Science and Technology of Advanced Materials最新文献

Ionic self-assembly (ISA) has emerged as a powerful nanoarchitectonics strategy for constructing functional supramolecular materials through electrostatic interactions. This approach enables the formation of highly ordered nano- and mesostructures with tunable electrochemical properties. A key application of ISA lies in electroactive polyelectrolyte-surfactant complexes, which serve as dynamic platforms for biosensing and electrochemical devices. These materials, easily integrated onto electrodes via solution-based deposition techniques, offer tailored charge transport and redox activity. Their ability to incorporate metal nanoparticles and enzymes further expands their functionality, enabling the development of amperometric biosensors for highly sensitive biochemical detection. This review explores the principles of ISA-derived materials, emphasizing their role in electrochemical applications and their potential in next-generation biosensors.

The excessive accumulation of monosodium urate crystals in joints leads to the pathological condition known as gout. While conventional treatments, which include Non-steroidal Anti-inflammatory Drugs, are available, their short half-life and low bioavailability limit their practical application. To overcome these limitations and leverage the Reactive Oxygen Species (ROS)-rich microenvironment, this study developed a novel ROS-responsive thioketal-linked hyaluronic acid-based micelle loaded with manganese oxide (HTO-MnO) for enhanced treatment. Following the synthesis of the HTO-MnO nanocomplex, the micelle was well characterized and the synthesized micelle were subjected to multiple tests to confirm their efficacy in reducing ROS. In addition, the in-vitro treatment of M1-polarized macrophages showed significant responses at both the gene and protein expression levels. Eventually, in-vivo analysis of the HTO-MnO nanoparticles was performed in the MSU-induced arthritis mouse model. The elevated ROS levels in the ankle joint of the mice triggered the release of MnO nanoparticles from the HTO micelles, suppressing the ROS levels and repolarizing macrophages to their M0 state, thereby effectively mitigating inflammation. This study demonstrates the potential of nanocomplex to reduce ankle swelling and intrinsic ROS levels by targeting M1 macrophages. The results highlight its precise therapeutic mechanism to alleviate inflammation and treat gouty arthritis.

In living systems, dynamic biomacromolecular assemblies are driven and regulated by energy dissipative chemical reaction networks, enabling various autonomous functions. Inspired by this biological principle, we report a chemically-fueled phase transition of a poly(N-isopropylacrylamide) (PNIPAAm)-based polymer bearing viologen units (P(NIPAAm-V)), wherein redox changes drive coil-to-globule phase transitions. Upon the addition of a reducing agent, viologen moieties in P(NIPAAm-V) are converted into their reduced state, resulting in enhanced hydrophobicity and polymer aggregation. Coexistence of a platinum catalyst couples these redox-driven structural changes to hydrogen evolution, which oxidizes the viologen radicals, thus restoring the polymer chains to their hydrated random coil state. As a result, transient polymer assemblies form and subsequently disassemble upon depletion of the reducing agent, leading to a temporally controlled out-of-equilibrium phase transition. Moreover, by tuning the platinum concentration and reaction temperature, we achieve precise control of both the size and lifetime of these assemblies. Notably, viologen moieties constitute only about 1% of the polymer repeating units, underscoring that chemically-fueled phase transition is efficient strategy for dynamically regulating molecular assemblies. These findings demonstrate that chemically-fueled phase transitions in redox-responsive polymers offer a promising blueprint for designing dynamic, biomimetic materials capable of spatiotemporally regulated structural transformations.

In the development of renewable energy sources, batteries are considered the best option for energy storage. High energy density and high performance are key demands for emerging technologies. Lithium-metal batteries (LMBs) are considered promising candidates for storing generated energy. However, the formation of lithium dendrites and infinite volume expansion during cycling are serious limitations in current LMB applications. 3D-structured anodes have received considerable attention as an effective solution to overcome these problems. Herein, we synthesize a lithiophilic 3D-Si/SiO_x host for LMBs via a simple magnesiothermic reduction process (MRP). The 3D porous SiO_x structure provides a large specific surface area, which reduces local current density and offers ample space for Li deposition. The 3D-Si/SiO_x anode not only accommodates volume changes but also demonstrates homogeneous, dendrite-free lithium deposition with a high coulombic efficiency of more than 99% at 0.1, 0.5, and 1.0C. The symmetric cell composed of prelithiated (4 mAh/cm²) 3D-Si/SiO_x shows stable long-cycle performance for over 350 hours. By utilizing a single porous particle material with surface-limited lithiophilic properties, rather than the conventional complex 3D lithium anode designs (which typically involve hierarchical structures and lithium-friendly seed materials), this work provides new insights into the design of 3D lithium metal anodes.

Inhaled nitric oxide (iNO) is a powerful therapy for the treatment of various cardiopulmonary and respiratory diseases. However, access to iNO therapy is often limited by the necessity of cumbersome gas tanks and/or elaborate gas blending apparatus. Here, we report a lightweight, inexpensive, and maintenance-free tablet that autonomously generates a therapeutic quantity of NO in air. The tablet is composed of a thimble filter paper containing a powdery mixture of nitrite (NO₂ ^‒)-type layered double hydroxide (NLDH) and ascorbic acid loaded on silica gel (AASiO₂). NLDH by itself generates trace amounts of NO in the air due to the left-shifting of the protonation equilibrium of NO₂ ^‒ by aerial CO₂ and H₂O (2[NO₂ ^‒]_LDH + CO₂ + H₂O $\rightleftharpoons$ 2HNO₂↑ + [CO₃ ^2‒]_LDH), which is followed by disproportionation of 2HNO₂ to NO, NO₂ and H₂O. In contrast, it was found that the protonation equilibrium can be shifted to the right side when volatile acid products (HNO₂ and NO₂) are readily converted to neutral NO over the AASiO₂ reductant. Based on this, even a single tablet (containing 0.30 g NLDH and 0.90 g AASiO₂) generates 5 ~ 20 ppm NO at 0.5 L/min for 24 h, which is sufficient to be useful for the relief of severe hypoxia caused by persistent pulmonary hypertension of the newborn (PPHN). Moreover, the tablet can be activated by exhaled breath for high-dose iNO therapy (80 ~ 180 ppm for several hours), revealing its potential utility for treating viral pneumonia. The NO tablet can be stored stably over long periods at ambient temperature in a gas barrier bag and has the potential to break the logistical, financial, and operational barriers that have long existed for the widespread implementation of iNO therapy.

We demonstrated the epitaxial lateral overgrowth of m-plane α-Ga₂O₃ using halide vapor phase epitaxy. An m-plane α-Ga₂O₃/sapphire template with a patterned SiO₂ mask was used as the substrate. The highest lateral growth rate for a radial spoke-wheel patterned mask was obtained when the spoke was perpendicular to the $\left(11\stackrel{-}{2}3\right)$ direction. In this case, the lateral-to-vertical growth rate ratio (L/V ratio), with L defined as the rate of increase in the width of an elongated α-Ga₂O₃ island, was as large as 5.8. This ratio was greater than that reported for an m-direction stripe mask on a-plane α-Ga₂O₃ by a factor of 3.3 and that for an a-direction stripe mask on c- and m-plane α-Ga₂O₃ by a factor of 13. The epitaxial lateral overgrowth (ELO) of α-Ga₂O₃ on a stripe mask (window/mask widths of 2.5 μm/7.5 μm) perpendicular to $\left(11\stackrel{-}{2}3\right)$ resulted in the selective nucleation of elongated α-Ga₂O₃ islands with a flat triangular cross-section on the window areas and their coalescence into a compact film. Transmission electron microscopy revealed that the dislocation density in the laterally grown area decreased drastically because the propagation of dislocations in the seed layer was effectively blocked by the mask. We believe these results greatly contribute to the realization of m-plane α-Ga₂O₃-based future power devices.

Extracellular vesicles (EVs) hold significant promise as biomarkers and therapeutics, yet their isolation remains challenging due to their low abundance and complex sample matrices. Here, we introduce EV-Osmoprocessor (EVOs), a novel device that leverages osmosis-driven filtration for rapid and efficient EV isolation. EVOs employs a high osmolarity polymer solution to concentrate EVs while simultaneously removing smaller contaminants. Compared to traditional methods such as ultracentrifugation and precipitation, EVOs offers speed and convenience, achieving a 50-fold volume reduction in under 2 h. Our results show that EVOs retained EVs and removed >99% albumin from the cell conditioned culture medium (CCM). The isolated EVs exhibited a particle size distribution centered around 140 nm, which was very similar to EVs isolated via precipitation or ultracentrifugation. The standalone EVOs process achieved a particle:protein ratio (EV purity) of ~10⁷ particles/µg protein. Comprehensive characterization, including cryo-electron microscopy, validation of protein markers and known miRNA cargo confirmed the successful isolation of EVs. Functional assays, based on protection of cardiomyocytes from hypoxia/reoxygenation injury, demonstrated the bioactivity of EVOs-isolated EVs. Furthermore, we show that EVOs can be used to concentrate 30 ml of CCM into a 0.5 ml solution, which was then further processed with size-exclusion chromatography (SEC), improving EV purity to ~10⁹ particles/µg protein. This work establishes EVOs as a promising tool for EV research and clinical applications, offering a streamlined approach to EV isolation with enhanced analytical performance.

Intense terahertz (THz) radiation in free space offers multifaceted capabilities for accelerating electron, understanding the mesoscale architecture in (bio)materials, elementary excitation and so on. Recently popularized spintronic THz emitters (STEs) with their versatility such as ultra-broadband, large-size and ease-for-integration have become one of the most promising alternative for the next generation of intense THz sources. Nevertheless, the typical W | Co ${ }_{20}$ Fe ${ }_{60}$ B ${ }_{20}$ | Pt necessitates an external-magnetic-field to saturate magnetization for stable operation, limiting its scalability for achieving higher THz field with uniform distribution over larger sample areas. Here we demonstrate the methodologies of enhancing the high-field THz radiation of external-magnetic-field-free IrMn ${ }_3$ | Co ${ }_{20}$ Fe ${ }_{60}$ B ${ }_{20}$ | W trilayer heterostructure via optimizing the substrate with superior thermal conductivity and integrating a one-dimensional photonic crystal (PC) structure to maximize the radiation efficiency. Under the excitation of a 1 kHz Ti: sapphire femtosecond laser amplifier with central wavelength of 800 nm, pulse duration of 35 fs, and maximum single pulse energy of 5.5 mJ, we successfully generate intense THz radiation with focal peak electric field up to 650 kV/cm with frequency range covering 0.1-5.5 THz from MgO-coated sample without external-magnetic-fields. These high-field STEs will also enable other applications such as ultra-broadband high-field THz spectroscopy and polarization-based large-size strong-field THz imaging.

This study presents an approach for fabricating durable superhydrophobic surfaces on 3D-printed structures inspired by the architectural design of beehives. Using fused deposition modeling (FDM) 3D printing technology, hexagonal macrostructures were fabricated using polylactic acid (PLA) filament. These structures were designed to protect an inner layer of hydrophobic nanoparticles, which were deposited by a squeegee coating method and immobilized by a photocurable resin. The relationship between hexagonal area size (ranging from 24 to 200 mm²) and the durability of superhydrophobic properties under frictional stress was systematically investigated. Wettability and surface morphology analyses performed before and after the friction tests showed that structures with hexagonal areas between 40 and 80 mm² retained superhydrophobicity even after 100 friction cycles, while larger hexagonal configurations exhibited diminished performance. To elucidate the underlying mechanisms, a theoretical model based on the Cassie-Baxter equation was developed and compared with experimental values alongside surface observations. This research advances the development of durable and functional superhydrophobic surfaces in 3D-printed materials, with promising implications for industries requiring water-repellent and self-cleaning technologies.

Ferroptosis, a form of non-apoptotic cell death, is emerging as a promising strategy for cancer therapy. Artesunate (ART), an extract obtained from the traditional Chinese medicine Qinghaosu, has been shown to exhibit anti-cancer activity by inducing ferroptosis in cancer cells. While previous research has focused on incorporating ART monomer into drug delivery systems for enhanced cancer targeting, this study presents 2-methacryloyloxyethyl ART polymer (poly(ARTEMA)), a novel polymer synthesized from ART for the first time. Our goal was evaluation of poly(ARTEMA) anticancer potential on breast cancer cells. First, we synthesized ARTEMA using esterification followed by its polymerization using the reversible addition-fragmentation chain transfer (RAFT) polymerization method. We evaluated its mechanism of action, focusing on two key pathways: temperature-triggered singlet oxygen generation and ferrous ions (Fe²⁺) release, both of which contribute to ferroptosis. Our results demonstrate that poly(ARTEMA) selectively generates singlet oxygen and Fe²⁺ due to the endoperoxide crosslinks, leading to cell death in breast cancer cells. We also investigated the anti-cancer potential of poly(ARTEMA) on breast cancer cells with and without a ferroptosis inhibitor. The IC₅₀ values were 125 µM for the MCF-7 cancer cell line and 300 µM for the normal MCF-10 cell line, indicating enhanced toxicity toward cancer cell lines. These findings suggested that poly(ARTEMA) induces ferroptosis in cancer cells and may serve as a promising candidate for cancer therapy with minimal cytotoxicity. To the best of our knowledge, this report may be the first that successfully synthesized poly(ARTEMA) using ART, with its anticancer potential evaluation.