ACS Applied Materials & Interfaces最新文献

Manganese oxides have been considered as the most competitive cathode materials for aqueous zinc-ion batteries (ZIBs) on account of their inherent safety, high operating voltage, environmental friendliness, and cost-effectiveness. Unfortunately, the manganese dissolution, inherently poor electronic conductivity, and the sluggish reaction kinetics of commercial manganese-based oxides severely hinder their practical applications. To address the above issues, we creatively developed hierarchical porous Y₂O₃-MnO_x/C nanorods (named O_V-YMO/C) with unique heterostructures and abundant oxygen vacancies via a facile MOF-assisted synthetic process and employed as the advanced cathode. Owing to the well-constructed porous structure, larger surface areas, abundant oxygen vacancies, and strong synergetic coupling effect at the heterogeneous interface, the as-obtained O_V-YMO/C cathode exhibited a fascinating discharge capacity of 389.6 mAh g^-1 at 0.1 A g^-1. Simultaneously, it demonstrated remarkable rate performance (233 mAh g^-1 at 4.0 A g^-1) and cycling durability (90.6% capacity retention over 3000 cycles at 4.0 A g^-1). The fabricated Zn//O_V-YMO/C pouch cell could deliver superior flexibility and electrochemical stability under extreme bending conditions. Furthermore, the electrochemical reaction mechanism was comprehensively explored by kinetic analysis and density functional theory (DFT) calculations. The synergistic strategy by subtly combining the MOF-assisted approach, heterojunction engineering, and oxygen defects engineering provides valuable insights into the construction of cathode materials for high-rate and ultrastable aqueous ZIBs.

The cationic surface charge critically influences the biological functions and therapeutic outcomes of the cancer nanomedicines. However, the basic correlation between the cationic group categories and their therapeutic efficacy has not been elucidated. In this study, cationic polymeric nanoparticles with amino groups (primary, tertiary, and quaternary amines) as the single variable were leveraged to investigate the various effects of amino species for enhanced antitumor chemotherapy. The nanoparticles were constructed from a series of triblock polymers with varying cationic repeating units at the hydrophilic-hydrophobic interface. Our results suggested that quaternary ammonium outperforms its primary and tertiary counterparts in destroying mitochondrial membranes to induce apoptosis, penetrating deep inside the tumor tissue, and damaging tumor vasculatures. As a result, we were able to effectively inhibit tumor growth in mice by a quaternary ammonium conjugate without causing significant toxicity. Our work demonstrated that the chemical structures played vital roles in regulating their biological functions and provided valuable information for designing cationic drug delivery systems.

The development of polymer radiative coolers with easy processing, low cost, and high inherent emissivity has significantly promoted the industrialization process of passive daytime radiative cooling. For excellent outdoor durability, however, the traditional strategy of using UV absorbers inevitably weakens the cooling performance of polymer-based coolers. The introduction of a high UV-reflective layer has been proven to be the most effective strategy to eliminate the negative effects of UV absorption and improve the durability of polymer coolers. Here, a polymer multilayer film (PMF) based on an optical interference mechanism is designed, which exhibits an average reflectance of up to 92.3% in the 300-400 nm UV wavebands. Using a TiO₂-doped epoxy resin (TiO₂-EP) cooler as an example, the solar reflectance of TiO₂-EP increases by 5.43% after introducing PMF as a UV reflective layer. Outdoor tests without shading or convection coverage demonstrate that the average cooling temperature of TiO₂-EP with PMF is further elevated by approximately 1.1 °C. Additionally, its aging rate decreases significantly, and the solar reflectance is 5.08% higher than that of TiO₂-EP without PMF after 120 h of UV aging experiments. Furthermore, PMF obtains a periodic multilayer structure by multilayer coextrusion, which has the advantages of low cost and the ability to be prepared over a large area. PMF is suitable for any type of polymer cooler, providing an efficient method to further promote large-scale application of polymer coolers.

Here we demonstrate direct ink write (DIW) additive manufacturing of carbon nanotube (CNT)/phenolic composites with heat dissipation and excellent electromagnetic interference (EMI) shielding capabilities without curing-induced deformation. Such polymer composites are valuable for protecting electronic devices from overheating and electromagnetic interference. CNTs were used as a multifunctional nanofiller to improve electrical and thermal conductivity, printability, stability during curing, and EMI shielding performance of CNT/phenolic composites. Different CNT loadings, curing conditions, substrate types, and sample sizes were explored to minimize the negative effects of the byproducts released from the cross-linking reactions of phenolic on the printed shape integrity. At a CNT loading of 10 wt %, a slow curing cycle enables us to cure printed thin-walled CNT/phenolic composites with highly dense structures; such structures are impossible without a filler. Moreover, the electrical conductivity of the printed 10 wt % CNT/phenolic composites increased by orders of magnitude due to CNT percolation, while an improvement of 92% in thermal conductivity was achieved over the neat phenolic. EMI shielding effectiveness of the printed CNT/phenolic composites reaches 41.6 dB at the same CNT loading, offering a shielding efficiency of 99.99%. The results indicate that high CNT loading, a slow curing cycle, flexible substrates, and one thin sample dimension are the key factors to produce high-performance 3D-printed CNT/phenolic composites to address the overheating and EMI issues of modern electronic devices.

The growing threat of antimicrobial resistance (AMR) necessitates innovative strategies beyond conventional antibiotics. In response, we developed a rapid one-step method to sythesize antimicrobial peptide (AMP) ε-poly-_L-lysine stabilized selenium nanoparticles (ε-PL-Se NPs). These polycrystalline NPs with highly positive net surface charges, exhibited superior antimicrobial activity against a broad panel of pathogens, including the Gram-positive and -negative bacteria Staphylococcus aureus, Enterococcus faecalis, Escherichia coli, and Pseudomonas aeruginosa and their drug-resistant counterparts, as well as the yeast Candida albicans. Notably, 10PL-Se NPs exhibited 6-log reduction of methicillin-resistant S. aureus (MRSA) at a concentration of 5 μg/mL within 90 min, with minimum bactericidal concentrations (MBCs) below 50 μg/mL for all tested bacterial strains. The minimum fungicidal concentration (MFC) of 10PL-Se NPs against C. albicans was 26 ± 10 μg/mL. Crucially, bacteria exposed to ε-PL-Se NPs exhibited significantly delayed resistance development compared to the conventional antibiotic kanamycin. S. aureus developed resistance to kanamycin after ∼72 generations, whereas resistance to 10PL-Se NPs emerged after ∼216 generations. Remarkably, E. coli showed resistance to kanamycin after ∼39 generations but failed to develop resistance to 10PL-Se NPs even after 300 generations. This work highlights the synergistic interactions between ε-PL and Se NPs, offering a robust and scalable strategy to combat AMR.

Carbon-based perovskite solar cells (C-PSCs) have acquired broad interest due to their superior stability and lower cost compared with metal-based perovskite solar cells (M-PSCs). However, the presence of perovskite defects greatly limits the power conversion efficiency (PCE) and long-term stability of C-PSCs. Herein, a natural dye Congo red molecule containing dual-functional groups of amino and sulfonic acids is first used as a surface passivation agent to treat the surface of perovskite films. High-quality perovskite films with reducing surface defect density and inhibiting nonradiative recombination are obtained. It is shown that the Congo red molecules not only effectively interact with the perovskite, enhancing the crystallization and enlarging the crystal size, but also demonstrate positive contribution for light harvesting in the visible range. The maximum PCE of 16.22% is achieved at the optimal concentration of 0.2 mg/mL Congo red, which is much higher than 13.57% for the control device. After 840 h of storage at 30-40% relative humidity at room temperature, the unencapsulated C-PSCs can still maintain a high initial performance of 87.21% compared with 43.26% for the control cells.

Cell state transitions are fundamental in biology, determining how cells respond to environmental stimuli and adapt to diseases and treatments. Cell surface-based sensing of geno/phenotypes is a versatile approach for distinguishing different cell types and states. Array-based biosensors can provide a highly sensitive platform for distinguishing cells based on the differential interactions of each sensing element with cell surface components. In this work, a highly modular polymer-based supramolecular multichannel sensor array (FNP sensor) was fabricated by encapsulating a hydrophobic dye (pyrene) into the monolayer of a positively charged fluorescent polymer through flash nanoprecipitation (FNP). We utilized this one-polymer sensor array to discriminate among cell types commonly found in tumors: 4T1 cancer cells, NIH/3T3 fibroblast cells, and RAW 264.7 macrophage cells. The sensor also successfully characterized varying ratios of NIH/3T3 cancer-associated fibroblasts (CAFs) and RAW 264.7 tumor-associated macrophages (TAMs). This single polymer-based sensor array provides effective discrimination and high reproducibility, providing a high-throughput tool for diagnostic screening of cell types and states associated with cancer progression.