Latest ArticlesCurrent immunotherapy for melanoma remains limited by low immunogenicity, immune-related toxicity, and an immunosuppressive tumor microenvironment (TME), necessitating more effective strategies to enhance treatment outcomes. Enhancing immunogenic cell death (ICD) induction with immune remodelling offers a promising approach to boost antitumor immunity. Here, we develop a transdermal microneedle (MN) system co-delivering garlic-derived nanovesicles (Ve) and immunomodulatory garlic polysaccharides (GP) to synergistically activate a self-reinforcing cell death pathway and reprogram the immunosuppressive TME. The dissolving MN platform enables efficient intratumoral delivery of Ve-fused thermosensitive liposomes (TSVL@PTX/ICG), loaded with paclitaxel (PTX) and the photosensitizer indocyanine green (ICG). Upon near-infrared (NIR) irradiation, ICG-mediated photothermal heating triggers rapid drug release, inducing pyroptosis via gasdermin E (GSDME) cleavage while amplifying photodynamic therapy (PDT)-driven mitochondrial damage. This dual cell death mechanism elicits robust ICD, releasing tumor antigens and damage-associated molecular patterns (DAMPs) to enhance dendritic cell activation and cytotoxic T-cell infiltration. Concurrently, GP reprograms tumor-associated macrophages (TAMs) from immunosuppressive M2 to pro-inflammatory M1 phenotypes, reshaping the TME into an immunostimulatory niche. This multi-modal approach, combining pyroptosis-driven ICD, PDT, and immune remodelling achieves potent antitumor immunity and melanoma suppression, highlighting the potential of plant-derived therapeutics in cancer immunotherapy.
Lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation energy storage systems owing to their high theoretical capacity and energy density. However, conventional polyolefin-based separators suffer from randomly distributed pores with broad size distributions, which are ineffective in suppressing the polysulfide shuttle effect. Moreover, they lack functional groups for catalyzing polysulfides conversion and promoting uniform lithium-ion deposition. Herein, we synthesized a hybrid material (denoted as DAAQ-TFP/MXene) via in situ growth of redox-active covalent organic frameworks (DAAQ-TFP) on amine-functionalized MXene nanosheets. The resulting DAAQ-TFP/MXene hybrid features a porous architecture and dual binding/catalytic sites, enabling efficient polysulfides adsorption and catalytic conversion, enhanced lithium-ion transport, and uniform lithium deposition. Consequently, the DAAQ-TFP/MXene-coated PP separator exhibits a high lithium-ion transference number (0.53). The LiLi symmetric cell incorporating this separator operates stably for 3800 h at 5 mA/cm2 and 1 mAh/cm2. Furthermore, Li-S full cells using DAAQ-TFP/MXene@PP separator delivers a high specific capacity (1224 mAh/g at 0.1 C), excellent rate performance (631 mAh/g at 5 C), and long-term cycling stability (71.3% capacity retention after 300 cycles at 1 C). This study provides a promising strategy for designing MXene-COF hybrid materials as functional coatings to improve the performance of Li-S batteries.
Respiratory diseases constitute a major global health burden, impacting both public health and socioeconomic conditions. Pulmonary mRNA delivery systems are now emerging as a promising therapeutic strategy to treat respiratory diseases, overcoming challenges of conventional mRNA formulations such as low pulmonary bioavailability and adverse side effects. Notably, lipid and polymer nanoparticles integrated into compatible inhaler devices represent the predominant pulmonary mRNA delivery systems. Despite the promising aspects, pulmonary mRNA delivery systems in respiratory diseases treatments face four key challenges, viz. complex airway tract structure, mucociliary clearance system, immune system, and the "last hurdle" intracellular delivery barrier. All these challenges are critical to the treatment effectiveness and safety. Recent progress made on inhalable mRNA delivery methods based on various vectors is highlighted for addressing the above challenges, boosting prospective development of mRNA-based therapies for the treatment of respiratory diseases. This review examines current challenges, strategies, and advances in inhalable mRNA formulations for respiratory diseases and explores prospects for pulmonary mRNA delivery systems, which hold great promise as a next-generation therapeutic platform.
The rational design of high-performance electrocatalysts for hydrogen evolution reaction (HER) through real-time tracking of dynamic active site evolution is both challenging and essential for the progress of sustainable energy technologies. Herein, NixCo1-xMoO4 solid solution nanotubes have been synthesized via electrospinning followed by calcination for electrocatalytic HER in a 1.0 mol/L KOH electrolyte. Optimized Ni0.25Co0.75MoO4 (denoted as NCMO-1) demonstrates high specific surface area, enhances charge transfer kinetics, and improves HER activity, achieving a low overpotential of 123 mV at 10 mA/cm2. Based on the inherent structural stability, the surface reconstruction relies on the reaction potential and the pH electrolyte via integrated approach, which involves hydroxide ion can etch the Mo species into the electrolyte accompanied by collapse and transformation from MO6 polyhedrons to amorphous cobalt-nickel hydroxides (M(OH)x (M = Co and Ni) with the electron transfer from Co to Ni sites via the oxygen-bridged cobalt-nickel bond (Co-O-Ni). Meanwhile, the dissolution of Mo enhances the hydroxylation at Co/Ni sites by revealing additional defect sites, while the formation of Co(OH)x and Ni(OH)x alters the local electronic environment. Due to the amorphous nature and structural complexity of the reconstructed sites, theoretical calculations indicate that the interaction between Co and Ni sites in NCMO-1 enhances charge transfer, strengthens adsorption, and accelerates the conversion of hydrogen and the key intermediate (*H···OH). This study provides fundamental insights into surface reconstruction behavior through the strategic integration of multi-scale in-situ characterization techniques and offers guidance for the rational design of advanced HER electrocatalysts.
Sub-nanometer high-entropy materials (HEMs) have opened new pathways in electrocatalysis and biomedicine, leveraging their tunable composition, ultrahigh specific surface area, abundant active sites, and multi-element synergy. In electrocatalysis, their highly disordered multi-element structures significantly enhance the intrinsic activity and stability for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and CO2 reduction reaction (CO2RR), while their unique "cocktail effect" enables precise electronic structure modulation. For biomedical applications, their ultrasmall size facilitates cellular uptake and tissue penetration. Simultaneously, their multi-element composition endows them with multifunctionality, including photothermal/photodynamic/catalytic/magnetic therapy, multimodal imaging, and drug delivery, while also optimizing biocompatibility and reducing toxicity. However, challenges remain in the precise synthesis and mechanistic understanding of sub-nanometer HEMs, hindering their development for next-generation high-performance electrocatalysts and intelligent theranostic platforms. In this review, we comprehensively explore the composition-structure design principles of HEMs, with a focus on the multifunctional properties achieved by small sizes, particularly in the sub-nano range, and their applications in electrocatalysis and biomedicine. Additionally, this paper prospectively discusses emerging strategies that may drive the future development of HEMs, with particular emphasis on the application potential of sub-nanometer HEMs.
Due to the abundant potassium resources, potassium ion batteries (PIBs) are gradually becoming a promising choice for large-scale energy storage. Among the many anode materials that have been investigated, antimony anode has attracted much attention due to its high theoretical specific capacity, low reaction potential and high electrical conductivity. However, these antimony anodes undergo significant volume changes (≈407%) during the potassium alloying reaction, which negatively affect their cycle stability and rate performance. In this paper, the research progress of antimony anodes in recent years is reviewed. Modification strategies to improve the performance of antimony anodes, including architectural design, alloying with other metals, composite system construction and electrolyte optimization, are discussed in depth. In addition, the possible future development directions for antimony anodes in PIBs with a view to accelerating their practical application are proposed. It is hoped that this review will help researchers design high-performance antimony anode materials more efficiently.
Lithium batteries have an exceptional energy density, efficiency, and long service lives, but their anodes show poor interfacial stability. This review summarizes recent advances in the use of atomic layer deposition (ALD) for interfacial modification of lithium battery anodes. It focuses on challenges, including the poor rate performance of intercalation-type anodes, the volume expansion and low initial Coulombic efficiency (ICE) of alloy-type anodes, and dendrite growth and solid-electrolyte interphase (SEI) instability in lithium-metal anodes. Based on this, the multifunctional roles of ALD-derived nanoscale passivation layers in regulating interfacial reactions, suppressing parasitic processes, and enhancing structural integrity are discussed. By evaluating the ability of ALD to improve the cycling lifespan, rate capability, and capacity retention, its application potential for fabricating high-energy-density storage systems is analyzed. This work provides theoretical principles and engineering pathways for the rational design of advanced anode materials.
Aptamers as synthetic oligonucleotide, exhibit exceptional target specificity and are increasingly employed in the development of high-performance aptamer-based sensors (aptasensors). Dye-displacement-based aptasensors have emerged as a label-free strategy, wherein between the aptamer and its cognate target displaces a pre-associated dye, eliciting an optical response. Despite this, conventional aptasensors rely on a single output signal, which constrains both sensitivity and detection robustness. Herein, we present a dual-mode aptasensor (DMApt) platform with fluorescence and colorimetric signal outputs derived from a systematic screening of a cyanine dye library, with CyFluor-8 identified as an optimal reporter. Notably, the DMApt features an ultrafast response time (5 s), making it highly suited for rapid, on-site detection applications. This approach leverages the superior binding affinity of native aptamers, avoiding the need for modification and ensuring high sensitivity. Mechanistically, signal generation arises from the concerted contributions of disaggregation-induced emission (DIE) and the attenuation of twisted intramolecular charge-transfer (TICT) through its application to a range of small-molecule and ionic targets, as well as its compatibility with aptamers exhibiting diverse secondary structures. This work establishes a modular, label-free framework for high-sensitivity small-molecule sensing, offering rapid response and excellent practicality for on-site biochemical, environmental, and diagnostic monitoring.
Mimicking natural energy conversion processes, the pursuit of metal-free porous organic polymers (POPs) as heterogeneous catalysts for photocatalytic oxidation is a major driving force in materials science, seeking to achieve high-performance artificial photochemical systems. In this work, we report the bottom-up synthesis of a hydrazone-linked pillararene POP in its keto form. The inherent pillararene cavities provide a unique nanoconfinement environment, enabling effective substrate recognition and electron enrichment, thereby facilitating sensitive photo-response and efficient photoenergy-to-chemical energy conversion for photocatalytic oxidation coupling of primary amines (up to 99% conversion). Crucially, the framework’s tautomeric state is precisely modulated via an irreversible keto-to-enol conversion using sodium borohydride reduction. This controlled tautomerism permanently tunes the nanoconfinement microenvironment, amplifying the polymer’s electron-rich character and optimizing pore electrostatic properties. Leveraging this tunable nanoconfinement, the resulting enol form framework achieves highly efficient adsorption of cationic pollutants (up to 95% removal for Rhodamine B). This work establishes tautomerism as a chemical tool to engineer nanoconfinement in macrocycle-based POPs, expanding the toolbox for advanced porous materials with tailored functionalities for diverse applications like photocatalysis and adsorption.
A significant challenge in organic synthesis has been the direct transformation of azaarenes into synthetically important aromatic aldehydes via formal nitrogen extrusion and carbon insertion. In this study, we present an efficient approach to reshape easily accessible azaarene-based onium salts, such as isoquinoliniums, pyridiniums, and pyrimidiniums, into functionalized multi-substituted aromatic aldehydes. This strategy relies on the strategic use of an inverse-electron-demand [4 + 2] cycloaddition-inspired cascade process with a wide tolerance of allenes, alkynes or alkenes as dienophiles. DFT calculations were conducted to gain insight into the reaction mechanism, revealing the significant catalytic roles of Na2CO3 and H2O for aldehyde formation and deamination. The operational simplicity enables widespread application of this strategy which has successfully been expanded towards the direct transformation of fused pyridinium and isoquinolinium salts as well as naturally occurring pharmaceuticals berberine sulfate and palmatine chloride into structurally novel atropisomeric N/P compounds. The resultant N/P compounds have demonstrated their potential application as ligands.
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