ACS Applied Materials & Interfaces最新文献

The oxygen evolution reaction (OER) in acidic media remains a major bottleneck for proton exchange membrane water electrolysis (PEMWE), demanding catalysts with both high activity and durability. Although Ir-based materials exhibit excellent performance, their scarcity and high cost hinder large-scale applications. Recent advances are focused on non-Ir-based catalysts, including Ru-based systems, transition-metal oxides, and metal-free materials, where strategies such as defect engineering, heteroatom doping, interface modulation, and high-entropy design can effectively tune electronic structures for better performance with improved stability. Active sites and reaction intermediates under working conditions are explored for getting deeper insights into the mechanism, using advanced in situ/operando characterization techniques. Nevertheless, under harsh acidic conditions, mental dissolution and structural degradation of catalysts still limit long-term operation. Therefore, future efforts will integrate AI-driven high-throughput screening to accelerate the rational design of catalysts while simultaneously optimizing PEM electrolyzer architectures and operando characterization techniques. Furthermore, developing sustainable seawater electrolysis technology could promote acidic OER toward large-scale green hydrogen production.

The ongoing antimicrobial resistance seriously threatens current therapies for infectious diseases and calls for new antibacterial agents. Gold nanoparticles (Au NPs) are particularly attractive in terms of antibacterial therapies, benefiting from their abundant and engineerable surface chemistries. γ-Aminobutyric acid (GABA) is a nonantibiotic nonessential amino acid acting as an inhibitory neurotransmitter in the human body and has numerous health benefits. In this study, we repurposed GABA to combat multidrug-resistant (MDR) bacteria by presenting it on Au NPs. GABA-capped Au NPs (Au_GABA) possessed a broad antibacterial spectrum against both Gram-positive and Gram-negative bacteria, including MDR strains like carbapenem-resistant Enterobacterales (CRE) and methicillin-resistant Staphylococcus aureus (MRSA). The action mechanism of Au_GABA included oxidative damage to nucleic acids, caused by the promotion of intracellular reactive oxygen species (ROS), and influence on the cell membrane, which leads to disturbances in bacterial metabolism, transport, and biosynthesis. In vivo studies demonstrated the excellent therapeutic efficacy of Au_GABA in MDR bacteria-induced purulent subcutaneous infections. Our study provided a new candidate for the treatment of MDR bacterial infections and a new direction for the novel uses of amino acids.

α-MgAgSb is an environmentally friendly alternative to traditional tellurium-based thermoelectric materials for near room temperature applications. In this study, we enhance the thermoelectric properties of α-MgAgSb by introducing a secondary Sb₂Te₃ phase using powder atomic layer deposition (powder ALD), with the aim to modify phonon scattering mechanisms and reduce the lattice thermal conductivity. Powder ALD is a thin-film deposition technique that allows for the deposition of self-limiting monolayers on high aspect ratio surfaces, enabling the conformal coating of nanopowder regardless of particle morphology. Sb₂Te₃ was selected as the coating material due to its oxygen-free synthesis route and its potential for good interfacial compatibility with the α-MgAgSb powders. Our results reveal a 10% decrease in lattice thermal conductivity of bulk α-MgAgSb as the powder ALD coating thickness increases from pristine to 20 cycles of Sb₂Te₃, without affecting the primary phase purity. Our findings highlight the effectiveness of nonoxide powder ALD coatings in suppressing lattice thermal transport, offering a promising pathway for interface-engineered, low-toxicity thermoelectric materials.

Rapid and quantitative characterization of atomic defects in two-dimensional (2D) semiconductors and transistors is crucial for growth optimization and understanding of device behavior. However, such defect metrology remains challenging due to limitations of existing characterization methods, which are generally destructive and slow or lack the necessary sensitivity. Here, we use nondestructive lateral force microscopy (LFM) to directly map surface defects in monolayer WSe₂ and WS₂ on different growth substrates (SiO₂ and sapphire), as well as in WSe₂ transistors. Through LFM measurements on various WSe₂ layers, we show that this technique can detect defect densities well below the range of typical Raman measurements on this material. We also demonstrate mapping of spatial variation of defect density within as-grown WSe₂ and that the LFM technique can detect defects on suspended and polymer-supported monolayers, expanding the application space. Applied to WSe₂ transistors, LFM uncovers defect densities over double that of similar as-grown films, suggesting that defects can be introduced by common fabrication processes. This work demonstrates the applications of LFM as a nondestructive defect characterization method for monitoring 2D material growth and device fabrication.

The resurgence of chemical warfare agents (CWAs) in recent decades underscores the urgent need for efficient and durable personal protective equipment (PPE). Conventional systems employing zeolites or activated carbons provide only passive protection via adsorption and suffer from limited porosity, low catalytic activity, and weak adhesion to textile substrates. To address these challenges, metal-organic cages (MOCs) offer a promising alternative to metal-organic frameworks (MOFs) due to their solubility, molecular nature, and tunable surface reactivity. In this study, we report the deposition of zirconium-based MOCs (ZrMOCs) onto cotton fabrics using impregnation and in situ growth techniques to develop catalytically active and mechanically robust composites. The resulting MOC-cotton materials were characterized for deposition uniformity and durability under abrasion and aging tests. Their catalytic performance was evaluated toward the hydrolytic degradation of dimethyl 4-nitrophenyl phosphate (DMNP), a nerve-agent simulant. The in situ growth method yielded homogeneous coverage and strong interfacial bonding between the ZrMOCs and cellulose fibers, resulting in enhanced resistance to mechanical stress and artificial aging, while retaining excellent breathability. Despite a moderate loading (6 wt %), the composite exhibited rapid DMNP decomposition (t_1/2 < 25 min) and maintained activity after the abrasion normed test. Although catalytic efficiency decreased after aging, it remained superior to that of MOF-based cotton composites (UiO-66-NH₂). These results demonstrate the potential of ZrMOC-functionalized textiles as active protective materials for next-generation PPE for CWA decontamination, offering a promising route toward durable and multifunctional fabrics.

Extractive diglycolamide (DGA) resins are used in several state-of-the-art techniques for purifying ²²⁵Ac, a promising radiometal for targeted alpha therapy. Unfortunately, separation processes that rely on resins are often limited to slow flow rates, high elution volumes, and long processing times. Membrane adsorbers functionalized with DGA ligands are an alternative separation material that may overcome these challenges. This work presents (1) the synthesis of an aminated tetrahexyldiglycolamide ligand, (2) the covalent tethering of the ligand to electrospun poly(vinylbenzyl chloride) fiber mats, and (3) the adsorption and desorption of La(III) and ²²⁵Ac. Chemical and physical characterization supports the covalent tethering of the ligand to the fiber mat, as well as the preservation of the fiber surface area and porosity after functionalization. Equilibrium adsorption experiments were performed with stable La(III) and radioactive ²²⁵Ac. Trends in affinity are consistent between commercial resins and the synthesized membrane adsorbers; however, the Langmuir constants and the maximum binding capacity of the membrane adsorbers were generally lower than the resins. Despite these differences, the modeled selectivity for an equimolar solution of La(III)/²²⁵Ac in 10 M nitric acid is 57. Furthermore, ²²⁵Ac is rapidly desorbed from the fibers in 10 M nitric acid (<20 min). The La(III)/²²⁵Ac selectivity and rapid ²²⁵Ac desorption indicate this class of materials is promising for rapid radioanalytical separations.

The recycling challenges of thermosetting polymers and the environmental burden from petroleum-based polymers drive the rapid development of recyclable biobased elastomers. However, cross-linked biobased elastomers face an inherent trade-off between high elasticity and high-throughput recycling: robust elastic recovery requires sufficiently cross-linked topologies, whereas efficient reprocessing favors low cross-linking densities. Herein, we address this dilemma by integrating phase separation modulation with dynamic covalent cross-linking to synthesize biobased thermoplastic elastomers via one-step in situ cross-linking. Using maleic anhydride-grafted ethylene-vinyl acetate copolymer (M-g-EVA) as the compatibilizer, biobased monomers, epoxidized soybean oil (ESO), and dimer acid (DFA) were in situ polymerized within the ethylene-propylene-diene rubber (EPDM) matrix to form a vitrimer dispersed phase. During thermal mechanical mixing, M-g-EVA was first selectively predispersed in the EPDM matrix. Subsequent in situ polymerization drives the cross-linked ESO/DFA aggregates to localize within the M-g-EVA phase, creating a distinct third phase. Meanwhile, M-g-EVA forms interfacial cross-linking with ESO and physically entangles with EPDM chains, thus constructing a stable multiphase network composed of a "continuous - interfacial - dispersed phase". The resulting material demonstrates enhanced elastic performance, featuring excellent room-temperature creep resistance (0.00184%/min), improved low-temperature compression set resistance (14% reduction at -25 °C relative to a traditional commercial TPV with similar hardness), and outstanding cyclic fatigue stability (stress retention rate >97% following 300 loading-unloading cycles). Owing to β-hydroxyester bond exchange and lubricating effect of EPDM, the multiphase polymer can be continuously extruded and reprocessed with high flux, retaining >85% of its mechanical property after 5 reprocessing cycles. In short, this study provides a scalable route to high-performance and recyclable biobased elastomers and offers design insights for sustainable elastomers.

Plasmonic gratings are versatile platforms for manipulating light-matter interactions; however, common unit-cell geometries, such as rectangular, sinusoidal, triangular, or blazed profiles, offer limited field enhancement and constrain further performance improvements. This paper reports a centimeter-scale plasmonic grating decorated with nanodendrites on the ridge sidewalls that enables strong near-field coupling and narrow resonance for ultrasensitive sensing. The structure was fabricated by interference lithography, where an in-plane interference pattern and an out-of-plane standing wave define double-nested unit cells. The subwavelength dendritic features promote strong near-field coupling and induce plasmon hybridization under perpendicular (x) polarization, whereas Rayleigh anomalies (RAs) with enhanced reflectance dominate under parallel (y) polarization. Dispersion analysis reveals a linear angle-dependent dispersion of the RA modes in contrast to the weak dispersion of the hybridized plasmon modes. A sharp, high-contrast RA resonance with enhanced reflection was achieved in high-index media, yielding a sensitivity of 510 nm/RIU and a figure of merit of 28.3 RIU^-1 for plasmonic sensing.