The optimal CNPFs catalyst achieves a current density of 50 mA∙cm−2 at 1.57 V versus RHE, representing a 180 mV reduction in overpotential compared to achiral Pd films. By varying the electrodeposition time, a series of CNPFs with tunable spin polarization were synthesized. The enhanced OER performance in CNPFs exhibits a positive correlation with spin polarization, primarily due to the spin‐polarized electron transfer promoting the formation of triplet oxygen. This work elucidates the fundamental relationship between spin polarization and OER performance, highlighting the critical role of chiral structure in the design of efficient spin‐polarized electrocatalysts.
