Advanced Science最新文献

The heat-sensitive transient receptor potential vanilloid 1 (TRPV1), which is highly expressed on cardiac sensory neurons, reportedly plays a crucial role in transmitting nociceptive signals from the heart to the spinal cord during myocardial ischemia and reperfusion. Here, iron oxide nanocubes (FeNCs) are developed that are conjugated with an antibody against the extracellular portion of TRPV1, and they are named FeNCs-TRPV1. In F11 cell line and primary dorsal root ganglion neurons, FeNCs-TRPV1 specifically activate TRPV1 channels and trigger Ca²⁺ influx through magnetothermal effect under an alternating current magnetic field (ACMF). Intraspinally injected FeNCs-TRPV1 induced TRPV1 desensitization in rats exposed to repetitive and transient ACMF before ischemia, resulting in the inhibition of TRPV1-mediated Ca²⁺ signaling and neuropeptide release in the spinal cord during myocardial ischemia and reperfusion. Consequently, FeNCs-TRPV1 reduce cardiac injury and ventricular arrhythmia, enhance the activity of prosurvival kinases, and inhibit myocardial cell apoptosis. These findings suggest that magnetic nanomaterials-mediated remote regulation of spinal TRPV1 can be a novel non-invasive neuromodulation therapy for the treatment of myocardial ischemia-reperfusion (IR) injury.

Perovskite and organic semiconductors exhibit analogous properties, including bandgap tunability, low-temperature solution processing, and high potential for lightweight applications. These similarities render them highly attractive for being integrated in multijunction architecture: perovskite-organic tandem solar cells (POTSCs). Nevertheless, the efficiency of POTSCs is limited by electrical losses, which stem from both the wide-bandgap (WBG) perovskite layers and the interconnecting layers (ICLs) between two subcells. These two essential components also constrain the tandem device stability. In this study, the underlying cause of open-circuit voltage (V_OC) losses in WBG perovskites is identified, which is ascribed to the presence of mobile defects distributed at surface regions. An employ effective passivation agent with functional chemical groups is further employed to facilitate the healing of the mobile defects, thereby enhancing the V_OC to 1.35 V for WBG perovskite solar cells with a bandgap of 1.81 eV. Subsequently, solution-processed graphene oxide layer ICLs are developed for tandem application, which not only reduces electrical losses but also improves tandem device stability. The synergistic integration of these two strategies has enabled POTSCs to surpass 25% efficiency while simultaneously achieving enhanced operational stability.

Solar-driven hydrogen supply systems filled with high-density hydrides can overcome the traditional limitations of external heating and power sources. However, these systems commonly rely on photothermal effects to elevate the hydride surface temperature, significantly restricting their photon-to-chemical conversion efficiency. Therefore, exploring hydrogen supply systems driven by visible-light photocatalysis offers immense potential for achieving enhanced photon-to-chemical conversion. In this study, a non-thermodynamic regulation mechanism based on the dehydrogenation of alane and driven by the broadband-responsive photocatalysis of AlH₃-MOF is investigated. The dehydrogenation rate under visible-light irradiation reaches 30.8 µmol g^-1 min^-1, achieving a better than 20-fold improvement compared to room-temperature dark conditions. Moreover, a hydrogen release capacity of 4.7 wt.% is achieved at an ultra-low light intensity of 0.37 W cm^-2 without external heating. Experimental investigations confirm the in situ formation of a novel Al/MOF heterostructure during photocatalytic dehydrogenation. Al nanoparticles induce the injection of hot electrons into the MOF via localized surface plasmon resonance, significantly prolonging the photogenerated charge carrier lifetime. Density functional theory calculations reveal that AlH₃ chemisorption at Al/MOF interfaces induces interfacial charge redistribution and establishes a direct interfacial charge transfer channel. This study pioneers a non-thermodynamic photocatalytic regulation paradigm for solid-state high-energy hydrides, enabling portable application in abundant solar-irradiated regions.

The introduction of the photothermal effect holds significant importance for enhancing the efficiency of solar-driven photoelectrochemical energy conversion, including water splitting, CO₂ reduction, and nitrogen reduction reactions. Distinguishing and quantifying the effects of local heating to photoelectrochemical reactions, however, remains challenging. Herein, it is reported that the local thermal in photoelectrochemical reaction can be in situ measured via an optical microfiber sensor, which captures thermo-optic signals from highly sensitive modal interference. For proof-of-concept, the laser-induced graphene (LIG) electrode as a model for photoelectrochemical reaction, which has emerged as a highly promising photoelectrode material owing its excellent photothermal conversion efficiency, tunable structure, and outstanding electrical conductivity. Experimental studies demonstrate that the local photothermal effects contribution can be quantified in real time, which further decoupling the photoelectronic effect contribution in photocurrent. Additionally, the potential for further enhancing sensitivity through dispersion turning point is demonstrated, achieving approximately five times the improvement over traditional fiber interferometers. This advancement holds promise for ultra-sensitive detection of weak photoelectrochemical reactions. Therefore, this work provides critical experimental evidence for decoupling the photothermal and photoelectronic effects in photoelectrochemical reactions through a highly sensitive microfiber in situ detection technique, facilitating the development of advanced photoelectric materials and more efficient solar energy conversion systems.

Antitumor immunotherapy has become a pillar therapy by activating the immune system to recognize and attack tumor cells. Yet its efficacy is limited by the immunosuppressive tumor microenvironment (TME) and related mechanisms like hypoxia, high glutathione (GSH) expression, and immune evasion. Due to TME complexity and tumor heterogeneity, monotherapy struggles to modulate immunosuppressive factors for potent results. To solve this, this work develops a multifunctional immune stimulator (3IZH), which can simultaneously boost immunity, downregulate GSH, and alleviate hypoxia. In weakly acidic TME, it releases photosensitizer (3ICy5) and Fe ions. Fe ions consume GSH and relieve hypoxia via redox reactions and hydrogen peroxide decomposition. 3ICy5 accumulates in the endoplasmic reticulum (ER), produces ROS, induces severe ER stress and DAMPs release, triggering immunogenic cell death (ICD). Fe ions and ROS also reduce glutathione peroxidase 4 (GPX4), causing ferroptosis. ICD and ferroptosis activate T cell infiltration to restructure TME. Combined with HIF-1α inhibitor digoxin, 3IZH further reduces HIF-1α resistance, enhances immune cell infiltration, and shows satisfying efficacy in bilateral tumor-bearing mice. The regulatory effect of the immune-suppressive TME, the remarkable therapeutic effect, as well as the safety profile, together indicate the potential of the multifunctional immune stimulator design strategy.

The escalating challenge of water contamination by recalcitrant organic pollutants and pathogens calls for sustainable, solar-powered technologies that operate without external energy or chemical inputs. Such systems require multifunctional materials capable of harvesting broad-spectrum sunlight to generate reactive oxygen species (ROS) for simultaneous degradation and disinfection. Conventional photocatalysts are hindered by their limited spectral absorption and rapid charge recombination, which restricts their practical efficacy in real-world applications. To overcome these challenges, we engineered a hybrid Bi₂Te₃@CdS nanostructure incorporated into a porous polyurethane (PU) foam scaffold, facilitating synergistic photothermal and thermocatalytic efficacy under comprehensive solar illumination. The hybrid architecture facilitates effective separation of photogenerated charge carriers, markedly diminishing recombination losses and augmenting the production of ROS, such as •O₂ ^-, •OH, and H₂O₂. Concurrently, Bi₂Te₃ functions as a thermoelectric absorber that effectively transforms NIR-induced heat into catalytic activation energy, thereby enhancing degradation kinetics. This dual-mode activation causes organic pollutants (such as dyes and pesticides) to mineralize quickly and inactivate E. coli and S. aureus with >99% photothermal assistance. High photostability and reusability enable the material to maintain its activity over multiple cycles without appreciable degradation. By synergistically integrating broadband solar harvesting, efficient ROS generation, and thermocatalytic activation, this study presents an energy-autonomous strategy for water remediation and sustained antimicrobial defense, offering significant potential for public health benefits.

Current intravesical therapies for bladder cancer after resection are limited by poor tissue penetration, off-target effects, and insufficient efficacy. To address these challenges, this study designs a thermo-responsive hydrogel (PNH) that encapsulates chitosan (CS)-coated Fe/Mn bimetallic nanozymes (FMCC) together with cholesterol oxidase (ChOx). FMCC displays multiple enzyme-mimicking activities, including peroxidase (POD), catalase (CAT), and glutathione oxidase (GSHox). ChOx amplifies this catalytic cascade, enhancing reactive oxygen species (ROS) production and inducing ferroptosis-mediated tumor cell death. The CS coating improves mucosal adhesion and tissue permeability, thereby facilitating intravesical delivery. Upon near-infrared (NIR) irradiation, FMCC generates heat that liquefies the hydrogel, enabling spatiotemporally controlled drug release and providing mild photothermal therapy (MPTT). This photothermal effect acts synergistically with ferroptosis induction and immune modulation, concurrently minimizing damage to normal tissues. In parallel, ChOx disrupts cholesterol-rich membrane rafts and promotes pro-inflammatory M1 macrophage polarization. Released Mn²⁺ ions further potentiate immune activation by stimulating the cGAS-STING pathway, driving IFN-β and IL-6 secretion, dendritic cell maturation, and T cell infiltration. Together, this nanozyme-hydrogel system integrates tissue penetration, metabolic disruption, and immune stimulation, representing a promising strategy for localized bladder cancer therapy.

As artificial substitutes for natural enzymes, nanozymes possess advantages such as high catalytic activity, low cost, excellent stability, and suitability for large-scale production. Inspired by the cascade reactions in biological systems, constructing cascade nanozyme systems with step-saving and high efficiency has been recognized as a key approach to enhancing the functional performance of nanozymes. With the discovery of more nanomaterials with various enzyme-like activities, especially the unique multi-enzyme activity of nanozymes, unprecedented opportunities have arisen for advancing biomimetic design to a higher level. Furthermore, aided by advanced tools such as theoretical calculations, the structural design and functional tuning of nanozymes have gradually become customizable and intelligent, significantly promoting their application in specific tasks ranging from biosensing to therapy. This review introduces the evolution of all-nanozyme cascade reaction systems from a self-cascading nanozyme system to immobilized nanozyme-based cascade catalytic system, and introduces key mechanistic insights and commonly used research methods to clarify their catalytic characteristics and design principles. A detailed classification of all-nanozyme cascade reaction systems is provided, and an analytical survey of recent applications of all-nanozyme cascade reaction systems in biosensing and therapy is covered. Finally, this review discusses the challenges that all-nanozyme cascade reaction systems may face in their application.

The limited spatial resolution of mainstream spatial transcriptomic technologies captures transcriptomic mixtures from multiple cells per spot, obscuring crucial single-cell information. While numerous methods leverage single-cell RNA sequencing references to infer cellular composition from ST data, they primarily rely on fixed cell type labels, overlooking the intrinsic hierarchical heterogeneity (subtypes within broad types) of cellular populations and its association with spatial organization. To address this limitation, HIDF, a Hierarchical Iterative Deconvolution Framework is proposed. HIDF progressively resolves cellular heterogeneity from coarse to fine granularity, it employs a hierarchical iterative optimization mechanism guided by the cluster-tree to recover single-cell spatial distributions. This process is further stabilized and enhanced by incorporating dual regularization constraints (spatial neighborhood and cross-level regularization). Comprehensive benchmarking demonstrates that HIDF outperforms existing methods on simulated and real tissue datasets. In addition, HIDF not only reveals cell type distributions consistent with known tissue functions but also uncovers spatially heterogeneous patterns of cell subtypes undetectable by conventional methods.

With a high redox potential and long half-life, high-valent cobalt-oxo species (Co(IV)═O) hold promise for water purification by eliminating persistent contaminants. However, the inefficient and unsustainable generation of Co(IV)═O limits its practical application. In this work, a phosphorus (P)-doped cobalt single-atom catalyst (Co─N₆/C─P) is developed, where P-substituted nitrogen (N) atoms are coordinated to the cobalt site at meta-positions. This remote modulation reduces the charge density of the cobalt site and positively shifts the d-band center of the cobalt atom, thereby lowering the energy barrier for Co(IV)═O generation. The P-doping increases the turnover frequency of the cobalt center by 3.5 times and the steady-state concentration of Co(IV)═O by 2.7 times. The (Co─N₆/C─P)/peroxymonosulfate (PMS) system exhibits a pollutant degradation kinetic constant three times higher than that of Co─N₆/C, surpassing most reported single-atom catalytic PMS systems. A continuous-flow reactor based on Co─N₆/C─P achieves over 87% contaminant removal after 24 h of operation. The treated real wastewater exhibits exceptionally low cytotoxicity (2.96 mg-phenol L^-1) and genotoxicity (0.08 µg-4-NQO L^-1) to mammalian cells, enhancing water safety. This study presents a reliable approach for the removal of persistent contaminants and the reduction of toxicity through efficient Co(IV)═O generation enabled by a remote modulation strategy.