共找到 20 条结果
This study developed and validated a non-invasive multi-metabolite magnetic resonance spectroscopy framework for preoperative molecular subtyping of adult diffuse gliomas. Using a cross-center, cross-vendor cohort of 268 patients, 48 features derived from 18 metabolites were systematically evaluated to identify discriminative metabolic signatures for predicting IDH mutation and 1p/19q codeletion status. The integrated metabolic model showed robust intra-center and cross-center performance for IDH prediction, with AUCs of 0.906 and 0.857, respectively, and for 1p/19q prediction, with AUCs of 0.858 and 0.787, respectively. These results suggest that synergistic metabolic profiling support molecular assessment in patients who may not be suitable for invasive biopsy.
Photothermal-enhanced photocatalytic hydrogen evolution (PHE) converts nonradiative losses into localized interfacial heating, while precious-metal single-atom catalysts (SACs) offer atom-efficient and well-defined active sites. However, progress remains difficult to compare and translate because reaction-zone temperatures are often poorly constrained, the active forms of single atoms under light and heat are rarely verified, and performance in model suspensions does not readily extend to practical reactors or long-term operation. This Review summarizes major material platforms for photothermal harvesting and single-atom site design, and defines key support requirements, including strong light absorption, efficient charge and heat transport, and stable anchoring sites. It also outlines the typical roles of different noble metals and proposes actionable frameworks for the field. Thermometry-anchored protocols help disentangle thermal, photochemical, and synergistic effects through temperature-matched controls, absorption-normalized kinetics, and activation-energy benchmarks. An operando and ultrafast evidence framework tracks coordination, valence, charge transfer, and intermediates in real time, enabling verification of dynamic active sites. Finally, scale-relevant design rules connect photon and heat management with mass transport, bubble dynamics, scalable synthesis, and long-term validation, guiding photocatalysis toward mechanistically accountable and deployable solar H2 production.
Covalent organic framework (COF) membranes with high crystallinity hold great promise in precise molecular separation, but often suffer from the intercrystalline defects and thus poor membrane-formation ability. This study reports a sequential imine exchange strategy to fabricate highly crystalline, defect-free COF membranes for precise molecular separation. Two functional amines (aromatic and aliphatic amines) are employed in highly reversible imine exchange reaction to separately conduct crystallization and defect remedy processes according to their different energy gaps. Aromatic amine, which serves as COF framework building unit, undergoes the first-step imine exchange for high crystallinity because of its lower energy gap. Afterward, the hyperbranched aliphatic amine with abundant amino groups undergoes the second-step imine exchange, affording the tight connections between adjacent crystals and the excellent membrane-formation ability. Accordingly, the COF membrane exhibits high permeance (344 L m-2 h-1 bar-1 for water, 462 L m-2 h-1 bar-1 for methanol) and rejection (> 99.9% for Congo red and Alcian blue). Meanwhile, the membrane is endowed with an ultrahigh separation factor (> 528) for mixed dye aqueous solutions and large-scale processability (> 290 cm2). This work offers a new strategy to fabricate highly crystalline and defect-free COF membranes, revealing their large potential in diverse practical applications.
Solar interfacial evaporation has undergone rapid development in recent years, yet its overall performance has reached a plateau due to limited advances in solar-thermal materials. Herein, we propose a synergistic nano-confinement and physical-field-modulation strategy that enables concurrent acceleration of solar-driven evaporation of water and on-site remediation of organic pollutants. Implemented in hollow mesoporous carbon nanocages integrated with Fe-N4 catalytic sites and inner wall plasmonic Au nanoparticles, the system couples mesoporous confinement with localized thermal and pressure perturbations to transform bulk water into thermodynamically activated intermediate states and substantially reduce the effective vaporization enthalpy. This integrated framework delivers high evaporation rates of 2.56 kg m-2 h-1 in planar devices and 6.84 kg m-2 h-1 in 3D architectures under one-sun irradiation, with a kinetic enhanced Hertz-Knudsen-Schrage-derived evaporation coefficient. Simultaneously, the Fe-N4 sites enable non-radical peroxymonosulfate activation for ultrafast degradation of bisphenol A, achieving a rate of 182.5 L g-1 min-1. This work establishes an ingenious strategy for coupling water-state regulation and catalytic pollutant degradation to break the performance bottleneck of solar-thermal purification.
Ovonic threshold switching selectors are indispensable for suppressing sneak currents in dense cross-point memories, but most established selector materials still rely on multicomponent chalcogenides with persistent trade-offs in leakage current, reliability, and compositional stability. Recent progress in elemental switching materials is beginning to change this picture. A new study identifies amorphous selenium as a highly effective selector, combining an ultralow leakage current of 4 × 10-12 A, an on/off ratio above 108, a drive current density of 21.2 MA cm-2, nanosecond-scale switching, and endurance up to 2 × 109 cycles. More importantly, spectroscopy and theory connect these metrics to a charge-triggered mechanism rooted in dense trap pairs in the amorphous network. These states strongly pin the Fermi level in the off-state, while field-induced carrier release near threshold drives abrupt conduction. Beyond introducing a new selector material, this work suggests that monatomic chalcogens may provide a cleaner platform for understanding and engineering threshold switching, with fewer complications from phase segregation, cation migration, and chemical overdesign.
Simultaneously achieving mechanical robustness and autonomous self-healing in ionogels remains a fundamental challenge for durable, skin-like electronics. Conventional approaches often improve mechanical strength by introducing rigid or densely cross-linked polymer networks, but such strategies inevitably restrict polymer chain mobility and hinder dynamic bond reconfiguration required for healing. Here, a zwitterionic side-chain engineered tough ionogel (ZESTI) is developed to overcome this trade-off through molecular-level design. Hydrophilic zwitterions are covalently grafted onto a hydrophobic polyurethane backbone to preferentially interact with the ionic liquid through ion-dipole interactions and thereby regulate its distribution. This architecture simultaneously facilitates dipole-dipole interactions for mechanical reinforcement and ion-dipole coordination for efficient self-healing under ambient conditions. As a result, ZESTI exhibits an exceptional combination of tensile strength (10.40 MPa), stretchability (1606%), toughness (56.03 MJ m-3), and ambient self-healing efficiency exceeding 83%, while maintaining high ionic conductivity via enhanced ion hopping. When constructed as a self-reporting packaging interface, ZESTI provides stable protection and state perception under sharp contact and restores signal output after mechanical damage through self-healing. This work offers a generalizable design strategy that reconciles mechanical toughness with dynamic functionality in ionogels, establishing a general design paradigm for next-generation self-sustaining iontronic devices.
Aqueous zinc-iodine batteries (AZIBs) show promise for grid-scale energy storage, but they are hampered by polyiodide shuttling, sluggish iodine redox kinetics, and irreversible active-site poisoning caused by uncontrolled adsorption. We provide a comprehensive screening of M1 (M1 = P, S, B) heteroatom dopants, and P is identified as the best candidate for achieving coordination-tuned, moderate adsorption that balances adsorption and catalytic activity while mitigating site poisoning. Using phytic acid as both the P source and an etchant, we create a universal in situ approach to core-shell single-atom catalysts (M2-P-CSNC, M2 = Fe, Co, Ni). The unique core-shell structure achieves stable confinement of polyiodides, rapid ion transport, and protection of active sites, while in situ P doping precisely regulates the local electronic environment and d-band center of the Fe-Nx active centers. In situ characterization confirms that Fe-P-CSNC has a strong reversible anchoring ability for polyiodides, which can significantly accelerate redox kinetics. The optimized Fe-P-CSNC/I2 exhibits almost no capacity decay after 20,000 cycles at a current density of 2 A g-1. This work's facile heteroatom doping strategy for electronic modulation offers a reference for high-performance catalyst design in conversion-type energy storage systems. Kindly check and confirm the edit made in the title.1. We have checked and confirmed the edited title. 2. We found some issues with Figure 3d and have uploaded the revised image as an attachment.
In the ongoing pursuit of energy-dense lithium-ion batteries (LIBs), Li-rich layered oxide (LLO) cathodes provide an attractive path forward with extraordinary capacity delivery and low raw material cost. However, the surface-originated degradations and local structure rearrangement incur severe capacity and voltage fading, which fundamentally impedes the practical deployment of LLOs. Here, we report a pre-constructed multifunctional carbon/fluorine-rich artificial cathode electrolyte interface (CEI) layer via a facile thermal treatment. This surface integrated layer, with high-voltage tolerance and amorphous features, is designed to mitigate surface-originated parasitic reactions and phase transformations induced by electrochemistry. Multiscale characterizations reveal that the artificial CEI layer exhibits excellent interfacial compatibility with both the LLO cathode and the electrolyte system, ensuring highly reversible anionic redox and low activation barrier for Li+ transport. Profiting from this architecture, remarkable cycling stability is achieved including 90.6% retention after 300 cycles in half cell, along with high energy efficiency and markedly alleviated voltage fading. More importantly, the artificial CEI layer demonstrates a distinct depolarization effect, which almost completely prevents the rise in charging voltage upon cycling. This work provides valuable insights into surficial/interfacial modulations and broadens research directions for designing high-voltage cathodes with more durable interphases for next-generation batteries.
Noninvasive detection of ultra-weak biomagnetic signals is crucial for modern biosensing, but conventional magnetic sensors are fundamentally limited by intrinsic noise. Orthogonal fluxgates (OFGs) enable high signal-to-noise-ratio detection of weak magnetic fields, yet their performance is still constrained by intrinsic 1/f noise and Barkhausen-related magnetic fluctuations. This study reports a low-noise orthogonal fluxgate in which a newly designed magnetic core and circuit mitigate existing noise limitations. The CoP/Ag composite core, featuring an amorphous-nanocrystalline dual phase, is associated with reduced low-frequency magnetic loss and improved noise performance. When integrated with a closed-loop feedback, the sensor achieves a noise floor of 8 pT/√Hz at 1 Hz. The sensor enables reliable detection of ultralow-concentration magnetic-bead signals. Alpha-fetoprotein (AFP) was used as a model biomarker in an immunomagnetic bead assay, yielding a linear response from 50 fg mL-1 to 100 ng mL-1 and a detection limit of 50 fg mL-1, which compares favorably with representative reported AFP magnetic biosensors. OFGs demonstrate strong prospects in biosensing, geomagnetic measurements, and weak field detection.
Electrochemical reduction of carbon dioxide (CO2RR) offers a route for sustainable chemical production using water as a clean proton source. However, water also promotes the competing hydrogen evolution reaction, limiting CO2RR performance. Here we establish interfacial water as a decisive but overlooked design parameter for selective CO2-to-ethanol electrolysis. A hetero-solvent microenvironment confining diglyme (DiG) near the Cu catalyst substantially suppresses HER under both neutral and alkaline conditions, where protons are supplied via water dissociation. In situ infrared absorption spectroscopy and theoretical calculation results reveal that DiG strengthens the hydrogen-bonding network of interfacial water, reducing free-water population prone to dissociation. Concurrently, the modulated water network effectively hinders solvent-mediated hydrogenation that favors ethylene formation, thereby promoting ethanol formation. Because this strategy modulates the microenvironment rather than the catalyst, it readily extends to Cu-Ag bimetallic catalyst. Moreover, confining hetero-solvent within microenvironment rather than in the bulk electrolyte enables high-current operation at low cell voltages, achieving an ethanol partial current density of 184.2 mA cm-2 at 3.6 V under neutral condition.
The exponential demand for energy-efficient and adaptive computing architectures drives the evolution of artificial intelligence (AI) and machine learning (ML). Neuromorphic computing, inspired by biological neural networks, overcomes the limitations of traditional von Neumann architectures, including high energy consumption and limited scalability. The introduction of two-dimensional (2D) materials, such as transition metal dichalcogenides, hexagonal boron nitride, black phosphorus, and tellurene, enables neuromorphic devices with unprecedented control over electronic and optoelectronic properties. These materials exhibit atomic-scale thickness, high carrier mobility, and tunable bandgaps, facilitating synaptic behaviours such as spike-timing-dependent plasticity and paired-pulse facilitation. This review describes the integration of 2D materials into neuromorphic systems, highlighting applications in wearable electronics, brain-machine interfaces, and quantum neuromorphic platforms. In wearable and edge computing, 2D-based devices enable localized, ultra-low-power data processing. In brain-machine interfaces, they enhance signal transduction and neural interfacing. Quantum effects in 2D materials further enable hybrid quantum-classical neuromorphic architectures for high-dimensional computational tasks. Despite significant advances, challenges in reproducibility, scalability, and stability remain. Addressing these limitations through innovations in synthesis and defect passivation is essential for practical application. This review underscores the transformative potential of 2D-material-based neuromorphic computing for energy-efficient AI. Integration of 2D materials into neuromorphic computing architectures offers a promising pathway toward energy-efficient and adaptive systems that bridge biological learning mechanisms with machine intelligence.
Hepatocellular carcinoma (HCC) responds poorly to immune checkpoint blockade, largely because of an immunologically cold tumor microenvironment (TME) characterized by deficient antigen presentation and impaired cytotoxic T cell responses. Analysis of numerous HCC clinical cohorts, including our institutional datasets, reveals that stimulator of interferon genes (STING) pathway activity is positively correlated with patient survival, enhanced antigen presentation capacity, and an immune-activated TME. However, achieving effective and controllable STING activation in immune-cold HCC tumors remains challenging. Here, we develop a biomimetic nanomedicine that integrates photothermal therapy (PTT), STING pathway activation, and immune checkpoint blockade to treat refractory HCC. A coordination nanomedicine MCI-NP is engineered by co-encapsulating the STING agonist MSA-2 and indocyanine green (ICG) via Cu2+-mediated chelation, enabling stabilized PTT-induced immunogenic cell death together with robust STING-driven innate immune activation. Further cloaked with PD-1-overexpressing cell membranes, MCI-NP@mPD-1 achieves an approximately fivefold increase in tumor accumulation compared with uncoated MCI-NP and enables localized PD-1/PD-L1 axis blockade. Following a single treatment, MCI-NP@mPD-1-based photothermal immunotherapy effectively suppresses primary tumor growth and significantly prolongs survival by remodeling the TME toward an immune-active state, while inducing durable systemic immune memory that effectively limited postoperative lung metastasis. Without introducing additional nanocarriers or excipients, MCI-NP@mPD-1 offers a promising therapeutic paradigm for photothermal immunotherapy of immune-cold HCC.
Wearable flexible sensors for underwater communication and biomotion monitoring are gaining attention. However, developing gel-based strain sensors with high toughness, anti-swelling performance, robust underwater adhesion, and long-term stability remains challenging. Herein, we present a hydrophobic eutectogel (DPF-Zn@LNP-HEG) fabricated via the assembly of a polymerizable hydrophobic deep eutectic solvent (PHDES), 2-phenoxyethyl acrylate (PEA), and Zn2+-coordinated lignin nanoparticles (Zn@LNP). The resulting structure, composed of hydrophobic polymer networks and metal-phenolic complexes, forms hydrophobic microdomains that disrupt the hydration layer and prevent water penetration. Meanwhile, Zn@LNP serve as dynamic sacrificial cross-linkers, enhancing the material's mechanical strength, energy dissipation, and anti-swelling properties. The resulting eutectogel exhibits remarkable tensile strength (1.14 MPa), superior toughness (3.15 MJ m-3), excellent anti-swelling properties (< 1% after 30 days), and robust underwater adhesion (1.07 MPa on glass). Based on these properties, we demonstrate an underwater strain sensor with high sensitivity (gauge factor = 8.12) and long-term stability, enabling underwater Morse code transmission, biomotion monitoring, and Bluetooth-based tracking of swimming movements. This work not only provides a versatile design paradigm for multifunctional underwater sensing platforms but also advances the high-value utilization of bio-based materials in next-generation flexible electronics.
High-density organic electrochemical transistor (OECT) arrays are essential for neuromorphic computing and bioelectronic interfaces, but progress has been limited by the low resolution of electrolyte patterning. Although conventional photolithography offers high feature resolution, it involves a fundamental trade-off among spatial resolution, ionic capacitance, and stability in the electrolyte. Here we report an ion compensation-assisted photolithography (ICAP) strategy that yields electrolyte micro-patterns combining high precision, high capacitance and high stability. A molecularly engineered electrolyte forms, under UV exposure, a physicochemical dual cross-linked network with strong solvent resistance and hydrophobicity, which suppresses swelling during both aqueous development and the subsequent ion-compensation step, preserving pattern fidelity. Ion compensation then restores and enhances the mobile-ion content, increasing areal capacitance. The resulting electrolytes achieve a record 2 μm resolution, 15.6 μF cm-2 capacitance, and strong thermal stability from - 50 to 200 °C. Integrated into OECTs, the ICAP-patterned electrolytes suppress crosstalk by 97.6% and boost on/off ratios by 325%, reducing parasitic coupling by more than 40 times compared to unpatterned arrays. The method is compatible with p-type and n-type organic semiconductors and inorganic oxides, providing a versatile route to scalable neuromorphic circuits and advanced bioelectronics.
The incompatibility of conventional electrolytes with high-voltage cathodes and lithium metal anodes limits the performance of lithium metal batteries (LMBs). Here, an in situ cross-linked polyurethane gel electrolyte (G-P3 AR) is designed through atomic and molecular structure regulation. The polyester segments widen the highest occupied molecular orbital-lowest unoccupied molecular orbital gap, extending the electrochemical stability window to 4.97 V for compatibility with NCM811 cathodes. Polyether segments exhibit a lower Li+ binding energy, reducing the desolvation barrier and enhancing anode stability. At the atomic level, sp2-hybridized boron in the chain extender immobilizes anions (TFSI- and DFOB-) through Lewis acid-base interactions, raising the Li+ transference number to 0.78 and enabling exceptional rate capability (157.7 mAh g-1 at 2 C in the Li||NCM811 cell). Hydrogen bonding between the polymer and solvent restructures the solvation sheath, promoting inorganic-rich interphases. The Li|G-P3 AR|NCM811 cell retains 81.7% capacity after 500 cycles at 0.5 C charge/1 C discharge, demonstrating a rational electrolyte design strategy for high-performance LMBs.
Artificial solid electrolyte interphase offers a promising route to improve the lifespan and safety of quasi-solid-state sodium-metal batteries (QSMBs), yet its limited ion conductivity and the low liquidity of the polymer electrolyte often result in unstable Na plating/stripping kinetics and poor interfacial durability. Herein, we propose a surface-induced "top" Na deposition mechanism facilitated by an ultra-sodiophilic ionic/electronic mixed conductor interphase exhibiting strong Na+ adsorption affinity, which ensures fast and dendrite-free Na anode operation. The embedded Na3Sb alloy phase, featuring high electronic conductivity and strong Na+ adsorption energy, significantly accelerates interfacial ion diffusion and nucleation kinetics, forming a smooth and compact Na deposition layer that facilitates stable solid electrolyte interphase formation and preserves interfacial integrity. Consequently, Na||Na symmetric cells employing a 1, 3-dioxolane-based gel polymer electrolyte deliver an ultra-long-cycling lifespan of 1000 h at 0.5 mA cm-2 with a low overpotential of 40 mV. Moreover, QSMBs incorporating the modified Na anode and Na3V2(PO4)3 cathode demonstrate outstanding cycling stability (74.1% capacity retention after 9000 cycles at 2C) and superior rate capability (91.7 mAh g-1 at 5C). The work provides mechanistic insights and practical strategies for regulating Na deposition, paving the way toward high-performance QSMBs.
The commercialization of liquid lithium-ion batteries has revolutionized the consumer electronics industry. However, conventional lithium-ion batteries with graphite anodes and organic electrolytes are approaching their intrinsic performance limits and struggle to meet the growing demands for higher energy density, reliability, and safety in electric vehicles and large-scale energy storage. Solid-state batteries utilizing lithium or sodium metal anodes are considered promising next-generation energy storage solutions. Despite this potential, the formation of dendrites during charge-discharge cycling remains a critical challenge. Dendrite growth can initiate a destructive feedback loop of crack propagation and further dendrite intrusion, ultimately leading to battery failure and performance degradation. Previous studies have predominantly focused on single physical domains, such as electrochemical, stress, or thermal fields. However, such single-physics approach limits the understanding of dendrite evolution under realistic, coupled multiphysics conditions. This review first compares the morphological characteristics of dendrites in liquid and solid-state metal batteries. It then critically examines the key factors and predictive models of dendrite formation, initially from single-physics and subsequently from an integrated multiphysics perspective. Finally, strategies for mitigating dendrite growth via multiphysics field regulation are summarized. By establishing a comprehensive framework that integrates morphology evolution, multiphysics modeling, and suppression strategies, this work provides a foundational theoretical understanding for addressing dendrite formation in solid-state lithium and sodium metal batteries.
Eco-nanozymology, as an emerging interdisciplinary field, integrates nanotechnology with principles of enzymology to offer innovative strategies for energy conversion and environmental remediation. In contrast with conventional enzymology, eco-nanozymology enhances catalytic efficiency through the precise regulation of interfacial microstructures, electronic distributions, active site configurations, multienzyme cascade catalysis, and functionalized carrier engineering. By harnessing and amplifying natural ecological processes, eco-nanozymology enables effective modulation of energy flow and material cycling within ecosystems. This review focuses on recent advances in the application of eco-nanozymology across energy-related domains, including nitrogen fixation, carbon fixation, methane oxidation, hydrogen production, and energy conversion devices. It further provides an in-depth analysis of the recent progress in the efficient degradation of environmental pollutants and resource-oriented valorization of low-value biomass, such as lignin, agricultural residues, livestock manure, and microplastics. These studies highlight the pivotal role of eco-nanozymology in enhancing the efficiency of environmental management, accelerating the development of green energy technologies, and advancing carbon neutrality goals. The continued development of eco-nanozymology is expected to open new horizons for the deepening and expansion of nanozyme applications, offering green, environmentally friendly, and sustainable technological pathways to address global energy and environmental challenges.
Realizing high-performance perovskite/silicon tandem solar cells requires precise control of wide-bandgap perovskite crystallization. Solvent engineering is the most direct lever for this task; yet, its intricate, multi-variable mechanisms defy intuition-driven design. Herein, we overcome this bottleneck by pioneering a retrieval-augmented large language model to screen > 8000 solvents, identifying γ-valerolactone (GVL) as a non-toxic, high-performance cosolvent. It is found that the GVL strongly coordinates FA+, thus precisely modulating crystallization kinetics, retarding nucleation, and promoting oriented, micrometer-scale grain growth. The resulting films exhibit not only superior crystallinity, reduced non-radiative recombination, but also improved scalability to large area and the tolerance to increased film thickness. Consequently, both the single-junction and tandem devices achieve efficiencies of 23.3% and 32.5%, respectively, along with excellent stability under moisture and illumination. This study establishes the first artificial intelligence (AI)-guided cosolvent strategy for 1-μm-thick perovskite layers in perovskite/silicon tandem architectures, underscoring the transformative role of generative AI in advancing high-performance photovoltaics.
暂无摘要（点击查看详情）