Cancer immunotherapy based on nanovaccines aims to elicit specific anti-tumor immune responses, demonstrating significant therapeutic potential. However, its clinical translation remains hindered by two major challenges: inadequate immunogenicity of the vaccine itself and limited antigen presentation efficiency in dendritic cells (DCs). To overcome these bottlenecks, we have developed a biomimetic nanovaccine for cervical cancer treatment. This vaccine employs a sophisticated biomimetic design: its core consists of iron oxide nanoparticles that serve as both an immune adjuvant and a carrier for the STING agonist DMXAA; the core is enveloped by a hybrid membrane formed by fusing cancer cell membranes (carrying a complete set of tumor-associated antigens) with bacterial membranes (rich in natural immune adjuvants); and the outermost layer is further functionalized with mannose ligands for specific targeting of DCs in the lymph nodes. This multi-layered architecture achieves exceptional synergistic immune activation: the hybrid membrane not only provides a personalized antigen repertoire but also, through its bacterial components, acts as a natural adjuvant to robustly activate innate immunity; upon external stimulation, the core synchronously releases the STING agonist, efficiently activating the cytosolic STING pathway and significantly amplifying the production of type I interferons and related cytokines, thereby shaping a potent anti-tumor immune microenvironment; meanwhile, the mannose-mediated active targeting ensures efficient uptake of the vaccine by DCs in the lymph node sinuses, ultimately greatly promoting antigen cross-presentation and the activation and proliferation of cytotoxic T lymphocytes. In vivo experimental results demonstrate that this nanovaccine can significantly inhibit tumor progression in mouse models of cervical cancer and effectively prevent tumor recurrence. This study provides a novel and translationally promising strategy for the development of highly effective and personalized cancer immunotherapy platforms.

Interstitial doping of metal cations has emerged as a promising strategy to suppress ion migration and enhance the stability of perovskite solar cells. However, excessive doping often introduces lattice strain that undermines structural integrity. Here we present a multi-scale regulation strategy using sodium 2,3,4,5,6-pentafluorobenzoate (PFSBZ) additive to concurrently inhibit ion migration across crystalline lattices, grain boundaries (GBs) and interfaces. The cationic and anionic moieties of PFSBZ suppress iodide-related defects from perovskite lattices and GBs via interstitial occupancy and anion-pi interaction, respectively. This cooperative suppression strategy reduces the required additive contents, thereby preserving crystal structure integrity. Density functional theory calculations further reveal that PFSBZ prevents direct contact between the perovskite and fullerene ring, effectively immobilizing iodide species at the perovskite/PCBM interface. As a result, the PFSBZ-modified perovskite films exhibit enhanced ion-migration energy barriers, reduced trap density, prolonged carrier lifetime, and improved band alignment. The resulting devices achieve a champion power conversion efficiency of 25.53% and retain 90.21% of initial performance after 800 h of continuous operation. Our work offers a multi-scale design principle for stabilizing metal halide perovskites against ion migration.

Uranium (U) is a widely distributed natural element with vast reserves, and its isotope U-235 has been extensively used as nuclear fuel. However, as the most dominant isotope of uranium, U-238 accounts for 99.3 % of natural uranium, but has been rarely utilized. Herein, uranyl-incorporated two-dimensional hydrogen-bonded organic framework (HOF-MA/TMA), designated as U@HOF-MA/TMA, is developed for the photocatalytic production of H2O2. The coordination of uranyl ions with organic ligands increases the formation of long-lived uranyl radicals (*UO22+) and the material exhibit high ability in producing photogenerated electrons. This enables U@HOF-MA/TMA to produce H2O2 through three distinct pathways, including the direct oxidization of H2O by *UO22+, the indirect reduction of O2 by *UO22+ via the cascade of the hydrogen atom transfer and single electron transfer processes, and the reduction of O2 by photogenerated electrons. Unlike previous reported uranium-based photocatalysts that operate via only two reaction pathways, U@HOF-MA/TMA engages three distinct pathways, thereby further boosting its photocatalytic efficiency. Consequently, U@HOF-MA/TMA achieves the highest H2O2 evolution rate of 559.8 mu mol g- 1 h- 1 among all uranium-based photocatalysts. This study provides new strategy for enhancing the photocatalytic activity of uranyl ion and will contribute to the utilization of the vast underutilized uranium resources.

Cerebrospinal fluid (CSF) leakage is a prevalent complication following dural injury, necessitating prompt implantation of dural patches. However, postoperative bacterial infections and tissue adhesion frequently compromise surgical outcomes and may lead to secondary complications. To address these challenges, a self-adhesive Janus dural patch is developed by integrating drug-loaded fibrous meshes with a layer of tissue adhesive hydrogel. Vancomycin and mitomycin C are co-loaded into the meshes to provide antibacterial and anti-tissue adhesion functions, respectively. The hydrophobicity of the electrospun fibers can make the patch effectively preventing CSF leakage. The tissue adhesive hydrogel is made of oxidized hyaluronic acid methylacrylate (OHAMA), whose aldehyde groups can react with amino groups to form robust tissue adhesion. As a whole, the patch shows a high burst pressure resistance (35 kPa). In repairing dural defects using rat models, the patch achieves rapid and suture-free self-tight sealing of dural defects. The sustained release of vancomycin and mitomycin C effectively prevents bacterial infection and postoperative adhesion to brain tissue. Promisingly, this Janus dural patch combines immediate mechanical sealing with multiple biological activities, offering a potential solution for dural repair.

Photocatalytic uranium extraction can surpass the intrinsic capacity limits of adsorption by converting soluble uranyl into insoluble uranium peroxides via H2O2 generation. However, this process requires simultaneous local enrichment of H2O2 and UO22+ beyond the solubility product constant, which is difficult to achieve in continuously flowing and ultra-dilute seawater. Here we report a hollow hierarchical covalent organic framework (COF) microcavity reactor, HH-COF-(CN/AO)x, that spatially decouples H2O2 generation from uranyl capture to overcome this thermodynamic barrier via a bidirectional reactant flux coupling strategy. A cyano-functionalized inner layer produces and stores H2O2 in a central cavity, whereas an amidoxime-rich outer layer selectively enriches uranyl ions. The convergence of outward H2O2 flux and inward uranyl adsorption establishes a persistent high-concentration interface that supports continuous formation of insoluble uranium peroxide. The optimized HH-COF-(CN/AO)0.35 achieves 25.1 mg g-1 uranium uptake in natural seawater, 3.9 times that of the non-hollow analog, which demonstrates a generalizable strategy for manipulating reactant fluxes in ultra-dilute environments for realizing effective resource extraction from water environment.

Purpose: Immunotherapy has attracted increasing attention in cancer treatment, but its efficacy is greatly limited due to the low immunogenicity of tumors and immunosuppressive tumor microenvironment (TME). To address this, we constructed a biomimetic M1 macrophage membrane-Camouflaged nanoplatform (M1@CTP) for the co-delivery of the natural antitumor compound Tanshinone IIA (Tan IIA) and the immunogenic cell death (ICD) inducer Copper-diethyldithiocarbamate (CuET) to enhance antitumor immunity. Methods: CuET/Tan IIA/PLGA (CTP) nanoparticles were synthesized using a previously reported two-step emulsification method. Subsequently, these nanoparticles were then coated with induced M1 macrophage membranes to obtain M1@CTP. We systematically characterized their morphology, physicochemical properties, and environmental stability. In vitro studies assessed cytotoxicity, immune activation, and tumor-targeting capability. Subsequently, the antitumor efficacy and modulation of the TME were assessed in vivo. Finally, the biosafety of the nanoplatform was evaluated via histopathological and biochemical analyses. Results: Endowed by M1 macrophage membran coating, M1@CTP enables immune evasion and tumor homing, thereby prolonging systemic circulation time and achieving efficient tumor accumulation. Our study demonstrates that M1@CTP synergistically induces potent ICD, promotes dendritic cell maturation, and remodels the TME, leading to the infiltration of cytotoxic T lymphocytes. This process effectively converts "cold" tumors into "hot" ones and elicits a robust systemic antitumor immune response with favorable safety profiles. In addition, M1@CTP significantly enhanced the efficacy of immune checkpoint inhibitors in cold tumor models. Conclusion: This study provides an innovative and precise immunotherapy nanoplatform that coordinately modulates the TME and induces robust antitumor immunity, offering a promising strategy to overcome current limitations in immunotherapy.

Solar-driven selective aerobic transformations of organic chemicals to specific products with high selectivity and productivity is significant for green chemistry but extremely challenging. This study presents a metal displacement strategy to construct magnetism-plasma coupled semiconductor systems comprising plasma Ag nanoparticles embedded within transition metal ion-substituted Ag-Bi halide double perovskites for photocatalytic aerobic oxidation of styrene. The resulting photocatalysts efficiently boosts the generation of 1O2, achieving an impressive benzaldehyde productivity of 18.3 mmol g- 1 h- 1 under light-magnetism field irradiation, without significant loss of reactivity. Transient absorption and in-situ photovoltage spectroscopy combined with computational simulations demonstrate that magnetism-plasma coupling effects in perovskite intensifies the localized electromagnetic field and facilitates the efficient separation of photogenerated charge carriers. Theoretical calculations elucidate that magnetism-plasma coupling in perovskite also boosts the interfacial electron transfer and the absorption and activation of O2. This study presents a strategic approach to reinforcing the reactivity of photocatalysts for aerobic oxygenation via advanced plasma and electronic engineering.

The mobility and toxicity of uranium in nuclear wastewater necessitate efficient recovery strategies, yet coexisting cations often hinder effective uranium capture. Here, we discovered that impurity ions significantly improve UO22+ separation efficiency by guanosine monophosphate (GMP). Using Cu2+ as a representative interfering ion, the separation efficiency of UO22+ enhances by approximately threefold. Notably, an optimal GMP dosage of merely 0.02 g/L achieves a removal efficiency of 90 %, with a maximum separation capacity reaching 2170 mg g-1. These results demonstrate the superior performance of GMP compared with conventional phosphate-based adsorbents. Mechanistic studies have confirmed the existence of the Cu-phosphate-U bond. Combined with the Cu-N7 and U-OH bonds, GMP forms a complex network structure with Cu2+ and UO22+. Additionally, Cu2+ significantly reduce the binding energy between GMP and UO22+. These findings demonstrate that GMP functions as a robust small-molecule platform for efficient and scalable uranium recovery under complex aqueous conditions.

Engineering heterostructured electrocatalysts with well-defined interfacial chemistry is an effective strategy to enhance catalytic activity, yet the fundamental origin of epitaxial heterojunction superiority remains insufficiently understood. Herein, a highly lattice-matched epitaxial heterostructure is constructed by growing nickel ferrite (NiFe2O4) nanocubes on nickel cobaltate (NiCo2O4) nanorods via a controllable coprecipitation method. The epitaxial growth process is regulated by tuning the coprecipitation time, enabling precise interface modulation. Using this model system, the structure–property relationship of epitaxial heterojunctions is systematically investigated. Combined experimental characterizations and theoretical calculations reveal that high lattice matching facilitates rapid interfacial electron transport, stabilizes the built-in electric field, and generates electron-/hole-rich active sites, thereby optimizing the adsorption/desorption balance of reaction intermediates during both ORR and OER processes. As a result, the epitaxial NFO@NCO heterostructure exhibits enhanced bifunctional catalytic activity and durability compared with physically mixed counterparts. When applied as an air cathode catalyst in zinc–air batteries, the optimized NFO@NCO-8-300 delivers a high peak power density of 126.46 mW·cm-2 and outstanding cycling stability exceeding 800 h. This work provides mechanistic insights and a general design principle for lattice-matched epitaxial heterostructures toward efficient and low-cost bifunctional electrocatalysts.

With the widespread replacement of lead-acid batteries by advanced alternatives, improper disposal and unregulated recycling of spent lead-acid batteries have emerged as major sources of lead pollution. Herein, a porous poly(acrylic acid/itaconic acid) (PAA/PIA) hydrogel adsorbent was synthesized via a one-pot method for efficient lead (Pb2+) removal. Itaconic acid introduces abundant carboxyl groups-twice that of acrylic acid-enhancing chelation with Pb2+, while acrylic acid facilitates the formation of a flexible three-dimensional crosslinked network. The porous architecture endows the material with excellent mass transfer properties and increased exposure of functional groups, thereby significantly enhancing adsorption efficiency. The effect of IA/ AA monomer ratio on Pb2+ adsorption was systematically investigated. At an optimal ratio of (m(AA):m(IA) = 4:1), the hydrogel achieved a maximum adsorption capacity of 697.12 mg g- 1at 25 degrees C, among the highest reported for hydrogel-based adsorbents. Through synergistic monomer design, this material enables efficient Pb2+ capture with excellent environmental adaptability and operational stability, offering a scalable material platform and sustainable technological pathway for the treatment of lead-contaminated wastewater from spent lead-acid batteries.

The two-electron electrochemical oxygen reduction reaction presents a sustainable strategy to hydrogen peroxide (H2O2) synthesis, opening avenues for decentralized environmental water treatment and chemical synthesis, yet its practical translation is impeded by inadequate catalyst selectivity and durability. Here, we report a universal design principle for anchoring iodine single atoms onto various high-entropy sulfide matrices. Experimental and theoretical analyses reveal that this architecture harnesses the dynamic redox activity of iodide to create an adaptive electron reservoir, reversibly modulating the local electronic structure to optimally stabilize reaction intermediates, thereby steering the oxygen reduction reaction pathway toward the two-electron route. The resulting electrocatalyst achieves a high H2O2 production rate exceeding 33 mol gcat-1 h-1, and exceptional longterm stability even in seawater. Most importantly, the integrated I/HES system capitalizes on in-situ H2O2 generation within actual wastewaters achieving over 99% uranium extraction efficiency from 1000 ppm solutions, demonstrating practical viability for on-site environmental remediation and resource recovery.

Efficient uranium extraction from wastewater is critical for environmental safety and resource sustainability, yet remains challenging because trace uranium often coexists with high concentrations of competing ions. To address this issue, a series of mixed-ligand defective metal-organic frameworks (MOFs), denoted as AIPA/UiO-67-X, were rationally constructed through a tailored defect-engineering strategy for selective uranyl capture. Incorporation of short-chain 5-aminoisophthalic acid (AIPA) into the UiO-67 framework generated coordinatively unsaturated Zr sites and accessible carboxyl groups, which enriched binding sites for uranyl adsorption while enhancing the Lewis basicity of the framework. Further ligand modulation using a diamino biphenyl dicarboxylate linker with a meta-amino configuration introduced additional amino coordination sites and created a more open local coordination environment, thereby reducing steric hindrance during uranyl binding. The resulting multifunctional microenvironment enabled stable equatorial multidentate coordination with the linear O=U=O structure of uranyl ions and exhibited a more negative adsorption energy (−10.55 eV). Consequently, AIPA/UiO-67-m-N achieved a maximum uranium adsorption capacity of 1392.9 mg g−1, a uranium removal efficiency of 98.81%, and a distribution coefficient of 7.91 × 105 mL g−1 in complex coexisting-ion systems. This work provides a rational strategy for designing highly selective MOF adsorbents for uranium recovery from complex wastewater.

Addressing uranium contamination in tailings wastewater is key to reducing ecological threats and securing the future of nuclear power. The integration of adsorption with in situ photocatalytic U(VI) immobilization has been explored as a green alternative, but charge separation inefficiency and poor ion selectivity continue to hinder its use in complex wastewater. Herein, we constructed a bimetallic metal–organic framework, OVs-Zr/Fe UiO-66-NH2, by incorporating Fe2+/Fe3+ species into the UiO-66-NH2 lattice. The incorporation of Fe into the UiO-66-NH2 lattice narrows the bandgap and improves visible-light absorption. The same Fe doping induces oxygen vacancies (OVs) within the framework. The OVs trap photogenerated electrons to enhance charge separation, while their electron-rich nature favors the selective uptake of UO22+. Meanwhile, the Fe2+/Fe3+ redox couple provides an internal electron mediation pathway, directing electrons to the OV-bound uranyl species and promoting the interfacial uranium conversion into stable species. With this combined adsorption–photocatalysis mechanism, OVs-Zr/Fe UiO-66-NH2 removed 99.2% of U(VI) within 6 h under ambient air without sacrificial agents, and its distribution coefficient (Kd) reached 1.96 × 105 ml g−1, 11.9 times that of pristine UiO-66-NH2. This work provides a synergistic strategy for crafting photocatalysts with high efficiency and selectivity for sustainable uranium remediation in complex waters.

High-energy electron irradiation provides an exceptionally fast, energy-dense route to fabricate porous crystalline frameworks, yet its utility for MOFs is fundamentally limited by a trade-off between accelerated crystallization and radiation-induced damage. Here, we show that this trade-off can be actively navigated by the systematic modulation of the irradiation dose. Using MOF-76 as a model, we identify a dose-dependent maturation regime centered at 120 kGy, at which the material retains high crystallinity while exhibiting a maximized concentration of beneficial defects. Comprehensive characterization confirms the coexistence of preserved framework order and enhanced defect density at this dose. The optimally defective MOF-76 displays markedly improved uranyl ion uptake, reaching a maximum adsorption capacity of 441 mg g-1, which is 4.4-fold higher than that of solvothermally synthesized MOF-76, outperforming both the pristine material and samples produced at other doses in terms of capacity and adsorption kinetics. These results establish dose-controlled electron-beam irradiation as a practical means to tailor defect landscapes in MOFs, enabling the rational design of high-performance adsorbents for radionuclide remediation and related separations.

Efficient adsorption and recoverable removal of uranium from aqueous media are crucial for resource utilization and environmental risk mitigation. However, conventional adsorbents often suffer from poor structural stability, limited reusability, and difficulties in deployment and recovery, which hinder practical applications. Herein, a robust macroporous ternary composite gel bead (PEI/SA-XLS) was fabricated from sodium alginate (SA), polyethyleneimine (PEI), and synthetic hectorite-type clay (laponite XLS) via synergistic polyelectrolyte complexation, supramolecular crosslinking, and freeze-drying. SA and PEI formed a 3D network through electrostatic interactions, while XLS nanosheets reinforced the framework through hydrogen bonding between surface silanol groups and amino/hydroxyl groups. Freeze-drying generated macropores (similar to 100 mu m), thereby significantly enhancing mass transfer and facilitating uranyl diffusion into the bead interior. Mechanistically, negatively charged XLS surfaces promoted electrostatic enrichment of UO22+, while silanol, amino, and carboxyl groups provided cooperative binding sites for efficient uranyl capture. The maximum adsorption capacity (q(m)) was similar to 2707 mg & centerdot;g(-1) (Langmuir). A removal efficiency of similar to 98% was achieved at 15.1 mg & centerdot;L-1 (V = 100 mL), and similar to 93% efficiency was maintained after ten adsorption-desorption cycles. These results highlight that macroporous transport channels and mechanically robust pore walls play a dominant role in adsorption efficiency and cycling stability for macroscopic adsorbents.

The sustainable recycling of platinum group metals (PGMs) from secondary resources requires task-specific adsorbents that offer both high extraction efficiency and environmental compatibility. However, rhodium recovery remains particularly challenging due to the high thermodynamic stability of its chloro-complexes, which hampers ligand exchange with adsorbent binding sites. Here, we report a series of porous organic polymer (POP)-based nanotraps for targeted rhodium extraction, functionalized with pincer-type chelators, whose installation was realized by mechanochemical imine bond formation in a green, solvent-free manner. Among them, POP-Py-OMe bearing electron-donating -OMe groups, exhibits the highest rhodium uptake capacity and the fastest extraction kinetics from aqueous solution, significantly outperforming its -OH and -H analogues. Furthermore, sequential breakthrough experiments employing various task-specific POPs as column packing adsorbents enable the efficient and selective separation of Pt, Pd, and Rh in sequence with high purity, highlighting a practical and modular strategy for comprehensive PGM recovery.

ABSTRACT Iodine, an indispensable element for both industry and biology, suffers from scarcity in the earth's crust and inefficiency in conventional recovery technologies. Herein, inspired by the iodide oxidation pathway in thyroid follicular lumens, we designed a bioinspired micro‐ionic‐reactor based on a porous organic polymer (MIR‐POP) that integrates iodide capture with in situ photooxidative conversion. The cationic framework of MIR‐POP enables ultrafast electrostatic enrichment of iodide (I−) ions within confined pores, where subsequent light irradiation drives their transformation into molecular iodine and polyiodide species. This bioinspired strategy outperforms adsorption‐based materials and achieves a record uptake capacity of 853.06 mg g−1. Moreover, MIR‐POP exhibits remarkable selectivity toward competing anions and delivers high recovery efficiencies of 93.8% in simulated mining wastewater and 85.8% in natural brine, highlighting its promising potential in complex environments. This bioinspired microreactor platform opens a new avenue for selective I− ions recovery and in situ conversion, advancing both environmental remediation and strategic iodine resource recovery.

Efficient extraction of dispersed uranium resources is crucial for sustainable nuclear energy, yet remains challenging because of the low concentration of uranium in aqueous environments, interference from coexisting ions, and the rapid recombination of photogenerated charge carriers in photocatalytic systems. Herein, a Co-N4 anchored porphyrin-based COF (ETPT-AO-Co) was constructed via amidoxime functionalization and subsequent Co coordination. By integrating selective uranyl-binding sites with electron-capturing Co-N4 centers, ETPT-AO-Co enables enhanced visible-light utilization, efficient charge separation, and sacrificial-agent-free photocatalytic uranium extraction. Under simulated sunlight, ETPT-AO-Co achieved a uranium extraction capacity of 1948.06 mg g-1, approximately 25% higher than that of Co-free ETPT-AO. Mechanistic studies reveal that Co-N4 sites promote electron transfer and O2 activation, driving the conversion of U(VI) into stable insoluble (UO2)O2 & sdot;2H2O. This work offers a molecular-level strategy for designing advanced COF photocatalysts for sacrificial-agent-free uranium recovery and broadens the application of metal-coordinated porous frameworks in solar-driven radionuclide remediation.

Garnet-type Li7La3Zr2O12 (LLZO) solid electrolytes (SEs) have garnered significant attention as promising candidates for solid-state lithium batteries (SSLBs), owing to their high ionic conductivity, excellent thermal stability, and wide electrochemical window. However, the major drawback is their poor air stability at room temperature, which hinders practical application. To address this issue, we designed a novel high-entropy solid electrolyte, Li6.1La3Zr0.8Ta0.3Nb0.3W0.3Y0.3O12 (LLZTNWYO), by introducing Ta, Nb, W, and Y cations to partially substitute for Zr in the LLZO lattice. Solid-state nuclear magnetic resonance (NMR) spectroscopy and density functional theory (DFT) calculations demonstrated that the high-entropy LLZTNWYO electrolyte possesses a lower Li+ migration energy barrier, thereby facilitating enhanced Li+ transport and yielding higher ionic conductivity. Moreover, thermogravimetric analysis, 3D Raman spectroscopy, and in-situ optical microscopy confirmed the outstanding air stability of LLZTNWYO, which effectively suppresses H+/Li+ exchange and inhibits the growth of lithium dendrites. Benefiting from such synergistic effect, the Li|LLZTNWYO|LiFePO4 SSLBs exhibit excellent cycling stability with 90% high capacity retention after 500 cycles under high rate conditions of 0.5C. This strategy effectively paves the way for realizing long lifespan SSLBs.

The development of efficient adsorbents for radioactive iodine capture is critical for environmental and human safety. Flexible covalent organic frameworks (COFs) are promising candidates due to their structural adaptability, yet how their structural reconfigurations govern iodine adsorption remains unknown. Herein, we report the design and synthesis of two highly crystalline, ether-embedded flexible COFs (F-TEA and F-BEA), along with a rigid, ether-free counterpart (R-TPA) as a control. In the triazine-containing F-TEA, the ether bond reduces steric hindrance between triazine and benzene rings, which improves adsorption-site accessibility and enhances halogen-bond interactions, thereby leading to superior iodine vapor capture (F-TEA>F-BEA>R-TPA). However, the triazine ring also induces an ether-bond locking effect, triggering a water-responsive structural rearrangement that reduces micropore accessibility and water-phase adsorption. In contrast, the triazine-free F-BEA possesses freely rotating ether bonds that enable adaptive framework swelling, which can accommodate more iodine molecules and facilitate iodine uptake through multi-site charge transfer. Consequently, F-BEA achieves a high iodine adsorption capacity of 7.25 g g-1 from aqueous solution, whereas the rigid R-TPA undergoes framework collapse and exhibits the lowest performance. This study establishes conformational control of flexible linkages as a key design principle for high-performance porous iodine adsorbents.